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org/est Article

Air Pollutant Emission Rates for Dry Anaerobic Digestion and

Composting of Organic Municipal Solid Waste
Chelsea V. Preble,* Sharon S. Chen, Toshifumi Hotchi, Michael D. Sohn, Randy L. Maddalena,
Marion L. Russell, Nancy J. Brown, Corinne D. Scown, and Thomas W. Kirchstetter
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ABSTRACT: Dry anaerobic digestion (AD) of organic municipal solid waste

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(MSW) followed by composting of the residual digestate is a waste diversion

strategy that generates biogas and soil amendment products. The AD-
composting process avoids methane (CH4) emissions from landfilling, but
emissions of other greenhouse gases, odorous/toxic species, and reactive
compounds can affect net climate and air quality impacts. In situ
measurements of key sources at two large-scale industrial facilities in
California were conducted to quantify pollutant emission rates across the AD-
composting process. These measurements established a strong relationship
between flared biogas ammonia (NH3) content and emitted nitrogen oxides
(NOx), indicating that fuel NOx formation is significant and dominates over
the thermal or prompt NOx pathways when biogas NH3 concentration exceeds ∼200 ppm. Composting is the largest source of CH4,
carbon dioxide (CO2), nitrous oxide (N2O), and carbon monoxide (CO) emissions (∼60−70%), and dominate NH3, hydrogen
sulfide (H2S), and volatile organic compounds (VOC) emissions (>90%). The high CH4 contribution to CO2-equivalent emissions
demonstrates that composting can be an important CH4 source, which could be reduced with improved aeration. Controlling
greenhouse gas and toxic/odorous emissions from composting offers the greatest mitigation opportunities for reducing the climate
and air quality impacts of the AD-composting process.

■ INTRODUCTION
Anaerobic digestion (AD) of organic waste is increasingly used
in the United States and Europe in commercial-scale facilities
to reduce greenhouse gas emissions, meet renewable energy
targets, build circular economies, and achieve zero waste
goals.1−3 The practice of AD for bioenergy production has
historically focused on sewage sludge and agricultural feed-
stocks, but new plants have been built to process organic solid
waste.2 For instance, state and local governments in the United
States are requiring greater landfill diversion of organic
municipal solid waste (MSW) in an effort to reduce fugitive
methane (CH4) emissions.1 Dry AD of organic MSW (22−
40% solids loading) produces biogasa fuel comprising
roughly 50% CH4 and 50% carbon dioxide (CO2)and
nutrient-rich solid digestate that can be composted to produce
soil amendment and landscaping products. Dry AD does not
require size reduction of incoming waste and can handle
inorganic contaminants that would be more problematic in wet
digesters (solids loading <16%) that rely on a relatively
homogenous slurry, such as at wastewater treatment plants.4,5
While dry AD is a promising municipal waste management
strategy, there are multiple emission sources throughout the
digestion and waste handling process that are not adequately
studied, including fugitive, combustion, and composting
emissions.
Dry AD and composting can lead to emissions of
greenhouse gases (GHGs), toxic air pollutants, and odorous
compounds to the environment that impact their net climate,
human health, and community benefits over landfilling.1 In
addition, emitted reactive compounds may increase the
atmospheric formation of criteria air pollutants, namely
tropospheric ozone and particulate matter (PM). During AD,
organic material is converted into CH4, CO2, and other trace
compounds in the absence of oxygen by a community of
microbes fed to the digester in an inoculum during startup.
This resulting biogas can be combusted in an engine for
electricity generation or further upgraded to renewable natural
gas for pipeline injection or compressed natural gas for vehicle
fueling. Biogas must be flared on-site during the startup and
shutdown phases of each digester, as well as when accumulated
biogas exceeds on-site storage capacities. Biogas may contain
significant amounts of ammonia (NH3) that is produced
during the degradation of amino acids during acidogenesis
Received: June 17, 2020
Revised: November 2, 2020
Accepted: November 6, 2020

© XXXX American Chemical Society https://dx.doi.org/10.1021/acs.est.0c03953

A Environ. Sci. Technol. XXXX, XXX, XXX−XXX
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one of the four primary stages in ADparticularly for protein-
rich feedstocks like food waste or manure.6,7 The oxidation of
NH3 present in the biogas to nitrogen oxides (NOx = NO +
NO2) can cause elevated flare emissions that contribute to air
quality problems and exceed permitted levels.1 The digestate
material remaining at the end of the dry AD cycle is aerobically
composted, a decomposition process that favors CO2 over
CH4 emissions but can also result in emissions of the GHG
nitrous oxide (N2O) and odorous/toxic NH3 and volatile
organic compounds (VOCs). These emissions depend on
aeration, windrow temperature and pH, and initial material
composition.8−13
Due to the short history of dry AD and other organic MSW-
to-energy systems in the United States, emission estimates are
limited. Few studies have considered emissions from
commercial-scale dry AD and/or composting of organic
MSW, and even fewer have followed the same organic waste
throughout its end-of-life to measure emissions at each point in
the process. Those studies that have been conducted have
typically focused on whole-site emissions, a limited number of
pollutant species, or relied on material mass balance, facility
reports, or measurements by commercial companies to
estimate emissions.14−19 Research is needed to better
characterize and quantify pollutant emission rates, from the
receiving hall at the AD facility through the production of
finished compost, to support the comprehensive climate and
air quality impact assessment of this waste diversion strategy.
