water

Article
Oxygen Transfer in Two-Stage Activated Sludge Wastewater
Treatment Plants
Maximilian Schwarz * , Justus Behnisch, Jana Trippel, Markus Engelhart and Martin Wagner

Institute IWAR, Technical University of Darmstadt, Franziska-Braun-Str. 7, 64287 Darmstadt, Germany;

j.behnisch@iwar.tu-darmstadt.de (J.B.); j.trippel@iwar.tu-darmstadt.de (J.T.);
m.engelhart@iwar.tu-darmstadt.de (M.E.); m.wagner@iwar.tu-darmstadt.de (M.W.)
* Correspondence: m.schwarz@iwar.tu-darmstadt.de

Abstract: Aeration is an energy-intensive process of aerobic biological treatment in wastewater

treatment plants (WWTP). Two-stage processes enable energy-efficient operation, but oxygen transfer
has not been studied in depth before. In this study, α-factors were determined with long-term ex
situ steady-state off-gas measurements in pilot-scale test reactors (5.8 m height, 8.3 m3 ) coupled to
full-scale activated sludge basins. A two-stage WWTP with more than 1 Mio population equivalent
was studied over 13 months including rain and dry weather conditions. Operating data, surfactant
concentrations throughout the two-stage process, and the effect of reverse flexing on pressure loss
of diffusers were examined. The values of αmean , αmin , and αmax for design load cases of aeration
systems were determined as 0.45, 0.33, and 0.54 in the first high-rate carbon removal stage and as 0.80,
0.69, and 0.91 in the second nitrification stage, respectively. The first stage is characterized by a distinct
diurnal variation and decrease in α-factor during stormwater treatment. Surfactants and the majority
of the total organic carbon (TOC) load are effectively removed in the first stage; hence, α-factors in



the second stage are higher and have a more consistent diurnal pattern. Proposed α-factors enable

 more accurate aeration system design of two-stage WWTPs. Fouling-induced diffuser pressure loss
Citation: Schwarz, M.; Behnisch, J.; can be restored effectively with reverse flexing in both treatment stages.
Trippel, J.; Engelhart, M.; Wagner, M.
Oxygen Transfer in Two-Stage Keywords: aeration; alpha (α); fine-bubble diffusers; high-rate activated sludge systems (HRAS);
Activated Sludge Wastewater off-gas; reverse flexing; surfactants; TOC F/M ratio; TOC sludge loading; wastewater treatment
Treatment Plants. Water 2021, 13, 1964.
https://doi.org/10.3390/w13141964

Academic Editor: Bing-Jie Ni 1. Introduction

Aeration is an essential process in aerobic biological wastewater treatment. In most
Received: 18 June 2021
Accepted: 15 July 2021
wastewater treatment plants (WWTPs), it accounts for more than half of the net energy
Published: 17 July 2021
consumption [1–3]. Engineers rely on technical standards providing design guidelines to
properly design aeration systems [4–6]. Various WWTP process configurations are possible
Publisher’s Note: MDPI stays neutral
depending on wastewater composition and required effluent target. Each process configura-
with regard to jurisdictional claims in
tion demands individual design considerations for the aeration system. Technical guidelines,
published maps and institutional affil- therefore, provide α-factors to consider inhibiting effects on oxygen transfer in the activated
iations. sludge (AS). The α-factor determines oxygen transfer efficiency as the ratio of oxygen transfer
under process conditions compared to clean water. However, comprehensive research on
oxygen transfer in two-stage AS processes is not available. This study provides planners with
α-factors required for the design of aeration systems in a two-stage configuration. We discuss
the impact of stormwater treatment and fluctuations of operating parameters such as TOC
Copyright: © 2021 by the authors.
Licensee MDPI, Basel, Switzerland.
F/M ratio on oxygen transfer in the individual treatment stages. Furthermore, surfactant
This article is an open access article
removal within a two-stage process and the effectiveness of reverse flexing to restore pressure
distributed under the terms and loss of diffusers in the different treatment stages are examined.
conditions of the Creative Commons
Attribution (CC BY) license (https://
1.1. Energy Efficiency of Two-Stage Activated Sludge Systems
creativecommons.org/licenses/by/ Currently, almost all conventional activated sludge (CAS) wastewater treatment plants
4.0/). operate in an energy-negative mode. When an HRAS system is followed by a second bi-

Water 2021, 13, 1964. https://doi.org/10.3390/w13141964 https://www.mdpi.com/journal/water

Water 2021, 13, 1964 2 of 19

ological treatment stage (e.g., for nitrogen removal), it can be operated differently than
a CAS system [7]. In this case, the first stage can redirect carbon into waste activated
sludge (WAS) through biosorption and energy self-sufficiently remove nutrients [8,9]. Liu
et al. [8] presented a variety of A-B process designs, and Jimenez et al. [10] described
design parameters to optimize carbon redirection. They defined a typical operation range
of HRAS systems as SRT < 1 day, HRT ≈ 30 min, DO < 1 mg O2 ·L−1 , and very high
sludge-specific organic loading rates that result in a concentration of influent particulate,
colloidal, and soluble chemical oxygen demand (COD) into the WAS through biosorption.
This improves direct energy recovery from carbon-loaded sludge through biogas produc-
tion [11,12]. Moreover, in-plant energy consumption is reduced by lower oxygen demand
for aerobic carbon removal and higher overall aeration efficiency [9]. The separation of
carbon- and nitrogen-removing biomass potentially reduces overall oxygen supply by more
precise aeration control according to the respective biomass’s specific oxygen demand [13].
Depending on the wastewater composition, not enough soluble COD to ensure complete
denitrification may be a critical limitation of two-stage processes that is aggravated by addi-
tional carbon redirection. Therefore, two-stage WWTPs are recommended for high-carbon
or low-nitrogen wastewater treatment; alternatively, they require side-stream short-cut
nitrogen removal processes (e.g., nitritation–denitritation or partial nitritation–anammox)
to decrease carbon requirement of nitrogen removal [8]. Nonetheless, two-stage activated
sludge configurations are a sustainable option in the ongoing shift from conventional
treatment by removal in WWTPs to more energy-efficient treatment and resource recovery
in water resource recovery facilities (WRRFs) [8].

1.2. Influences on Oxygen Transfer in Two-Stage Activated Sludge Systems

The α-factor is determined as the ratio of volumetric oxygen mass transfer coefficient
in process water compared to clean water as described in ASCE 18-18 [14] and DWA-M
209 [15]. The use of a separate fouling factor (F or αF) to distinguish between diffuser-
and wastewater-specific effects on oxygen transfer is described by EPA [4]. Recent review
articles summarize the influences on oxygen transfer in process conditions. Baquero-
Rodríguez et al. [3] reviewed a variety of factors including diffuser aging and fouling,
influent wastewater variability, and airflow rates for fine-pore diffuser aeration. Amaral
et al. [16] focused on the modeling aspect of the gas–liquid transfer in activated sludge. Both
studies concluded that the development of a model to consider all factors affecting oxygen
transfer in activated sludge systems would be extremely valuable. So far, the complexity of
interactions between factors complicates the development of a comprehensive α-model. To
achieve this goal, more knowledge about the involved processes has to be acquired.
Therefore, one path to gain deeper insight is to look at extreme variations of activated
sludge process designs such as two-stage configurations. The biosorption mechanism
utilized for carbon redirection in HRAS stages describes surface adsorption of particu-
late and colloidal organic matter on sludge flocs and storage of soluble COD inside of
biomass [17,18]. This can have a positive effect on oxygen transfer as substances inhibiting
gas-transfer at the bubble–bulk interface are removed or adsorbed on sludge flocs. Garrido-
Baserba et al. [19] discussed strategies to increase oxygen transfer efficiency through
biosorption, inter alia by specifically removing surfactants. The amphiphilic structure
of surfactants causes a negative effect on oxygen transfer at low concentrations in clean
water [20] and activated sludge [21]. High biosorption of surfactants in a first treatment
stage could improve oxygen transfer in a subsequent treatment stage. The overall energy
efficiency of an aeration system is determined not only by oxygen transfer in the bulk
liquid, but also by pressure loss of diffuser elements. This pressure loss resembles the extra
resistance that blowers have to overcome to widen membranes and diffuse air through
the membrane perforation. Pressure loss increases due to fouling, aging, and scaling of
membranes, and it also negatively affects oxygen transfer efficiency [22,23]. Reverse flexing
is a mechanical cleaning method where diffuser membranes are relaxed by turning off
the blowers and releasing pressure from the air pipes. This causes a rapid collapse of the
Water 2021, 13, 1964 3 of 19

diffuser membrane onto the diffuser’s frame under hydrostatic pressure. Turning on the
blowers flexes the diffuser’s membrane and reopens its slits, which removes biofilm and
particulate matter from the membrane surface. As a result, previously built-up pressure loss
is mitigated which enables more energy-efficient operation of the aeration system [24,25].

1.3. Goals of This Study

Factors relevant for energy-efficient operation of aeration systems have been studied
for CAS systems; however, comprehensive research is not available for two-stage AS
processes. This paper addresses this research gap and defines α-factors for design load
cases applicable to design aeration systems of two-stage AS systems by measuring oxygen
transfer on a pilot scale. Most importantly, the underlying measurements include variations
of diurnal cycle of WWTP operation and influent characteristics, rain and dry weather, and
seasonal variations affecting oxygen transfer and the α-factor. The resultant dataset covers
various load cases of a two-stage WWTP. Some procedures to design aeration systems use
static α-factors, whereas the approach of German guideline DWA-M 229-1 [5], as described
in Wagner and Stenstrom [26], distinguishes three load cases with αmean , αmin , and αmax
factors that we determined accordingly. We also quantified surfactant concentrations in
samples throughout the treatment process to examine the distribution of surfactants in the
treatment stages of a two-stage configuration. Additionally, different operation of treatment
stages within a two-stage system affects bioflocculation capability and resultant sludge
composition, which could have an effect on diffuser fouling. We investigated operation
and maintenance of fine-bubble diffusers in those conditions through a series of diffuser
pressure loss measurements after reverse flexing to determine if fouling can be mitigated
effectively in two-stage processes.

2. Materials and Methods

2.1. Design and Operation of Pilot-Scale Test Reactors
Long-term ex situ steady-state off-gas monitoring was conducted in pilot-scale test reac-
tors as described in ASCE/EWRI 18-18 (2018). Tank dimensions were 1.2 m × 1.2 m × 5.8 m
(L × W × H) with a volume of 8.3 m3 . Two reactors were operated to examine both AS
stages of a two-stage process in parallel. Both reactors were equipped with fine-bubble
disc diffusers (ELASTOX-T EPDM TYP B, WILO GVA, Wülfrath, Germany) with a diffuser
density of 13.5%. Unlike off-gas measurements using off-gas hoods, the airflow rate within
an ex situ reactor can be varied independently from the operation of the WWTP it receives
its sludge from. A range of airflow rates (specified for aerated tank volume—qVol,aer )
between 0.75 and 2.25 Nm3 ·m−3 ·h−1 was set, covering typical ranges of two-stage WWTPs.
Sludge transfer pumps (AGNM02 NEMO® , NETZSCH Holding, Selb, Germany) were op-
erated to maintain a constant hydraulic retention time (HRT) of 15 min as recommended by
ASCE/EWRI 18-18. Sludge flow was measured with electromagnetic flowmeters (Promag
W 400, Endress + Hauser AG, Reinach, Switzerland). Mixing conditions within the tanks
can be assumed close to an ideal continuous stirred tank reactor (CSTR), because of the
combined energy input of aeration and sludge transfer.
Mean values of clean water tests of standard oxygen transfer rate (SOTR) were used
as a denominator for the α-factor. Clean water tests were conducted with electrochem-
ical dissolved oxygen (DO) probes (Oxymax COS51D, Endress + Hauser AG, Reinach,
Switzerland) with a fast response time t90 of 30 s. Slower optical DO probes Oxymax
COS61D, Endress + Hauser AG, Reinach, Switzerland) were used in process conditions,
as long-term testing did not require a fast response time, and their lower maintenance
offers more reliable DO measurement in activated sludge operation. While off-gas mea-
surements require a steady inflow, clean water tests were conducted without continuous
inflow. In our pilot plant lateral sludge inflow improved oxygen transfer at low airflow
rates, which resulted in overestimates of the α-factor. As a consequence, only airflow rates
above 0.75 Nm3 ·m−3 ·h−1 were considered in this study. Clean water tests were conducted
before and after a long-term off-gas measurement period to evaluate diffuser conditions.
Water 2021, 13, 1964 4 of 19

This revealed a decrease in SOTR of 2–6% depending on airflow rate and a dynamic wet
pressure increase of about 1 kPa. These results primarily indicate inevitable aging of
diffusers and secondarily indicate scaling and fouling. Overall, the effect of scaling and
fouling during the long-term off-gas measurement was kept low due to monthly pressure
cleaning and reverse flexing of disc diffusers twice a week. Therefore, in this study, the
oxygen transfer is reported as an α-factor instead of an αF-factor. Additionally, potential
biofilm build-up on the reactor tank walls was prevented with monthly cleaning and visual
inspection to ensure only suspended biomass transferred from the adjacent full-scale AS
tanks was examined in the ex situ reactors for off-gas measurements. Online sensors were
cleaned twice a week to prohibit solids deposition and biofilm growth affecting optical
instruments.32op
Other parameters and their sensors and instruments for off-gas measurements were airflow
rate measured with thermal mass flowmeters (Proline t-mass A 150, Endress + Hauser AG,
Reinach, Switzerland), off-gas concentrations of oxygen (paramagnetic sensor) and carbon
dioxide (NDIR) measured with a gas-analyzer (X-STREAM Enhanced, Emerson Electric Co.,
MO, USA) that receives dry off-gas free of particles (CSS-V, M&C TechGroup, Ratingen,
Germany), atmospheric pressure (Cerabar PMC21, Endress + Hauser AG, Reinach, Switzer-
land), atmospheric temperature (Omnigrad T TST434, Endress + Hauser AG, Reinach ,
Switzerland), and electrical conductivity (Indumax CLS50D, Endress + Hauser AG, Reinach,
Switzerland). Data were recorded in 30 s intervals by online sensors and summarized as
15 min averages. This resulted in high-resolution data that matched the HRT of the test
reactors and the interval of operating data provided by the WWTP operator. However, resi-
dence time distribution in an ideal CSTR yields a 63% replacement of activated sludge in
the reactors at HRT of 15 min and 98% at 1 h, respectively. Therefore, for final analysis, 1 h
intervals were composed to prevent autocorrelating observations. In total, α-factors were
recorded for 9 months in long-term off-gas measurements covering a period of 13 months.

2.2. Design and Operation of Examined Two-Stage WWTP

The examined two-stage activated sludge WWTP has a design capacity of more than
1 Mio PE. It has a mean dry weather influent flow of 2.6 m3 ·s−1 and a maximum wet
weather influent flow of almost 7 m3 ·s−1 of mostly municipal wastewater, complying with
German effluent standards. Raw wastewater is first treated in screens (width 10 mm) and
an aerated grit chamber before it flows into the primary clarifier with a mean HRT of
60 min that ranges from 35 to 100 min depending on influent flow. Biological wastewater
treatment is split into a first high-rate activated sludge stage for carbon removal and a
subsequent second stage for nitrification with a fivefold larger tank volume. Both aerated
stages are plug flow reactors with tapered aeration, while 25% of tank volume of the second
stage is a continuously mixed upstream denitrification zone. Both treatment stages have
no internal recirculation and are followed by clarifiers that return activated sludge into the
respective stages. A bypass line can pass 0.2 m3 ·s−1 of primary effluent into the second
stage to redirect organic carbon required for biological nutrient removal in the upstream
denitrification. A recirculation line can recirculate 0.5 to 0.55 m3 ·s−1 of nitrate containing
final clarifier effluent into the first stage. This relieves the final downstream denitrification
(biofiltration) which removes remaining nitrate. These concepts are described in more
detail in Jimenez et al. [10] and Wandl et al. [27].
Influent wastewater load is diluted in activated sludge tanks and the concentration of
removable substances changes within AS tank zones during treatment, especially in plug
flow reactors. Therefore, determining the α-factor of a whole plug flow reactor tank at a
certain time requires off-gas testing across all subsequent aeration zones [28,29]. However,
to closely monitor the diurnal cycle of oxygen transfer, activated sludge was transferred
from the front aeration zone of both plug flow aerated stages into the pilot-scale test
reactors. Operating data of the first and second stage of the examined two-stage activated
sludge WWTP are summarized in Table 1.
Water 2021, 13, 1964 5 of 19

Table 1. Operating data of examined two-stage WWTP.

First Stage Second Stage

Parameter (Abbreviation) Unit 5th–95th 5th–95th
Mean ± SD Mean ± SD
Percentile Percentile
Volume specific airflow rate (qVol,aer ) Nm3 ·m−3 ·h−1 1.8 ± 0.5 0.9–2.3 0.7 ± 0.2 0.5–1.0
Dissolved oxygen (DO) mg·L−1 0.6 ± 0.3 0.2–1.0 3.2 ± 0.2 3.0–3.4
Actual hydraulic retention time (HRTa ) h 0.7 ± 0.1 0.5–0.9 1.9 ± 0.3 1.4–2.4
Nominal hydraulic retention time (HRTn ) h 2.0 ± 1.0 0.9–3.6 6.2 ± 2.6 2.8–10.5
Sludge retention time (SRT) d 1.9 ± 0.7 0.7–3.2 31 1 ± 7.3 21–44
Total solids in AS (TS) g·kg−1 3.0 ± 0.4 2.4–3.7 6.1 ± 0.6 5.1–7.1
Volatile fraction in AS (MLVSS/TS) % 72 ± 6 63–85 59 ± 4 53–65
TOC inflow concentration (TOCin ) mg·L−1 75 ± 22 44–113 18 ± 5.4 12–25
Water temperature (TW ) ◦C 17 ± 3 13–22 17 ± 3 13–22
Total suspended solids in effluent (TSSeffluent ) mg·L−1 25 ± 12 12–46 4.1 ± 1.7 2.1–7.6
Sludge volume index (SVI) mL·g−1 99 ± 35 51–164 49 ± 5.5 41–56
Note 1: Median value; for all other parameters the median deviates by less than 10% from the above-listed means.