This study quantifies emission rates of GHGs, criteria air
pollutants, and toxic/odorous compounds from the AD-
composting process at each point where substantial emissions
occur via measurements at two large-scale industrial facilities in
California: the Zero Waste Energy Development Company
(ZWEDC) dry AD facility in San Jose and Z-Best Products
composting facility in Gilroy. Both of these facilities employ
common practices that are representative of similar operations
across the United States and Europe.19−23 With in situ
measurements, this study seeks to: (1) develop an emission
inventory of the dry AD and composting process and identify
the dominant emission sources of each pollutant; (2)
understand the relationship between biogas NH3 content and
NOx emissions from the flare; and (3) characterize emissions
during composting. In addition, we estimate the effectiveness
of some of the employed emission control technologies. By
quantifying emission rates from the AD-composting process, it
will be possible to gain a fuller understanding of the air quality
impacts of this waste diversion strategy.
■
METHODS
Facility Operations and Emission Sources. ZWEDC is
the first large-scale dry AD facility in the United States,
employing a thermophilic, batch dry AD system that is capable
of processing up to 82,000 metric tons (8.2 × 107 kg) of MSW
per year and generating 1.6 MW of electricity. Figure S1 in the
Supporting Information (SI) shows an aerial overview of
ZWEDC, and Figure S2 shows a simplified flow diagram of the
dry AD process.
Most of the produced biogas is fed to two on-site combined
heat and power (CHP) units, consisting of internal lean-
combustion engines (2G Cenergy, model 2G-800 BG, 800 kW
nameplate capacity) that are generally operated at 500 kW.
Each CHP unit is equipped with selective catalytic reduction
(SCR) as an emission control for nitrogen oxides (NOx = NO
+ NO2). Operation of the CHP units is nominally continuous
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but depends on the need to balance forecasted sales of
electricity back to the grid with biogas production,
consumption, and storage.
When methane cannot be combusted on-site for electricity
generation, biogas is combusted in the enclosed biogas flare
system (John Zink Company, ZTOF) to convert CH4 to CO2.
The flare stack is approximately 2 m in diameter and 9 m in
height. It is designed to operate at 760−980 °C to achieve at
least a 98% destruction efficiency of non-CH4 hydrocarbons
and combustion is characterized by turbulent diffusion flames.
Biogas is regularly combusted in the flare at the end of each
AD cycle when its CH4 content is too low (less than ∼20%)
for combustion in the CHP units. This low-CH4 biogas results
from the purging of the digestion chambers at the end of each
anaerobic cycle, when ambient air is introduced to the digester
so that it can be safely opened and emptied of the remaining
digestate material. When the CH4 concentration of the digester
biogas is ultralow and falls below 3%, it is sent through the
facility’s air handling system to the biofilters. In addition to the
regular flaring of low-CH4 biogas, biogas with high-CH4
content (∼50%) is sometimes flared when on-site storage
approaches maximum capacity.
Each batch digester operates for 21 days, after which the
remaining solid digestate material is transferred to in-vessel
composting (IVC) tunnels and aerated for 4−5 days. The
ZWEDC facility is negatively pressurized, with an exhaust air
system that includes four biofilters downstream of two acid
scrubbers that remove volatile organic compounds (VOCs)
and NH3, respectively, from the air prior to emission to the
atmosphere. Together, these biofilters continuously process
∼53,000 m3 h−1 of air that collectively comes from the waste
receiving hall, ultralow-CH4 biogas from digester startup and
shutdown phases, and effluent from the IVC tunnels. Each
biofilter is 7.6 m in diameter, and the substrate is kept
sufficiently wet to promote a viable biofilm via a sprinkler
system atop each biofilter surface.
Post-AD digestate material is trucked off-site to Z-Best and
placed into commercial composting bags that are approx-
imately 100 m long, 6 m wide, and 3 m tall when filled. These
enclosed, static windrows are placed immediately adjacent to
each other. Two blowers at each windrow head force aerate the
post-AD digestate material via two perforated pipes that are
buried longitudinally along the bottom of the pile. Vent holes
are cut into each bag ∼2.5 m from the ground every ∼5 m on
either side of the pile. Throughout the 14 week composting
period, the two blowers independently and regularly cycle on
and off. For example, a blower may be set to aerate the
windrow for 40% of every hour over the composting period.
The piles are not turned or otherwise altered. After 14 weeks,
the plastic bag is opened and the remaining material is
removed and screened for usable compost. Residual inorganic
material is sent to the landfill.