The sample standard deviation marks the dispersion from mean values during stan-
dard operation of the WWTP, while the 5th and 95th percentiles are stated to describe
reasonable minimum and maximum operation conditions that are only exceeded in excep-
tional cases. Volume specific airflow rate qVol,aer is specified in relation to aerated basin
volume. The reported sludge retention time is temperature-corrected to 15 ◦ C (correction
coefficient = 1.072, compare Clara et al. [30]), and outliers outside 1.5 times the interquartile
range above and below Q1 and Q3 quartiles were removed. A rolling mean was calculated
of the remaining data spanning 2 days for the first stage and 30 days for the second stage.
These chosen timespans resemble the median SRT in the respective stages. Online turbidity
sensors (SOLITAX sc, Hach Lange GmbH, Düsseldorf, Germany) measuring mixed liquor
suspended solids are calibrated for total solids (TS) and regularly compared with laboratory
analysis (according to EN 12880). Mixed liquor suspended solids (MLSS) are not measured
regularly. On average, MLSS was 0.8 g·L−1 lower than TS. Total organic carbon (TOC)
inflow concentration (TOCin ) considers all inflows of a treatment stage (e.g., supernatant of
return activated sludge and bypass flows) proportional to their respective water flow. This
combination is required because effluent TOC of the intermediate clarifier recycled into
the first stage with return activated sludge has a share of about 30% of total TOC inflow in
the first stage. TOC concentrations are measured by ex situ online analyzers (QuickTOC,
LAR, Berlin, Germany) in the influent and effluent of the first stage and drift-corrected to
match laboratory analysis (EN 1484). We used TOC as a suitable sum parameter to describe
influent wastewater characteristics instead of COD, because ex situ online analyzers of
TOC are common in larger WWTPs and enable an analysis with higher temporal resolution
than COD laboratory analysis. For comparison, TOC/COD ratios based on laboratory
analysis were 0.33 ± 0.05 in the influent of the first stage and 0.46 ± 0.10 in the influent of
the second stage. TSSeffluent is recorded in the supernatant of the respective clarifier (2 µm
pore size). Hydraulic retention time (HRT) refers to the retention time in activated sludge
tanks, not the whole treatment stage with clarifiers. It is stated either as nominal HRTn
which considers only influent flow or as actual HRTa , which includes recirculation flows,
as well as main wastewater inflow (compare nomenclature in Henze et al. [31]). The TOC
F/M (feed to mass) ratio is typically derived from TOC concentration in the inflow, MLSS
in the AS, and volume of biological treatment stage. To account for dilution in the AS tank
and return TOC load of recirculation flows, we use the volume proportional TOCin and
HRTa as described above. To simplify comparison, TS is assumed as given in units of g·L−1
similar to MLSS. Thus, we derived an actual TOC F/Ma ratio from parameters given in
Table 1 as follows:

TOC F/Ma ratio = TOCin ·TS−1 ·HRTa −1 (kg·kg−1 ·day−1 ). (1)

 concentration in the inflow, MLSS in the AS, and volume of biological treatment stage. To
account for dilution in the AS tank and return TOC load of recirculation flows, we use the
volume proportional TOCin and HRTa as described above. To simplify comparison, TS is
assumed as given in units of g∙L−1 similar to MLSS. Thus, we derived an actual TOC F/M a
Water 2021, 13, 1964 ratio from parameters given in Table 1 as follows: 6 of 19

TOC F/Ma ratio = TOCin∙TS−1∙HRTa−1 (kg∙kg−1∙day−1). (1)

The use of actual HRTa, volume proportional TOCin, and resultant TOC F/Ma ratio
The use of actual HRT , volume proportional TOCin , and resultant TOC F/Ma ratio
reflects organic load in the aAS tanks more reasonably regarding their effect on oxygen
reflects organic load in the AS tanks more reasonably regarding their effect on oxygen
transfer in the front aerated zones than the nominal HRT n and TOC F/M ratio.
transfer in the front aerated zones than the nominal HRTn and TOC F/M ratio.
2.3.
2.3. Separate
Separate Rain
Rain and
and Dry
Dry Weather
Weather Conditions
Conditions
This
This study distinguished rainand
study distinguished rain anddrydryweather
weather conditions
conditions to to
examine
examine their impact
their impacton
oxygen transfer in the AS tanks. WWTP operators typically record
on oxygen transfer in the AS tanks. WWTP operators typically record all-day weather all-day weather condi-
tions; however,
conditions; thesethese
however, do not doreflect the diurnal
not reflect the diurnalinflow dynamic.
inflow dynamic. Instead,
Instead, wewe assigned
assigned a
weather
a weather category on the basis of the diurnal variations of collected inflow data. Figure 11
category on the basis of the diurnal variations of collected inflow data. Figure
shows
shows the
the inflow
inflow course
course during
during diurnal
diurnal cycle
cycle asas smoothed
smoothed functions
functions of of percentiles
percentiles of of the
the
inflow
inflow represented
represented by by the
the lines.
lines. Top
Top and
and bottom
bottom lineslines describe
describe the the percentiles
percentiles at at 0%
0% and
and
100%,
100%, while
while thethe lines
lines in between
between depict
depict percentiles
percentiles from 5% to 95% in 10% steps. The The
dashed line serves as a distinction where data above were assigned as
dashed line serves as a distinction where data above were assigned as rain and data below rain and data below
were
were assigned
assigned as as dry
dry weather
weather category. ItIt represents
represents the the 80th
80th percentile
percentile of of inflow
inflow data
based
based onon recorded
recorded weather
weather conditions.
conditions. In In the
the operating
operating data data ofof the examined two-stage
WWTP,
WWTP, 77% of days were recorded as dry weather (dry and frost conditions), while the
remaining
remaining 23% 23% were
were recorded
recorded as as rain
rain weather
weather (e.g.,
(e.g., rainfall,
rainfall, snowfall,
snowfall, andand discharge
discharge fromfrom
stormwater
stormwater retention
retention basins).
basins). Therefore,
Therefore, the 80th
80th percentile
percentile was chosen
chosen to to clearly
clearly separate
separate
rainfall periods
rainfall periodsfromfromregular
regularoperation.
operation.AAwastewater
wastewaterinflowinflowofof3 3mm 3∙s ·s−is1 considered
3−1 is considered as
as rain
rain weather
weather at 6:00
at 6:00 and and
as dryasweather
dry weather at 12:00.
at 12:00. The 85th The 85th
and 95thand 95th percentiles
percentiles are
are catego-
categorized
rized as rain as rain weather
weather but havebuta have a distinct
distinct diurnaldiurnal inflow pattern.
inflow pattern. While a Whilesingle arainfall
single
rainfalldoes
runoff runoff
notdoes
follow notthis
follow this on
pattern, pattern,
average,on average, lightisrainfall
light rainfall added is onadded
the dry onweather
the dry
weather In
pattern. pattern. In contrast,
contrast, the 100th thepercentile
100th percentile represents
represents maximum maximuminflow inflow capacity
capacity of theof
the WWTP and is constant throughout
WWTP and is constant throughout the diurnal cycle.the diurnal cycle.

Figure 1. Assigning weather category on the basis of diurnal variations of total wastewater inflow.

2.4. Surfactant Analysis

Surfactant concentrations of successive treatment stages of the two-stage AS WWTP
were measured with Hach cuvette tests (Hach Lange GmbH, Düsseldorf, Germany) for
anionic (LCK 332), nonionic (LCK 333), and cationic surfactants (LCK 331) in a spectropho-
tometer (DR 3900, Hach Lange GmbH, Düsseldorf, Germany). Accordingly, 24 h composite
samples were taken from primary clarifier influent, first-stage influent, second-stage influ-
ent, and second-stage effluent. Grab samples were taken from the first- and second-stage
Water 2021, 13, 1964 7 of 19

activated sludge tank and settled before taking an aliquot from the supernatant to analyze.
The samples were not centrifuged or filtered. However, when taking an aliquot, intake
of particles was avoided. Overall, surfactant cuvette tests are error-prone because other
surfactant types may cause low-bias results according to working procedure information by
the manufacturer. Duplicate measurements of each sample with a recovery were conducted
according to the manufacturer’s working procedure. The measurement series was repeated
three times over the course of 1 year. In total, at least five evaluable tests per surfactant
type are available for each sample location with a recovery between 80% and 120%.