In situ measurements of the emission sources across this dry
AD and composting process included: GHGs CO2, CH4, and
N2O; toxic and odorous NH3, H2S, and VOCs; criteria
pollutants NOx and carbon monoxide (CO); and black carbon
(BC), a short-lived climate pollutant (SLCP) and product of
incomplete combustion. Table S1 summarizes the measured
air pollutants, their significance, instrumentation used, and
sampled sourcesincluding the ZWEDC flare, CHP units,
and biofilters, and the Z-Best digestate composting windrows.
Due to the heterogeneous nature of the MSW received at
facilities like ZWEDC, it was not possible to characterize the
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Table 1. Average Pollutant Emission Factors by Source, with Mass Emissions Normalized to Mass of MSW Anaerobically
Digested at ZWEDCa
emission factor (mass emitted per kg MSW digested)
greenhouse gases odorous/toxic species criteria pollutants SLCP

source CH4 CO2 N2O NH3 H2S TVOC NOx CO BC

(g kg−1) (g kg−1) (mg kg−1) (mg kg−1) (mg kg−1) (mg kg−1) (mg kg−1) (mg kg−1) (mg kg−1)
flare, low-CH4 biogas  14.4 0.0    13.9 6.0 0.0
flare, high-CH4 biogas  22.3 0.1    5.3 14.8 0.0
CHP units, SCR active  50.7   0.2  4.2 16.5 
CHP units, SCR 0.22 50.7 0.0 0.1 18.3  78.0 101.9 
inactive
biofilters 1.28 28.5 7.4 64.6 4.0 3.3  8.0 
composting windrows 3.35 167.3 10.5 871.1 46.8 49.3  83.5 
a
Reported values represent emissions from both CHP units, all four biofilters, and the full 14 week composting cycle. Not all pollutant species were
measured at all sources, as denoted by () and summarized in Table S1. Emission factors <0.05 mg kg-MSW−1 are reported as 0.0 mg kg-MSW−1.
TVOC is reported as toluene-equivalents.

organic waste prior to digestion or the digestate material prior
to composting.1 The present study relied on making multiple
measurements across the dry AD and composting process to
capture the variability in emissions that may result from such
compositional differences.
Determination of Pollutant Emission Rates. Pollutant
emission factors were calculated for each species to relate the
emitted pollutant mass to the amount of MSW digested at
ZWEDC, based on average facility operations data (Table S2).
See the Supporting Information for additional details.
For the flare and CHP units, exhaust concentrations were
directly measured and a carbon balance was used to calculate
fuel-based emission factors (EFp), with units of g of pollutant
emitted per kg of CH4 combusted (g kg−1):24,25
Δ[P ] MWP wc
EFP = · · × 103
Δ[CO2 ] MWC wCH4
Here, Δ[P] and Δ[CO2] are the background-subtracted
concentrations of pollutant P and CO2 measured in the
exhaust of the CHP or flare and have molar concentrations of
ppm. The molecular weights (MW) of pollutant P and carbon
C are in units of g mol−1. Finally, wi is the weight fraction of
species i in biogas fuel. Assuming a typical 50/50 mixture of
CO2 and CH4 by volume in the biogas, this constant is 0.27 for
CH4 and 0.4 for C, assuming all carbon present in the biogas is
present as CO2 in the exhaust.
The flared biogas and corresponding exhaust were directly
measured over a 5 day period in 2018 to relate NOx emissions
from the ZWEDC flare and relate those emissions to the
biogas NH3 content. The effluent of one of the CHP units was
sampled over the course of a day when the SCR system was
inactive; these measurements were compared to the regular
compliance sampling conducted by the facility operators to
show the effectiveness of this emission control technology. To
prevent condensation and bring the measured concentrations
down to the operational ranges of the pollutant analyzers, the
effluent sampling lines were respectively diluted by a factor of
6.3 and 7.9 at the flare and CHP exhaust sampling ports. The
exhaust sample lines also passed through a condensate trap
consisting of three 50 mL glass impingers connected in series
and submerged in an ice water bath to ensure all analyzers
sampled dry exhaust. The flared biogas sample line was
likewise diluted by a factor of 6.8 and heated to prevent
condensation losses of NH3. More detailed descriptions of the
sampling setups are included in the Supporting Information.
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For the biofilters and composting windrows, exhaust
concentrations were measured and the aeration flow rate was
used to determine time-based emission rates (ERp), with units
of g h−1:
ER P = CP × Q
Here, CP is the emitted pollutant concentration in mass
concentration units (g m−3) and Q is the volumetric flow rate
for that source (m3 h−1).
A new high-density spot sampling method was developed for
this study to characterize the spatiotemporal variability of
emissions of many gases from across these aerated sources.
This method was especially necessary for the composting
measurements, since the microbial communities and con-
ditions in the windrow can vary considerably over time and
space. Such variability has previously been noted in other
emissions studies of agricultural and composting piles with
heterogeneous material.26,27 Dozens of spot samples of emitted
GHGs and toxic/odorous compounds were collected across
the biofilter and composting windrow surfaces during each
sampling window (∼1 h). A short chimney/sampling port was
inserted into the emitting surface to ensure that the sampled
volume was undiluted by ambient wind (Figures S10 and S13).
The chimney was allowed to purge with exhaust, and then
140−420 mL of gas was drawn from within the port using
syringes and injected into metal-foil-lined sampling bags
(Calibrated Instruments, Cali-5-Bond gas sampling bags).
Sample bags were brought back to the laboratory, and
compressed nitrogen was added to each to dilute the sample
by a factor of 5−25, depending on the emission source and
sample volume. This dilution enabled sufficient sampling
volume for a steady-state response by the analyzers, reduced
the relative humidity of the sample (<30%) as required by the
analyzers, and brought concentrations into the operational
measurement ranges of the analyzers. A much larger sample
volume was required to achieve a steady-state response from
the NH3 analyzer; this larger sample volume was not feasible at
all sampling locations, so NH3 measurements were instead
conducted with a subset of targeted samples.
Bag samples were collected at the same sampling locations
on each biofilter surface three times in the course of 1 day of
operation, and across multiple windrows over the 14 week
composting cycle. As noted above, the total aeration flow rate
of the four biofilters monitored by ZWEDC is 53,000 m3 h−1.
The composting aeration flow varied by windrow and was
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directly measured using differential pressure sensors. More
detailed descriptions of the biofilter and compost high-density
bag sampling are included in the Supporting Information.
VOC emissions from the biofilters and composting wind-
rows were also quantified. As the sample bag volumes were too
small and the stabilities and recoveries of some compounds in
the sample bags were poor, a different sampling approach was
used. Integrated samples were instead collected using a series
of flux chambers distributed along the centerline of the
emitting surface. These chambers were connected to the main
sample line that delivered diluted exhaust to a sampling
manifold. Exhaust flow was integrated from the five flux
chambers and sampled in parallel from the surface sampler
manifold. The emitted VOC concentrations were measured
using four integrated sampling methods that targeted different
compounds: (i) volatile carbonyls collected on adsorbent
cartridges (USEPA Method TO-11); (ii) volatile amines
collected on sulfuric acid coated filters followed by
derivatization; (iii) volatile acids collected on silica gel
cartridges; and (iv) volatile organic compounds collected on
thermal desorption sorbent tubes (USEPA Method TO-
17).28,29 More detailed descriptions of VOC sample collection
and analysis are included in the Supporting Information.
■ RESULTS AND DISCUSSION
The following results focus on the flare and composting
emission sources, as the relationship between biogas NH3
content and flare-emitted NOx and emissions from post-AD
digestate composting windrows have broad significance yet
have not been well characterized in prior literature. Emission
factors for the CHP units and biofilters are summarized in
Table 1 and are included in the emission inventory results
below.
NOx Formation in Biogas Flare. Given the potential of
significant NH3 levels in the flared biogas at AD facilities, a
focus of the present study was to measure the relationship
between emitted NOx and the NH3 content (i.e., fuel NOx).30
Elevated NOx emissions that contribute to the atmospheric
formation of ozone and PM can be of concern for AD facilities
that must comply with permits set by their local air quality
agency, as emissions that exceed maximum allowable levels can
result in citations and fines.1
During sampling at the flare, 13 high-CH4 biogas flaring and
four low-CH4 biogas flaring events were measured. As shown
in Figure S3, there are important operational differences for
these two combustion types at the flare, with low-CH4 flaring
requiring a dynamic mix of low- and high-CH4 biogas
combustion to keep the mixture’s CH4 content at ∼20% and
the flare temperature steady. Figure S15 in the Supporting
Information plots the concentration of biogas NH3 and the
corresponding emitted NOx concentration over a typical low-
and high-CH4 flaring event. NH3 concentration was directly
measured in the biogas at a point just before it was delivered to
the flare, and NOx concentration was directly measured in the
flare effluent prior to emission to the atmosphere (Figure S6).
The NH3 concentration in the flared biogas increases from
∼20 to 1000 ppm over the course of the low-CH4 combustion,
as the digester biogas is increasingly diluted during the
shutdown. As the fuel NH3 increases, flare-emitted NOx
concentrations also increase. In contrast, both the fuel NH3
and emitted NOx concentrations remain nearly constant ∼20
ppm during the high-CH4 biogas flaring event. This difference
in fuel NH3 content may be related to changes in pH during a
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digester shutdown, as the system shifts from an acidic
anaerobic state to an increasingly more alkaline aerobic
condition that promotes volatilization of NH3.31,32
Figure 1 shows minute-average NOx emission factors versus
the biogas NH3 concentration during low- and high-CH4
Figure 1. Minute-average NOx emission factors from high- and low-
CH4 biogas flaring events relative to NH3 concentrations measured in
the flared biogas.