2.5. Dynamic Wet Pressure Measurement and Reverse Flexing Procedure

Dynamic wet pressure (DWP), also known as pressure drop, pressure loss, or diffuser
headloss, is the pressure difference of a submerged diffuser calculated as the difference
between pressure in the air pipe close to the diffuser and the hydrostatic pressure. DWP
increases with higher airflow rates; therefore, it is usually specified at a specific airflow
rate. Pressure was measured with a capacitive digital pressure transmitter in the air pipes
close to the diffuser frame (Cerabar PMC21, Endress + Hauser AG, Reinach, Switzerland).
DWP was calculated as the difference of this sensor reading and the hydrostatic pressure
in the reactor defined by blow-in water depth, which is limited by an overflow in the test
reactors.
Reverse flexing was performed twice a week during maintenance of the pilot reactors,
which resulted in a period of 3 to 4 days since the last procedure. To perform reverse
flexing, blowers were shut off for up to 2 h and relative pressure in the air pipes was
reduced to 0 kPa. The diffusers remained sealed during the long-term measurements as no
water leakages were detected in the diffuser frame. Because DWP increases with airflow
rate, long-term measurement series were conducted at a constant airflow rate for better
comparison. Activated sludge from the first stage was aerated at constant airflow rate
of 1.5 and 1.9 Nm3 ·m−3 ·h−1 , and sludge from the second stage was aerated at constant
airflow rate of 0.8 and 1.0 Nm3 ·m−3 ·h−1 . Tests at lower airflow rates were run for 36 days
and those at higher airflow rates were run for 26 days. Diffusers were cleaned with high
pressure before each measurement series.

3. Results and Discussion

3.1. Effect of Rainfall and Diurnal Cycle on Oxygen Transfer
The oxygen transfer in the AS process is subject to a multitude of influence factors
that vary seasonally and within daily cycles. Additionally, hydraulic and organic loading
differ tremendously between rain and dry conditions, thus affecting oxygen transfer in
the activated sludge tanks. Table 2 presents all α-factors measured within this study as
described in Section 2 for mean ± standard deviation and 5th and 95th percentiles.

Table 2. α-factors determined with ex situ off-gas measurements in a two-stage WWTP.

First Stage Second Stage

Parameter (Abbreviation) Unit 5th–95th 5th–95th
Mean ± SD Mean ± SD
Percentile Percentile
α-Factor (ex situ
- 0.43 ± 0.06 0.33–0.54 0.80 ± 0.07 0.69–0.91
measurement)

Figure 2A divides α-factors by treatment stage and weather conditions in an empirical

cumulative distribution. The horizontal dashed lines mark the 5th and 95th percentiles.
Lower mean α-factors were measured in the first stage (0.43) than in the second stage
(0.80), as indicated by the vertical dashed lines. Kroiss and Klager [9] stated similar
α-factors of 0.45 and 0.7 in first and second stages of the Vienna main wastewater treatment
plant. Overall, influences affecting oxygen transfer differ tremendously between the first
and second stage in a two-stage AS configuration. In particular, the first high-rate stage
 α-Factor (ex situ measure-
- 0.43 ± 0.06 0.33–0.54 0.80 ± 0.07 0.69–0.91
ment)

Figure 2A divides α-factors by treatment stage and weather conditions in an empiri-

Water 2021, 13, 1964 cal cumulative distribution. The horizontal dashed lines mark the 5th and 95th percentiles. 8 of 19
Lower mean α-factors were measured in the first stage (0.43) than in the second stage
(0.80), as indicated by the vertical dashed lines. Kroiss and Klager [9] stated similar α-
factors of 0.45 and 0.7 in first and second stages of the Vienna main wastewater treatment
plant.be
cannot Overall,
compared influences
with affecting oxygenwhere
CAS systems, transfer differ tremendously
α-factors for systemsbetween the first and
with nitrification
denitrification typically fall into the range of 0.6 to 0.75 [32]. Additionally, thestage
and second stage in a two-stage AS configuration. In particular, the first high-rate distinction
ofcannot
rain andbe compared with CAS systems, where α-factors for systems with nitrification and
dry weather reveals that α-factors in the first stage decreased during high
denitrification typically fall into the range of 0.6 to 0.75 [32]. Additionally, the distinction
inflows of rainwater, whereas no such effect was apparent in the second stage. The effect
of rain and dry weather reveals that α-factors in the first stage decreased during high
of stormwater runoff on oxygen transfer has not been discussed in the literature so far.
inflows of rainwater, whereas no such effect was apparent in the second stage. The effect
However, rain events
of stormwater runoff have an impact
on oxygen transferonhas
multiple parameters
not been discussed potentially affecting
in the literature so far.oxygen
transfer
However, in rain
the events
activatedhavesludge
an impacttank, as shown
on multiple before. potentially
parameters Stormwater runoff
affecting affects the
oxygen
hydraulic
transfer inand the influent
activated load
sludgeoftank,
a WWTP.
as shown A before.
first flush often brings
Stormwater a highthe
runoff affects load
hy-due to
washout of sewer
draulic and influentsediments followed
load of a WWTP. by slightly
A first contaminated
flush often rainwater
brings a high load afterward [33].
due to washout
Wilén et al.sediments
of sewer [34] concluded
followedthat biological
by slightly processes rainwater
contaminated in the sewer system
afterward areWilén
[33]. moreetaerobic
at al. [34]flows
high concludedand that
more biological
anaerobicprocesses
at lowin flows,
the sewer
thussystem are more
changing aerobic at high
wastewater properties.
flows and
Typical more
effects of anaerobic
rain events at low
alsoflows,
includethuslower
changing wastewater
conductivity properties.
and Typical ef- with
water temperature
fects of rain
increased totalevents also(data
inflow includenotlower conductivity
shown), which is and water temperature
compensated for bywith increased
standardization to
total inflow (data not shown),
norm conditions when determining α-factors.which is compensated for by standardization to norm con-
ditions when determining α-factors.

Figure 2. Empirical
Figure cumulative
2. Empirical distribution
cumulative distribution(A)
(A)and
and diurnal variation(B)(B)
diurnal variation of of α-factors
α-factors as percentiles
as percentiles (solid(solid
lines) lines) and means
and means
(dashed
(dashed lines)lines) in the
in the examined
examined two-stageAS
two-stage ASWWTP.
WWTP.

Figure2B
Figure 2Bshows
shows the
the diurnal
diurnalvariation
variation of of
recorded
recordedα-factors in both
α-factors stages.
in both The lines
stages. The lines
represent the course of percentiles from 5% to 95% as described in SectionFigure
represent the course of percentiles from 5% to 95% as described in Section 2 for 1.
2 for Figure 1.
The first stage was characterized by a distinct peak of the α-factor at noon,
The first stage was characterized by a distinct peak of the α-factor at noon, regularlyregularly fluc-
tuating between 0.39 and 0.48, as indicated by the dashed line representing the mean α-
fluctuating between 0.39 and 0.48, as indicated by the dashed line representing the mean
factor. Peak α-factors are measured during daytime instead of nighttime due to a long
α-factor. Peak α-factors are measured during daytime instead of nighttime due to a long
retention time of wastewater in a large sewer system. In contrast, α-factors in the second
retention
stage hadtime of wastewater
a smoother in a large
course without sewer
a distinct system.
peak. Here, In contrast,
α-factors α-factors
fluctuated in the second
on average
stage had a smoother course without a distinct peak. Here, α-factors fluctuated on average
between 0.78 and 0.83 within a day. The influent load into the second stage was decreased
and buffered by the preceding HRAS tank and upstream denitrification zone, resulting in a
smoother diurnal cycle of α-factors. This also explains the different extent of rain effects on
oxygen transfer in two-stage AS treatment stages, as further discussed below.
The diurnal cycle of α-factor observed in the first stage was previously described by
an inverse relationship of α-factor and influent load [35,36]. For operators of WWTPs, this
negative correlation means that oxygen transfer is generally at its lowest when oxygen
demand is highest. To illustrate this relationship, Figure 3 displays the volume specific
airflow rate (qVol,aer ) in the full-scale AS tanks as the dependent variable of TOC inflow
concentrations (TOCin ) and α-factor. Blowers were controlled by DO in the aeration
basins to set the airflow rate. First, Figure 3A shows that volume specific airflow rate was
increased in response to higher TOCin to meet resulting oxygen demand of biomass in
 on oxygen transfer in two-stage AS treatment stages, as further discussed below.
The diurnal cycle of α-factor observed in the first stage was previously described by
an inverse relationship of α-factor and influent load [35,36]. For operators of WWTPs, this
negative correlation means that oxygen transfer is generally at its lowest when oxygen
Water 2021, 13, 1964 demand is highest. To illustrate this relationship, Figure 3 displays the volume specific 9 of 19
airflow rate (qVol,aer) in the full-scale AS tanks as the dependent variable of TOC inflow
concentrations (TOCin) and α-factor. Blowers were controlled by DO in the aeration basins
to set the airflow rate. First, Figure 3A shows that volume specific airflow rate was in-
creased
both in response
stages. Secondly, to lower
higher α-factors
TOCin to meet resulting
forced oxygen
operators todemand
increaseofairflow
biomassrates
in both
to meet
stages. Secondly, lower α-factors forced operators to increase airflow rates
this oxygen demand, as shown in Figure 3B. This figure also reveals that this relationshipto meet this
wasoxygen
moredemand,
distinct as
inshown in Figure
the first 3B. This
stage than thefigure alsoThe
second. reveals
twothat this relationship
stages was
also differed during
more distinct in the first stage than the second. The two stages also differed during rain
rain weather, where lower α-factors coincided with higher airflow rates in the first stage,
weather, where lower α-factors coincided with higher airflow rates in the first stage, but
but no significant decrease in α-factor was apparent in the second stage. It is important to
no significant decrease in α-factor was apparent in the second stage. It is important to note
note that α-factor is usually not affected by airflow rate directly, but rather coincides with
that α-factor is usually not affected by airflow rate directly, but rather coincides with
changes
changesininoxygen
oxygendemand
demand due toinfluent
due to influentload
load [29,37].
[29,37].