biogas flaring events. The nonzero intercept of the NOx
emission factor trend means that the flare would emit NOx
even if there was no NH3 in the biogas, indicating thermal or
prompt NOx formation. Thermocouple readings show that the
ZWEDC flare operates at ∼900 °C, far below the temperature
threshold of >1600 °C for thermal NOx formation when N2 in
air can be cleaved to form NO.30 However, the fixed
temperature measurement is not representative of the
turbulent flame temperature everywhere, and hot spots may
exist where thermal NOx is formed. Some NOx could also be
formed via the prompt NOx mechanism, which occurs in the
flame at lower temperatures than the thermal formation
pathway.30
The NOx emission rate increases with NH3 concentration in
the flared biogas. When the biogas NH3 concentration is below
∼200 ppmtypical of high-CH 4 biogasthe thermal
mechanism can be significant in poorly mixed regions where
diffusion flames occur and the prompt NOx pathway can be
important in flame zones where radical concentrations are
larger than equilibrium values.30 When NH3 concentration
exceeds ∼200 ppm, which is common during low-CH4 biogas
flaring, the fuel NOx formation pathway dominates. The flare
operates overall as fuel-lean and fuel NOx formation is
kinetically favored and expected under such lean combustion
conditions.30 The flare manufacturer previously reported that
when ammonia was injected into a natural gas fuel stream to
simulate landfill gas flaring, NOx emissions increased with fuel-
bound nitrogen.33 Those tests were conducted up to ∼200
ppm NH3 and showed a NOx increase of up to 100% across
that concentration range, whereas the results presented in
Figure 1 expand the observed range to 200−1000 ppm NH3
and show increases of up to 350% in emitted NOx.
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Figure 2. Distributions of composting spot measurements of emission rates of (a) CO2, (b) CH4, (c) N2O, (d) NH3, and (e) H2S as a function of
composting windrow age. The horizontal axis shows unique identification names of the windrow sampled and the windrow age when samples were
taken; this is a category axis and the windrow ages are not spaced evenly in time. Windrows sampled multiple times during the 14 week composting
process are color-matched. Note that the mean emission rate from each distribution is the average value used to characterize each windrow, and
these distributions show the potential range of calculated emission rates that could result from relying on a single spot measurement.

Current NOx emission standards for industrial flares are
linked to emission estimates from the Environmental
Protection Agency (AP-42) that are based upon a 1973
industrial flare emissions study.34,35 There are important
differences between typical industrial flare gas and biogas,
the latter of which includes elevated levels of CO2 that are
nearly equal to CH4 and act as a thermal diluent. In addition,
these guidelines may underestimate NOx generation from a
biogas flare because the typical industrial flares contained little
to no fuel nitrogen. The results of this study indicate that
reducing the NH3 content of the flared biogas would reduce
fuel NOx emissions, in particular during flaring of low-CH4
biogas. Moreover, NH3 removal is of interest more broadly for
AD because high concentrations (>1,700−14,000 g L−1) can
inhibit digestion through a variety of mechanisms; most
removal technologies seem to target wet AD systems, though,
and many are not economically viable.36,37
Composting Emissions. Sampled windrows ranged in age
from a few days to 13.1 weeks old, and three of five windrows
were sampled more than once in the composting cycle. An
average emission rate in units of pollutant mass emitted per
hour per windrow pile was calculated as the product of the
effective hourly aeration flow rate and the average concen-
tration of emitted gas from each windrow, the latter of which
was calculated as the average of all bag samples taken during a
sampling window (∼1 h). The effective hourly volumetric
aeration rate supplied to the pile was determined from the sum
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of the two measured blower flows, which were steady during
the sampling period, and their cycle settings (Table S3).
Pollutant mass emitted when the blowers were off was assumed
to be negligible relative to the amount of mass emitted when
the blowers were active, as discussed in the Supporting
Information.
During aerobic composting, organic carbon is biochemically
converted to CO2, which is generally assumed to be part of the
contemporary carbon cycle in which equivalent amounts of
CO2 are resequestered during plant regrowth.12,13 Insufficient
aeration can lead to anaerobic conditions and CH 4
emissions.13,38 Nitrogen transformation can lead to N2O
emissions via nitrification under oxygenated conditions and
denitrification under anoxic conditions. NH3 can also be
formed, depending on aeration, temperature, pH, and initial
ammonium content.10,13,39 There was a large amount of spatial
variability in pollutant concentrations emitted from the
sampled composting surfaces, indicating that these pollutant
formation pathways are not uniform across post-AD digestate
composting windrows. Figure 2 shows the distributions of
emission rates captured from nine measurements of five unique
windrows at various stages in the 14 week composting cycle.
The characteristic emission rate for each measured pile is the
mean value, plotted as a closed circle on each distribution. The
breadth of the boxes and extents of the whiskers show the
range of calculated emission rates based on individual surface
sample concentrations and the windrow’s total aeration rate,
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rather than the exhaust flow rate of any individual surface spot.