FigureFigure 3. Volume
3. Volume specific
specific airflow
airflow raterate
of of full-scaleaeration
full-scale aeration basins
basins for
forTOCin (A) and α-factor (B) grouped for treatment
TOC in (A) and α-factor (B) grouped for treatment
stages and weather conditions.
stages and weather conditions.
In Figure 3, the individual points represent mean data recorded within 1 h intervals.
In Figure 3, the individual points represent mean data recorded within 1 h intervals.
Colors distinguish between rain and dry weather periods as specified in Section 2. To vis-
Colors
ualizedistinguish between distribution
the two-dimensional rain and dry weather
of the periods
resulting as they
clusters, specified
were in Section
divided by 2. To
visualize
three density lines with each interval containing 25% of the respective cluster data. divided
the two-dimensional distribution of the resulting clusters, they were A
by smaller
three density lines with
area enclosed withineachtheseinterval
density containing
lines denoted25% of the
a higher respective
density cluster data. A
of the contained
smaller area enclosed within these density lines denoted a higher density of the contained
data points.
data points.
Overall, these results show that oxygen transfer in the second stage was more stable
than in the these
Overall, first stage. It isshow
results important to emphasize
that oxygen theinresultant
transfer effectstage
the second on the
wasrequired
more stable
airflow
than in the rate to meet
first stage.oxygen demand in the
It is important treatment stages;
to emphasize the described
the resultant effectdaily
on fluctua-
the required
tion ofrate
airflow α-factor
to meetfrom 0.48 to demand
oxygen 0.39 in theinfirst
thestage required
treatment an increase
stages; of 22% ofdaily
the described the airflow
fluctuation
of α-factor from 0.48 to 0.39 in the first stage required an increase of 22% of the0.83
rate to compensate for oxygen transfer inhibition. In comparison, a decrease from to rate
airflow
0.78 in the second stage required adjustment of airflow rates of only 6% within a typical
to compensate for oxygen transfer inhibition. In comparison, a decrease from 0.83 to 0.78
in the second stage required adjustment of airflow rates of only 6% within a typical day.
Moreover, Table 2 and Figure 2 reveal the range and distribution of potential α-factors in
the two stages caused by various influences on oxygen transfer.

3.2. Influence of Organic Loading on Oxygen Transfer

Below, we further examine influences that resulted in the presented range of α-factors.
The TOC F/M ratio is a suitable aggregate parameter that correlates with oxygen transfer
inhibition [38]. Figure 4 displays four scatterplots of measured α-factors for TOC F/Ma
ratio and its individual components: actual hydraulic retention time (HRTa ), TOC inflow
concentration (TOCin ), and total solids (TS).
 3.2. Influence of Organic Loading on Oxygen Transfer
Below, we further examine influences that resulted in the presented range of α-fac-
tors. The TOC F/M ratio is a suitable aggregate parameter that correlates with oxygen
Water 2021, 13, 1964 transfer inhibition [38]. Figure 4 displays four scatterplots of measured α-factors for
10 TOC
of 19
F/Ma ratio and its individual components: actual hydraulic retention time (HRT a), TOC
inflow concentration (TOCin), and total solids (TS).

Figure4.4.The
Figure α-factorsfor
Theα-factors forHRT
HRTa a(A),
(A),TOC
TOCinin (B)
(B)TS
TS(C),
(C),and
andthe
theaggregated
aggregatedparameter
parameterTOC
TOCF/M
F/Maa ratio
ratio (D)
(D) grouped
grouped for
for
treatment
treatmentstages
stagesof
ofaatwo-stage
two-stageWWTP
WWTPand andweather
weatherconditions.
conditions.

Figure
Figure4A 4Ashows
showsthe theα-factors recorded
α-factors in the
recorded firstfirst
in the and and
second treatment
second stagesstages
treatment at their
at
respective HRT . The treatment stages of the examined two-stage WWTP
their respectivea HRTa. The treatment stages of the examined two-stage WWTP were op- were operated
differently and, asand,
erated differently a result,
as a all diagrams
result, in Figure
all diagrams 4 clearly
in Figure distinguish
4 clearly both stages
distinguish from
both stages
each other. Moreover, rain and dry weather categories were clearly
from each other. Moreover, rain and dry weather categories were clearly separated withinseparated within
treatment
treatment stages,
stages, as
as HRT
HRTaa reflects
reflects high
high and
and low
low water
water inflow.
inflow. Overall,
Overall, lower
lower α-factors
α-factors
were
were recorded in the first treatment stage with its shorter HRTa. The longerHRT
recorded in the first treatment stage with its shorter HRT a . The longer HRTaawithin
within
the first stage indicated slightly higher α-factors, while no such effect could be seen in the
the first stage indicated slightly higher α-factors, while no such effect could be seen in the
second stage. Although water inflow and the resultant HRTa have no known direct impact
second stage. Although water inflow and the resultant HRTa have no known direct impact
on oxygen transfer, a change of hydraulics in a WWTP affects other parameters that have
on oxygen transfer, a change of hydraulics in a WWTP affects other parameters that have
an impact on the α-factor.
an impact on the α-factor.
TOC inflow concentrations in the first stage were higher and spread over a wider
TOC inflow concentrations in the first stage were higher and spread over a wider
range than in the second stage, as displayed in Figure 4B. Roughly two-thirds of TOC
range than in the second stage, as displayed in Figure 4B. Roughly two-thirds of TOC
influent load was removed in the first stage. While Figure 3 suggests a clear correlation
influent load was removed in the first stage. While Figure 3 suggests a clear correlation
between α-factor and TOC influent concentration, Figure 4B shows that it was less evident
between α-factor and TOC influent concentration, Figure 4B shows that it was less evident
within the respective treatment stages. However, looking at both treatment stages, a
within the respective treatment stages. However, looking at both treatment stages, a
negative correlation between TOC inflow concentration and oxygen transfer can still be
confirmed. Jiang et al. [36] concluded a similar negative logarithmic relationship between
α and COD on the basis of measurements in three WWTPs. Ahmed et al. [39] applied a
power function to fit an α-model for SBR reactors. Both approaches came to similar results
to this study but examined different WWTP process configurations that are not directly
comparable to the examined two-stage process. The major difference between α-factors
in treatment stages can be attributed to the oxygen transfer inhibiting characteristics of
readily biodegradable substrate [39], especially accumulation of surfactants on the bubble
surface [32,40]. During rain periods, α-factors observed in the first treatment stage were
lower than in dry conditions, although TOC inflow concentrations were similar or lower.
However, TOC load increased when considering the increased water flow and organic load
Water 2021, 13, 1964 11 of 19

of a first flush in the sewer system as a result of a rainfall event, thus explaining lower
α-factors. This effect was not apparent in the second stage. Here, TOC inflow concentration
was slightly higher during rainy weather as some organic load remained untreated at low
HRTa in the first stage. Nonetheless, α-factors in the second stage did not decrease because
most influent organic load was buffered in the first stage and the upstream denitrification
zone of the second stage. The implementation of an upstream denitrification stage has
been reported as advantageous for oxygen transfer in CAS systems [41]. Thus, the high
α-factors in the second stage can be attributed in part to this, even though some readily
biodegradable substrate was passed into the second stage by the bypass line.
Figure 4C displays α-factors for total solids (TS). The α-factors and TS in the second
stage were higher than in the first stage and high for activated sludge process in general.
Within the second stage, no correlation with TS was indicated, while a slight decrease in α
was apparent in the first stage, coinciding with rain weather. This outcome is discussed in
more detail in Section 3.3.
The TOC F/Ma ratio in Figure 4D combines the previously discussed parameters. Its
course was similar to TOCin in Figure 4B, except for the first stage during rainfall events.
Here, high water inflow and TOC concentration produced higher TOC F/Ma ratios with a
negative effect on α-factor. Günkel-Lange [38] examined the relationship between COD
F/M ratio and α-factor for extended aeration, nitrogen-removal, and carbon-removal CAS
systems and proposed an inverse linear correlation. Again, the examined two-stage WWTP
is different from CAS systems and complicates direct comparison. However, the presented
data complement the understanding of oxygen transfer dynamics in more complex WWTP
process configurations.
According to the diagrams in Figure 4, oxygen transfer in the second treatment stage
was seemingly unaffected by any variation of the presented parameters. However, this
cannot be concluded from the above analysis with certainty, as at most only two interactions
were taken into account in each diagram. Furthermore, the combined parameter TOC F/Ma
ratio obscured variation of its individual components (e.g., 100 kg/h TOC load at 3 g/L
TS would result in the same TOC F/M ratio as 200 kg/h TOC load at 6 g/L TS, but the
resulting conditions would affect oxygen transfer differently). Considering both treatment
stages, our results confirm the inverse relationship between TOCin or TOC F/Ma ratio and
α-factor, as presented in previous studies. However, no single parameter illustrated in
Figure 4 correlated significantly with the α-factor when considering oxygen transfer in
individual treatment stages.

3.3. Interaction of Suspended Solids and Hydraulic Load with Oxygen Transfer
Generally, TSS concentration, usually measured as mixed liquor suspended solids
(MLSS), inversely correlates with the α-factor. This has been extensively demonstrated
for membrane bioreactors (MBR), where different rheology of thick sludge at MLSS up
to 30 g·L−1 has an influence on gas transfer dynamics [42–44]. Henkel [45] proposed that
the volatile fraction of suspended solids (mixed liquor volatile suspended solids—MLVSS)
in particular causes oxygen transfer inhibition. These studies extrapolated the inverse
relationship measured in MBRs into conventional activated sludge systems (CAS), where
typical MLSS concentrations are below 6 g·L−1 . In contrast, newer studies stated that
biosorption decreases the concentration of organic substances in the soluble phase, thereby
reducing oxygen transfer and inhibiting accumulation in the gaseous phase [39,46]. Higher
MLSS increases the biosorption of organic matter in CAS, which additionally improves
carbon redirection in HRAS stages [10,47]. As a consequence of biosorption as the dominant
impact on oxygen transfer, a positive correlation between MLSS concentrations up to
6 g·L−1 and α-factor was proposed by Baquero-Rodríguez et al. [3]. Overall, there seems
to be no robust relationship between MLSS and α-factor for CAS [39]. Modeling α from
MLSS does not include possible influences of floc structure on oxygen transfer, which vary
inevitably between WWTPs. It is probable that floc size (e.g., measured as particle size
distribution), settling characteristics (SVI), or addition of precipitants (e.g., for phosphorus
Water 2021, 13, 1964 12 of 19

removal) alter the liquid–solid interface, thus also influencing the gas–liquid and gas–solid
interfaces. To summarize, MLSS or TS as typical parameters in wastewater treatment
cannot describe all properties of the solid and liquid phase that are relevant to the dynamic
of oxygen transfer once the gas phase is added.
Below, we discuss various parameters to describe the solid and liquid phase in the
treatment stages of the examined two-stage WWTP and their potential influence on the
α-factor. As shown in Figure 4C, total solids were overall higher in the second stage
(6.1 ± 0.6 g·kg−1 ) than in the first stage (3.0 ± 0.4 g·kg−1 ). In contrast, the volatile fraction
of the respective sludges was higher in the first stage (72 ± 6%) than in the second stage
(59 ± 4%). Although Henkel [45] argued that the inverse relationship between the α-factor
and the solid phase is better described by MLVSS than MLSS, this is not immediately
obvious when comparing the absolute MLVSS in the two-stage WWTP. Here, MLVSS was
still higher in the second stage (~3.6 g·L−1 ) than in the first stage (~2.2 g·L−1 ), even though
α-factors were higher in the second stage. Thus, in our results, a potential negative effect of
organic content of sludge measured as MLVSS was superimposed by enhanced biosorption
in the second stage, ultimately increasing oxygen transfer. This is supported by various
characteristics that could be beneficial to oxygen transfer in the second stage compared to
its preceding first stage, such as better sludge settling (SVI of 49 ± 5.5 mL·g−1 compared
to 99 ± 35 mL·g−1 ). This would also result in lower total suspended solids in effluent
(4.1 ± 1.7 mg·L−1 in second stage instead of 25 ± 12 mg·L−1 in first stage). The activated
sludge was also altered by addition of sodium aluminate as precipitant for phosphorus
removal in the influent and effluent of the second stage. Overall, this also affected the
liquid phase, which had a visually distinguishable higher turbidity of supernatant from
the first-stage activated sludge compared to the clear supernatant of sludge samples from
the second stage. SVI, TSSeffluent , precipitant use, or turbidity of supernatant have not
previously been used to explain oxygen transfer in the AS process. Their individual
influence on oxygen transfer cannot be quantified, because only two stages with opposed
characteristics were examined in our study. However, these parameters further describe
characteristics of the solid phase within the two-stage process that could explain the overall
difference of α-factors between the first and second stage.
Within the second stage, no correlation of α-factor with TS was indicated, whereas
a slight decrease in α was apparent in the first stage, coinciding with rain weather, as
depicted in Figure 4C. Rainfall affected TS concentrations differently in the treatment
stages of the two-stage WWTP. Figure 5A illustrates the relationship between TS and HRTa
for both rain and dry weather inflow in the respective treatment stage. At lower HRTa
and high hydraulic load during rainy weather, TS decreased in the second stage, while it
remained stable in the first stage. This is unexpected as processes with higher HRT and
SRT are generally less susceptible to biomass washout due to stormwater flows [48,49].
Examining operating data indicated that this may have been caused by washout of TS
from the primary clarifier into the first stage at shorter HRTa (data not shown). However,
the elevated TS concentrations might not have been the only cause of lower α-factors
during stormwater treatment in the first stage. HRTa represents the possible adsorption
contact time of soluble and colloidal organic substances with sludge flocs within the AS
tank. Once this organic load is adsorbed on sludge flocs, it is removed through waste
activated sludge in the clarifier, and it is also less likely to inhibit oxygen transfer in the
gas phase. Jimenez et al. [10] determined optimal operating conditions of an HRAS system
(260 L, CSTR) for removal of soluble, colloidal, and particulate COD at HRTs of >15 min,
>30 min, and >45 min, respectively. As a conclusion, low HRTa caused by rainwater inflow
decreased biosorption capacity in the first stage which left more soluble and colloidal
organic substances that could accumulate in the gas phase, thus decreasing the α-factor.
On the contrary, the α-factor did not drop at lower HRTa and TS in the second stage (see
Figure 3A,C). However, as the second stage received low organic load (see Figure 3B),
biosorption mechanisms most probably were much less pronounced than in the first stage.
 Jimenez et al. [10] determined optimal operating conditions of an HRAS system (260 L,
CSTR) for removal of soluble, colloidal, and particulate COD at HRTs of >15 min, >30 min,
and >45 min, respectively. As a conclusion, low HRT a caused by rainwater inflow de-
creased biosorption capacity in the first stage which left more soluble and colloidal or-
ganic substances that could accumulate in the gas phase, thus decreasing the α-factor. On
Water 2021, 13, 1964 the contrary, the α-factor did not drop at lower HRTa and TS in the second stage (see13 of 19
Figure 3A,C). However, as the second stage received low organic load (see Figure 3B),
biosorption mechanisms most probably were much less pronounced than in the first stage.

5. TS for
FigureFigure HRT
5. TS (A)aand
for aHRT (A) and for for
α-factor
α-factor volatile fraction
volatile inin
fraction activated
activatedsludge
sludgeas
asdaily
daily mean (B), grouped
mean (B), groupedfor
forboth
bothtreat-
treatment
stagesment stages of a two-stage
of a two-stage WWTP and WWTP and weather
weather conditions.
conditions.