The distributions illustrate the variability in the aeration-
normalized concentrations of pollutants across each windrow
surface and potentially significant sampling bias that could
result from an insufficient number of spot samples. Given the
measured surface concentration variability, the mean value of
many surface samplesin this study, 25−73 samples per
windrow for GHGs and 8−19 samples per windrow for NH3
and H2Sis the best representation of the emission rate from
the entire windrow, short of integration over the entire
emitting surface.
Prior studies of composting emissions have used other
measurement techniques, including flux chambers, enclosed
chambers, tracers, inverse dispersion analysis, and micro-
meteorological mass balance.8,9,13,38,40,41 Flux chambers are the
standard protocol for measuring gaseous emission rates from
land surfaces, but these spot measurements may not be
representative of the entire emitting area.42 This is likely
especially true for the composting windrows consisting of
heterogeneous post-AD digestate in the present study. The
other sampling approaches that can capture emissions from an
entire emitting surface or facility were not feasible at Z-Best
due to the close proximity of individual windrows and high
ambient wind speeds. It was not possible to fully envelop the
emitting windrow surface or use downwind measurements to
isolate individual windrow emissions. As such, the high-density
spot sampling method was developed in this study to capture
the spatial variability of emissions of multiple pollutants across
the windrow surface.
The distributions shown in Figure 2 also indicate that there
may be differences in some pollutant emission rates as a
function of composting time or windrow aeration. Previous
work has found differences in CO2 and CH4 over time for
turned green waste and manure piles, whereas there is no
discernible trend with windrow age for these force-aerated,
post-AD digestate windrows.9,13,43 Emissions of N2O, NH3,
and H2S do appear to increase over time, though data on
individual windrows over time is limited. Windrow A-21 Figure 3. Relationship of individual composting spot measurements
of coemitted concentrations of (a) CO2 and CH4 and (b) H2S and
(shown in red) stands out, however, with much higher CH4 NH3. Windrow A-21 is highlighted in red in (a) with a different
and lower CO2 emissions distributions than the other sampled trendline from the other windrows, with more elevated CH4 emissions
windrows. that are likely a function of lower aeration rates and more anaerobic
Figure 3 shows the relationship for individual spot composting conditions.
measurements of coemitted concentrations of GHGs CO2
and CH4 and odorous/toxic species H2S and NH3. For each VOC samples were collected on two additional windrows,
pair of pollutants, a strong linear correlation between emitted each aged ∼4 weeks. These samples were analyzed by two
concentrations indicates a common formation process. The methods: a targeted chemical analysis that included calibrated
significantly elevated CH4/CO2 emission ratio for windrow A- measurements of 102 VOC species and a secondary analysis
21 across the 14 week composting cycle stands out as an that identified a broader suite of 250 species that contribute to
outlier compared to the other sampled windrows: 34% for A- total VOC (TVOC) mass emissions. Some aldehyde and
21 versus 4% for all others. While there are many differences ketone species identified in the targeted analysis are not
across the other windrows, including age, heterogeneous detected in the broader analysis method, including form-
material composition, and aeration levels, the gray dots aldehyde, acetaldehyde, and acetone. These compounds were
generally follow the same trendline. Thus, the difference is added to the TVOC mass, with acetone contributing the most
likely attributed to the set aeration rate, which for windrow A- of the three species. These analytical methods are described
21 was approximately one-third the average aeration of the further in the Supporting Information. The 102 targeted
other windrows (Table S3). A singular strong linear relation- species represented ∼60% of the TVOC mass in these samples,
ship between H2S and NH3 concentrations indicates that the and their emission rates varied by two orders of magnitude
formation process of these species is linked and insensitive to between phthalates and ketones (Figure S18).
this aeration difference, although the sample size for this The average contribution of each chemical class to TVOC
comparison is more limited. Emitted concentrations of CO determined by the broader analysis is shown in Figure 4, with
and CO2 were weakly linearly correlated, whereas there was no an average TVOC emission rate as toluene-equivalents of 18 g
linear relationship between N2O and NH3 (Figure S17). TVOC emitted per hour per windrow. Percent mass
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Environmental Science & Technology
Figure 4. Percent contributions of speciated TVOC emissions from
sampled composting windrows, by chemical class and including 253
total species. Per kg of digestate material composted over 14 weeks,
66 mg of toluene-equivalent TVOC are emitted. The number (n) of
individual species in each class is noted. Chemical classes that
contributed <1% to TVOC emissions were grouped together as other,
including acid, aldehyde, ester, and ethyl compounds.
contributions of the 253 individual VOC species to this TVOC
emission rate are reported in Table S4. Aromatics, alkenes,
alkanes, and terpenoids comprise the largest fractions of
emitted TVOC and together represent two-thirds of the total.
This differs from previous composting studies of green waste
and non-AD MSW, whose emissions were, respectively,
dominated by lighter alcohols that contributed 66−85% and
terpenes that represented ∼50% of total VOC emitted.9,27 On
a mass and time integrated basis, the average emission rate is
equal to 66 mg TVOC emitted per kg digestate material
composted over 14 weeks, assuming these two measurements
are representative of the entire composting cycle. These VOC
emissions, along with other odorous species like NH3, can lead
to odor nuisance concerns.8−11 For example, ZWEDC initially
composted digestate material on-site, but citations for odor
complaints from the surrounding community forced compost-
ing operations off-site instead.