TheThe α-factors are

α-factors are summarized
summarized as daily meanmean
as daily valuesvalues
in Figure in 5B and compared
Figure with
5B and compared
volatile fraction determined from grab samples of activated sludge.
with volatile fraction determined from grab samples of activated sludge. Overall, the Overall, the volatile
fraction was lower in the second stage than the first stage due to lower load, higher SRT,
volatile fraction was lower in the second stage than the first stage due to lower load,
and the addition of sodium aluminate as precipitant for phosphorus removal. Within the
higher SRT, and the addition of sodium aluminate as precipitant for phosphorus removal.
treatment stages, the regression line surrounded by 95% confidence intervals revealed a
Within the treatment stages, the regression line surrounded by 95% confidence intervals
negative correlation of α-factor with volatile fraction in the first stage. While an effect po-
revealed
tentiallya remained,
negative no correlation
significantofcorrelation
α-factor waswithapparent
volatileinfraction in the
the second first
stage. stage. While
Operating
an data
effect potentially
revealed remained,
a slightly elevated no significant
volatile fractioncorrelation
in activated was apparent
sludge, in return
as well as the second
stage. Operating
activated sludge,data revealed
at lower a slightly
HRTa (data elevated
not shown), which volatile fraction
could have in decreased
further activatedα- sludge,
as factor
well as return
during activated
rainy weather.sludge, at lowerthe
As a conclusion, HRT a (data negative
suggested not shown), which
correlation of could
α-fac- have
tor with
further the volatile
decreased fractionduring
α-factor of solids by Henkel
rainy weather. [45] As
is one of the mechanisms
a conclusion, determining
the suggested negative
oxygen transfer
correlation dynamics
of α-factor within
with the the first stage.
volatile A stronger
fraction impact
of solids by of volatile[45]
Henkel fraction wasof the
is one
demonstrated
mechanisms in the first stage,
determining oxygen whereas,
transfer in dynamics
the second within
stage, itthewasfirst
superimposed by
stage. A stronger
otherof
impact influences.
volatile fraction was demonstrated in the first stage, whereas, in the second stage,
It is worth mentioning that the individual impact of wastewater parameters on α-
it was superimposed by other influences.
factor discussed in this study cannot be derived and quantified from the above analysis.
It is worth mentioning that the individual impact of wastewater parameters on
In contrast to a controlled experimental design in which all examined parameters are var-
α-factor discussed in this study cannot be derived and quantified from the above analysis.
ied systematically, we measured oxygen transfer of an operating full-scale WWTP. The
In resulting
contrast dataset
to a controlled experimental
describes only a combination design in whichoccurring
of parameters all examined parameters are
in real conditions.
varied
Additionally, building a mechanistic model of influences on oxygen transfer with aWWTP.
systematically, we measured oxygen transfer of an operating full-scale mul- The
resulting dataset describes only a combination of parameters occurring
tivariate analysis produces unreliable results when based only on two AS stages that are in real conditions.
Additionally, building a mechanistic model of influences on oxygen transfer with a mul-
tivariate analysis produces unreliable results when based only on two AS stages that are
operated as differently as in the examined two-stage WWTP. The diagrams in Figure 3
show no overlap between α-factors measured in the treatment stages and their process
parameters. Hence, complementing our results with further data from CAS systems is
necessary to fill these gaps and enable more general inference from wastewater treatment
parameters on oxygen transfer dynamics. Lastly, although treatment capacity and overall
oxygen demand certainly change throughout seasons, no strong seasonality of α-factor can
be derived from our results thus far. Nonetheless, our results allow a complete assessment
of α-factors for aeration system design purposes in a two-stage WWTP.

3.4. Design Load Cases for Aeration Systems of Two-Stage WWTPs

The design of aeration systems of WWTPs specifies the number of diffusers and
airflow rates to meet oxygen demand in activated sludge tanks. Diffuser manufacturers
state standardized oxygen transfer parameters determined in clean water. However,
Water 2021, 13, 1964 14 of 19

to consider oxygen transfer inhibition occurring in activated sludge, these parameters

have to be multiplied by the α-factor. This design process has been described in various
technical guidelines and reference books [4,6,50]. Oxygen transfer inhibition depends
on the WWTP’s treatment goal and various processes, among other factors. However,
no α-factors have been proposed for two-stage WWTP process configurations thus far.
Therefore, according to our results from long-term measurements, we propose α-factors
for the design of aeration systems in two-stage systems.
The design approach of German standard DWA-M 229-1 [5], based on Günkel-
Lange [38], applies mean, minimum, and maximum α-factors to define load cases. The
αmean represents the average operation conditions of a WWTP. We, therefore, calculated
αmean as the average of all α-factors measured during dry weather operation at the ex-
amined two-stage WWTP that fell between the mean ± standard deviation of HRTa , TS,
and TOCin , as stated in Table 1. From this, we derived αmean values of 0.45 and 0.80 for
the first and second stages, respectively. Because no rainy weather was considered for
αmean , it was slightly higher than the average of all measurements in the first stage (0.43),
while there was no difference in the second stage (0.80, compare Table 2). The αmin and
αmax values describe oxygen transfer inhibition during high and low load of the WWTP,
respectively. We defined these α-factors on the basis of a comprehensive dataset including
seasonal variation, as well as rain and dry weather conditions, measured within a 13 month
period of conducting long-term off-gas measurements. Hence, we approximated αmin and
αmax as the 5th and 95th percentiles of the full dataset, respectively. These percentiles were
chosen with a remaining measurement uncertainty in mind. If the design process requires
otherwise, the full set of measured data is shown in Figure 2. Our proposed α-factors to
design aeration systems in two-stage configurations are summarized in Table 3. These
results are applicable for the design of aeration systems in two-stage WWTPs similar to the
one examined in this study.

Table 3. The α-factors for design load cases of two-stage activated sludge WWTPs.

Treatment Stage αmean (−) αmin (−) αmax (−)

First stage (HRAS) 0.45 0.33 0.54
Second stage 0.80 0.69 0.91

3.5. Removal of Surfactants in Two-Stage WWTPs

Surfactants have a negative effect on oxygen transfer even at low concentrations due
to their amphiphilic structure. They adsorb on the gas–liquid interface of bubbles, as well
as on the solid phase of sludge flocs and other particles. Quantifying surfactant loads
throughout the wastewater treatment process allows identifying which treatment stage is
particularly affected by oxygen transfer inhibition and which treatment process eliminates
surfactants. Although a decrease in surfactant concentrations with each treatment stage is
expected, the extent of such a reduction is not obvious in two-stage configurations. Effluent
quality of a HRAS stage is poor because it is followed by a second treatment stage. First-
stage settling tank effluent is characterized by a visible turbidity, remaining mean TOC
of 48 mg·L−1 , and TSSeffluent of 25 mg·L−1 (see Table 1). Thus, the remaining surfactant
concentration passing into the second stage cannot be neglected for oxygen transfer and
has to be measured.
Figure 6 shows boxplots of surfactant concentrations of successive treatment stages of
the examined two-stage WWTP divided into three surfactant types. The median of each
surfactant type in a sample is summed and connected by a dashed line (median total).
Boxplots and the trendline show that surfactant concentrations decreased throughout the
treatment stages. Most importantly, total surfactant concentration decreased about 70%
from first-stage influent to second-stage influent, and a dilution of influent concentration in
both treatment stages was apparent, as concentrations in the activated sludge supernatant
were lower than the preceding influent concentrations. Anionic and nonionic surfactants
 concentration passing into the second stage cannot be neglected for oxygen transfer and
has to be measured.
Figure 6 shows boxplots of surfactant concentrations of successive treatment stages
of the examined two-stage WWTP divided into three surfactant types. The median of each
surfactant type in a sample is summed and connected by a dashed line (median total).
Water 2021, 13, 1964 Boxplots and the trendline show that surfactant concentrations decreased throughout the 15 of 19
treatment stages. Most importantly, total surfactant concentration decreased about 70%
from first-stage influent to second-stage influent, and a dilution of influent concentration
in both treatment stages was apparent, as concentrations in the activated sludge superna-
were
tantmore
were prevalent
lower than inthethe samples,
preceding whichconcentrations.
influent is typical forAnionic
municipal
and wastewater composi-
nonionic surfac-
tion [51,52].
tants Although
were more absolute
prevalent concentrations
in the samples, which isof individual
typical cuvette
for municipal tests are com-
wastewater unreliable,
theposition
performed measurement
[51,52]. seriesconcentrations
Although absolute provides a reasonable
of individualspan of concentrations
cuvette for each
tests are unrelia-
treatment stage. In comparison,
ble, the performed measurementOdize series [46] measured
provides anionicspan
a reasonable surfactants in HRASfor
of concentrations influent
each
(8 ± 2 mg ·L−1 ) and
treatment stage. In comparison,
effluent (1 ± 0.1 mg ·L−1[46]
Odize measured
), both of whichanionic surfactants
are within in HRAS
the above described
influent (8
surfactant ± 2 mg∙L−1) and
concentration effluent
range. The(1overall
± 0.1 mg∙L −1), both of which are within the above
surfactant removal of more than 95% within
thedescribed
WWTP issurfactant concentration
in line with range.
other studies TheThe
[51]. overall
highsurfactant
surfactantremoval of more than
concentrations measured
95% within the WWTP is in line with other studies [51]. The high surfactant
in the first treatment stage correspond to low α-factors (0.43 ± 0.06), as well as lower concentrations
measured in the first treatment stage correspond to low α-factors (0.43 ± 0.06), as well as
surfactant concentrations and higher α-factors (0.80 ± 0.07) in the second stage. Hence,
lower surfactant concentrations and higher α-factors (0.80 ± 0.07) in the second stage.
the previously described higher alpha values in the second stage can also partially be
Hence, the previously described higher alpha values in the second stage can also partially
attributed to the
be attributed to adsorption
the adsorption and biological
and biologicalremoval
removal of surfactantsininthe
of surfactants the first
first stage.
stage.