Process Emission Inventory. Table 1 and Figure 5
summarize the emission inventory for the AD-composting
process. Average emission factors are reported by emission
source, with pollutant mass emissions normalized to the mass
of MSW anaerobically digested at ZWEDC. The CO2 emission
rate reported for the flare and CHP units was not measured
but instead calculated using a carbon balance of the
combustion of 1 kg of CH4, equal to 5488 g CO2 per kg
CH4 (see Supporting Information for details). CHP emissions
with inactive SCR are reported to illustrate the influence on
NOx emissions; active SCR is the normal condition.
Per kg of MSW digested, composting dominates emissions
of CH4, CO2, NH3, H2S, CO, and TVOC. Other studies of
post-AD MSW digestate are limited, and the magnitude of
reported emission factors can vary widely. Compared to the
present study, Jensen et al. reported a similar N2O emission
factor for post-AD composting in Germany but found NH3
and CH4 emissions were 1−2 orders of magnitude smaller.14
Beylot et al. found a comparable CH4 emission factor for post-
AD digestate composting in France as is reported in Table 1,
but the present study measured CO2, NH3, and N2O emission
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Figure 5. Average pollutant emission factors for the (a) flare and two
CHP units and (b) four biofilters and 14 week composting cycle. All
pollutant mass emissions are normalized to the mass of MSW
anaerobically digested at ZWEDC. Note that CO2 emission factors
have been scaled down by a factor of 100.
rates that were 7−14 times greater.19 These contrasts could be
due to operational differences that promoted more or less
aerobic conditions than the enclosed, static windrows at Z-
Best. While the windrows in Germany were outdoors, open,
and turned twice a week, the plant in France first composted
their material indoors on an agitated bay with periodic turning
and aeration and then stored this material in outdoor
windrows.
Approximately 60% of biogas combustion CO2 emissions are
from the CHP units while ∼40% are from flaring high- and
low-CH4 biogas, which means that a considerable amount of
CH4 is flared rather than used for power and heat production.
Conversely, less than 20% of NOx emissions are emitted by the
CHP units, indicating the significance of SCR treatment of the
CHP effluent.
NOx emissions are nearly 20 times greater when the CHP’s
SCR system is inactive compared to when it is operational
(Table 1). Similarly, emissions of VOCs would have been
much higher without biofilter treatment of facility air. With the
exception of the halogenated and miscellaneous species (77
and 91% removal efficiency, respectively), the biofilters remove
>95% of each VOC class on average; TVOC removal efficiency
exceeded 98% (Figure S19). Previous studies of biofilter
effectiveness have noted a wide range of VOC removal
efficiencies from ∼40% to >95%, depending on the chemical
family and age of the biofilter substrate.44−46 Jensen et al.
noted a comparable CH4 emission factor ∼1.3 g kg−1 for the
biofilters at a dry AD and composting facility in Germany but
reported NH3 and N2O emission factors that were respectively
7 and 65 times greater than those measured in the present.14
This facility similarly employed a dry, batch AD system, but
Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Environmental Science & Technology
operated under mesophilic (∼38 °C) rather than thermophilic
(∼55 °C) conditions.
Figure 6 shows CO2-equivalent emission rates with units of
g of equivalent CO2 emitted per kg of MSW anaerobically
Figure 6. CO2-equivalent emission factors by source and pollutant
species, based on global warming potential values for a time horizon
of 100 years. CO2 and CO emissions are included in (a) to account
for all emissions, whereas (b) excludes biogenic CO2 and CO as part
of the contemporary carbon cycle. High- and low-CH4 biogas flaring
have been combined into one category of emissions from biogas
combustion at the flare.
digested by pollutant and source. As detailed in the Supporting
Information, these CO2-equivalent emission rates were
determined using the average emission factors reported in
Table 1 and the global warming potential (GWP) values
summarized in Table S5, which include direct and indirect
aerosol affects for a time horizon of 100 years.47−50 CO2 and
CO are included in Figure 6a to account for all emissions and
excluded from Figure 6b to recognize that these biogenic
emissions are part of the contemporary carbon cycle.50,51
Regardless of carbon scenario, GWP-weighted emissions from
composting digestate (62% of the total for all emissions and
69% when excluding biogenic carbon) are greater than the
combined emissions from flaring, power and heat production,
and the facility air treatment system. CH4 comprised 35% of
these emissions from composting when CO2 and CO
emissions are included and 97% of GWP-weighted emissions
when CO2 and CO are excluded. This contribution could be
reduced with increased aeration of the windrows (Figure 3a).
When all emissions are included, the GWP for combustion
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activities is dominated by CO2 emissions that are the result of
the near-complete conversion of CH4 in the biogas to carbon
dioxide during combustion, as intended. However, the CH4
emission rate for the CHP units is nonzero (equal to 24 g kg-
CH4−1; Figure S20), meaning that ∼2% of CH4 is emitted
rather than combusted and converted to CO2. When biogenic
carbon is excluded, this emitted CH4 equates to nearly the
entire GWP footprint of this CHP activity. CH4 emissions
were not measured in the flare exhaust and may be nonzero.
The near-zero BC emissions from high-CH4 biogas flaring had
little impact on the GWP-weighted emission rate. NOx has a
net cooling effect on the climate, such that emitted NOx
reduced overall CO2-equivalent emissions by ∼3% at the flare
when all emissions are considered. When biogenic CO2 and
CO are excluded, NOx emissions dominate GWP emissions at
the flare, resulting in a net negative CO2-equivalent emission
factor. The biofilters contributed 16% of the total CO2-
equivalent emissions for all emissions, with CH4 accounting for
more than half of that total. When biogenic carbon is excluded,
these contributions increased to 27% of total GWP emissions
of which CH4 comprised 95%.
Controlling GHG and toxic/odorous emissions from
composting offer the greatest mitigation opportunity for
reducing the climate and air quality impacts of the AD-
composting process. In particular, the high CH4 contribution
to GWP-weighted emissions suggests that the composting of
post-AD digestate is not completely aerobic. The AD-
composting waste management strategy is favorable to
landfilling, though, and is comparable to other options like
composting MSW directly or upgrading biogas to renewable
natural gas.51 However, the air quality impacts of atmospheric
PM formed from composting NH3 emissions may be
substantial, comprising the largest share of total monetized
climate and air pollution damages for an AD-composting
system.51 NH3 emissions can increase with aeration and
temperature, which are key to maintaining aerobic conditions
that reduce CH4 emissions and sustaining microbial activity for
composting.10,52 Future work should include determining the
optimal windrow management practices that maximize com-
post yield while minimizing CH4 and NH3 emissions.
Technologies to capture and treat composting effluent prior
to emission to the atmosphere could also be developed, such as
coupling biofilters with composting systems.44 In addition,
given the strong relationship established between biogas NH3
content and flare NOx emissions, it is also important to limit
NH3 in flared biogas to minimize contributions to regional
ozone and particulate matter issues. The emission factors
determined in this study can be used to develop emission
inventories and serve as inputs to odor modeling and life-cycle
assessments. More research should be conducted to better
understand how emissions vary across other AD-composting
facilities that may employ different practices and identify
additional emissions mitigation measures that enable greater
deployment of this waste diversion strategy.
■ ASSOCIATED CONTENT
* Supporting Information
sı
The Supporting Information is available free of charge at
https://pubs.acs.org/doi/10.1021/acs.est.0c03953.
Detailed sampling and analysis methods, including
descriptions of facility operations and emission sources,
instrumentation and measurement approaches, and
Environ. Sci. Technol. XXXX, XXX, XXX−XXX
Environmental Science & Technology
pollutant emission rates calculations; and supplementary
emissions results for the flare, composting windrows,
biofilters, and CHP units (PDF)
■
AUTHOR INFORMATION
Corresponding Author
Chelsea V. Preble − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States; Department of Civil and Environmental
Engineering, University of California, Berkeley, California
94720, United States; orcid.org/0000-0002-6489-5718;
Email: cvpreble@berkeley.edu
Authors
Sharon S. Chen − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States
Toshifumi Hotchi − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States
Michael D. Sohn − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States
Randy L. Maddalena − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States
Marion L. Russell − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States
Nancy J. Brown − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States
Corinne D. Scown − Energy Technologies Area, Lawrence
Berkeley National Laboratory, Berkeley, California 94720,
United States; orcid.org/0000-0003-2078-1126
Thomas W. Kirchstetter − Energy Technologies Area,
Lawrence Berkeley National Laboratory, Berkeley, California
94720, United States; Department of Civil and
Environmental Engineering, University of California,
Berkeley, California 94720, United States
Complete contact information is available at:
https://pubs.acs.org/10.1021/acs.est.0c03953
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
This work was supported by the California Energy
Commission under Contract No. EPC-14-044 and the
Department of Energy under Contract No. DEAC02-
05CH11231. The statements and conclusions herein are
those of the authors and do not necessarily reflect the views
of the project sponsors. The authors thank Greg Ryan, John
Pena, Osvaldo Cordero, James Moore, and Amelin Norzamini
of the Zero Waste Energy Development Company and John
Doyle, Fred Ochoa, and Beto Ochoa of Z-Best Products for
their partnership in conducting this work, including access to
their facility and to their facility data; the Bay Area Air Quality
Management District for use of their mobile laboratory; and
the many students who contributed to this study, including
Nick Tang, Brandon Yee, Yannick Johnson, Marie-Anne Hatte,
Caroline Loffredo, Isabelle Kavanagh, and Kelly Archer.
I https://dx.doi.org/10.1021/acs.est.0c03953
■
pubs.acs.org/est Article
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