Figure
Figure 6. Surfactant
6. Surfactant concentrationsof
concentrations of successive
successive treatment
treatmentstages divided
stages intointo
divided surfactant types.types.
surfactant

3.6. Reverse Flexing in Two-Stage Processes

3.6. Reverse Flexing in Two-Stage Processes
Influencing factors on fouling in biological wastewater treatment have been studied
Influencing factors on fouling in biological wastewater treatment have been stud-
extensively for membrane bioreactors [53], whereas the effect of fouling on diffuser mem-
iedbranes
extensively for membrane
has focused primarily on bioreactors [53], whereas
quantifying economic the effect
implications of fouling
[22,54,55]. on diffuser
Knowledge
membranes
about site-specific wastewater characteristics and WWTP operation on fouling of diffuserKnowl-
has focused primarily on quantifying economic implications [22,54,55].
edge about site-specific
membranes wastewater
is sparse. Thus, characteristics
Rosso et al. and WWTP
[56] even suggested operation
implementing onlong-
on-site fouling of
diffuser membranes
term column testingisofsparse.
variousThus, Rosso
diffusers et al.of[56]
as part even suggested
the design procedureimplementing
to take site-spe-on-site
long-term column
cific fouling effectstesting of various
into account when diffusers as part of
selecting diffusers. Asthe designbefore,
discussed procedure
inflowto take
site-specific fouling effects into account when selecting diffusers. As discussed before,
inflow wastewater characteristics in the treatment stages of the examined two-stage WWTP
and their operation differ; therefore, sludge characteristics differ as well. The resulting
separated biomasses with higher content of heterotrophic organisms in the first stage for
high-rate carbon removal and autotrophic organisms in the second stage for nitrification
could affect fouling behavior of diffusers differently. So far, it is unknown whether existing
diffuser maintenance procedures can be applied to mitigate the pressure loss of diffusers in
two-stage WWTPs.
Figure 7 shows the boxplots of measured DWP within 12 h intervals after reverse
flexing was performed. Median values revealed an expected increase of DWP within the
typical 3.5 day interval between maintenance. Most interquartile ranges spanned less
than 1 kPa of DWP difference except the test series in the first stage at 1.9 Nm3 ·m−3 ·h−1 ,
where airflow rate fluctuated by ± 0.5 Nm3 ·m−3 ·h−1 due to blower limits. Within the test
series, no systematic increase in DWP during multiple cleaning intervals was observed
(data not shown), which would be expected over longer periods without periodic pressure
cleaning [23,24]. According to these test series, we can conclude that pressure loss can be
 two-stage WWTPs.
Figure 7 shows the boxplots of measured DWP within 12 h intervals after reverse
flexing was performed. Median values revealed an expected increase of DWP within the
typical 3.5 day interval between maintenance. Most interquartile ranges spanned less than
Water 2021, 13, 1964 1 kPa of DWP difference except the test series in the first stage at 1.9 Nm3∙m−3∙h−1, where 16 of 19
airflow rate fluctuated by ± 0.5 Nm3∙m−3∙h−1 due to blower limits. Within the test series, no
systematic increase in DWP during multiple cleaning intervals was observed (data not
shown), which would be expected over longer periods without periodic pressure cleaning
[23,24]. effectively
restored According to thesereverse
with test series, we can
flexing in conclude that pressure
both treatment stagesloss
of can be restoredWWTP.
a two-stage
effectively with reverse flexing in both treatment stages of a two-stage
In conclusion, operators of a two-stage WWTP do not have to adapt different WWTP. In conclu-
diffuser
sion, operators of a two-stage WWTP do not have to adapt different diffuser maintenance
maintenance intervals or procedures for the two treatment stages.
intervals or procedures for the two treatment stages.

FigureFigure 7. Increase
7. Increase in DWP
in DWP of disc
of disc diffuserssince
diffusers sincelast
last reverse
reverse flexing
flexingprocedure during
procedure operation
during in activated
operation sludgesludge
in activated from from
first and second stage and at two specific airflow rates (Nm
first and second stage and at two specific airflow rates (Nm ·m ·h ).
3∙m−3−
3 ∙h
3 −1).−1

4. Conclusions
4. Conclusions
On the basis of our long-term off-gas measurements, we summarize below our find-
On
ings the basis
relevant for of our long-term
design off-gas
and operation measurements,
of aeration systems in we summarize
two-stage below
activated our find-
sludge
ings relevant
WWTPs. for design and operation of aeration systems in two-stage activated sludge
WWTPs.
1. This paper defined α-factors for the first and second stages of a two-stage WWTP.
1. This
Thepaper defined
underlying off-gas for the first
measurements
α-factors on aand
pilotsecond stages of
scale covered a two-stage
a typical WWTP.
range of op- The
eration conditions
underlying off-gas of such a process,on
measurements asadetailed in Table
pilot scale 1, including
covered a typicalseasonal
range ofvaria-
operation
tion, as well
conditions ofassuch
dry and wet weather
a process, conditions.
as detailed As a result,
in Table α-factors
1, including for design
seasonal load
variation, as
cases were derived for practical application to design aeration systems more
well as dry and wet weather conditions. As a result, α-factors for design load cases accu-
rately. They were determined as 0.45 for αmean and 0.33/0.54 for αmin/αmax in the first
were derived for practical application to design aeration systems more accurately.
stage (HRAS), and as 0.80 for αmean and 0.69/0.91 for αmin/αmax in the second stage.
They were determined as 0.45 for αmean and 0.33/0.54 for αmin /αmax in the first
Because different process configurations of two-stage processes exist, these α-factors
stage (HRAS), and as 0.80 for αmean and 0.69/0.91 for αmin /αmax in the second stage.
Because different process configurations of two-stage processes exist, these α-factors
can be transferred to configurations similar to the one examined in this study. No
range of α-factors for two-stage processes was previously proposed.
2. Our results show how key operating parameters influence the oxygen transfer in the
activated sludge system. Most importantly, the impact of high TOC concentrations
in inflow resulting in lower oxygen transfer rates can be confirmed and quantified
for a two-stage activated sludge process. TS and HRTa in the treatment stages were
affected differently by stormwater treatment. As a result, α-factor decreased in the first
stage, whereas the second stage remained unaffected during high wastewater inflow.
Hence, engineers can more accurately decide whether an aeration system design
meets the demands of a similar WWTP to that examined in this study. Nonetheless,
individual wastewater parameters cannot describe α-factor due to various interacting
influences. Therefore, applying machine learning methods to predict oxygen transfer
is a multivariate approach that we will examine in the future.
3. Inflow surfactant concentrations measured in 24 h composite samples revealed that
surfactant load was significantly lower in the second stage compared to the first stage.
Surfactants had a disproportionate influence on oxygen transfer compared with TOC.
Water 2021, 13, 1964 17 of 19

Lower α-factors in the first stage could be attributed to this effect but not quantified
specifically for surfactants compared to TOC in general.
4. The positive effect of reverse flexing as a maintenance method to restore dynamic
wet pressure was observed in both stages. There was no significant difference
in fouling effect on diffusers, although sludge composition differed tremendously
between the high rate and nitrification stage. Therefore, operators of two-stage
WWTPs do not have to adapt different maintenance intervals when planning a re-
verse flexing schedule.

Author Contributions: Conceptualization, M.S.; methodology, M.S. and M.W.; validation, M.S., J.B.,
J.T., M.E., and M.W.; formal analysis, M.S.; data curation, M.S.; writing—original draft preparation,
M.S.; writing—review and editing, M.S., J.B., J.T., M.E., and M.W.; visualization, M.S.; supervision,
M.E. and M.W.; project administration, M.S. and M.W.; funding acquisition, J.B., M.S., and M.W. All
authors read and agreed to the published version of the manuscript.
Funding: We thank the German Federal Ministry of Education and Research (BMBF) for funding the
research project WOBeS “Advanced optimization of aerations systems: Investigation for increase
efficiency of fine bubble diffusers through adapted process engineering and operational management”
(Research Grant 02WA1461).
Institutional Review Board Statement: Not applicable.
Informed Consent Statement: Not applicable.
Data Availability Statement: Measurement data presented in this study are available on request
from the corresponding author. Operating data from WWTP operators are not publicly available.
Acknowledgments: We acknowledge support from the Deutsche Forschungsgemeinschaft (DFG—
German Research Foundation) and the Open Access Publishing Fund of Technical University
of Darmstadt.
Conflicts of Interest: The authors declare no conflict of interest. The funders had no role in the design
of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or
in the decision to publish the results.

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