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Airborne Methane Emission Measurements for Selected Oil and Gas Facilities Across California Shobhit Mehrotra, Ian C. Faloona, Maxime Suard, Stephen A. Conley, and Marc L. Fischer Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.7b03254 • Publication Date (Web): 11 Oct 2017 Downloaded from http://pubs.acs.org on October 12, 2017
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Airborne Methane Emission Measurements for Selected Oil and Gas Facilities Across California Shobhit Mehrotra1, Ian Faloona1, Maxime Suard1, Stephen Conley1,2, and Marc L. Fischer3,4* 1
Land Air and Water Resources, University of California, Davis, California 95616
2
Scientific Aviation, Inc., Boulder, Colorado 80301
3
Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720 4
Air Quality Research Center, University of California, Davis, California, 95616
ABSTRACT
We report 65 individual measurements of methane emissions from 24 oil & gas facilities across California. Methane emission rates were estimated using in-situ methane and wind velocity measurements from a small aircraft by a novel Gauss' Theorem flux integral approach. The estimates are compared with annual mean emissions reported to the US-EPA and the California Air Resources Board (CARB) through their respective greenhouse gas reporting programs. The average emissions from 36 measurements of 10 gas storage facilities were within a factor of 2 of emissions reported to US-EPA or CARB, though large variance was observed and the reporting database did not contain all of the facilities. In contrast, average emissions from 15 measurements of the three refineries were roughly an order of magnitude more than reported to
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the US-EPA or CARB. The remaining measurements suggest compressor emissions are variable and perhaps slightly larger than reported, and emissions from one oil production facility were roughly concordant with a separate (not GHG reporting) bottom-up estimate from other work. Together, these results provide an initial facility-specific survey of methane emissions from California oil and natural gas infrastructure with observed variability suggesting the need for expanded measurements in the future.
* Corresponding Author Marc L. Fischer; Phone (510)-486-5539; Email (
[email protected])
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1. INTRODUCTION 1
US Natural Gas (NG) consumption has increased 70% from 16.2 to 27.5 trillion cubic feet per
2
year from 1986 to 2016 [1]. NG is composed of approximately 80-90% methane (CH4), a very
3
potent greenhouse gas (GHG), which has a global warming potential (GWP) of 34 and 86 times
4
that of CO2 on a 100- and 20-year time scales, respectively [2]. Therefore production, storage,
5
transport, and consumption of NG must be carefully monitored to ensure that methane is not lost
6
to the atmosphere, undercutting its environmental benefit as a relatively clean energy source. For
7
example, the above GWP of 86 (gCO2eq/gCH4) suggests that if 3.3% of CH4 is emitted
8
unburned, it will produce warming roughly equivalent to the remaining 97% of CH4 carbon that
9
is combusted to CO2 on a 20 year timescale. Similarly, it has also been estimated that if more
10
than 3.2% of NG is lost before combustion, the global warming impact would be the same as an
11
equivalent output from coal powered plants [3].
12
According to the annual report of Greenhouse Gas Emissions and Sinks released by the US
13
Environmental Protection Agency (US-EPA), methane emissions from oil and gas operations
14
account for about 6% and 25%, respectively, of the national methane emissions inventory [4]. In
15
California, most natural gas is imported and the Air Resources Board (CARB) estimates oil and
16
gas production, processing, transmission, and distribution contribute a total of only 16% of the
17
state's methane emissions [5], with the bulk of this (~10%) coming from the natural gas
18
transmission and distribution system. However, statewide methane emissions might be expected
19
to grow as demand for power generation from NG climbed 30% from 2001 to 2012 [6]. Here,
20
roughly 90% of the natural gas used in California is imported to the state (as of 2013), primarily
21
from the Anardarko and Permian Basins in Texas (38%), the Rocky Mountain Basin (36%), and
22
the Western Canadian Sedimentary Basin (16%) [7,8].
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In California, total natural gas storage has increased about 24% in the last 25 years as shown in
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Figure 1 [9]. In addition, there are also both large seasonal variations and smaller inter-annual
25
variations. Seasonally, NG storage typically peaks at the end of the summer when NG utilization
26
and typically reaches a minimum sometime in March following larger winter demand for space
27
heating drops. In the context of this work, it is worth noting that storage facility emissions might
28
depend more on the amount of stored gas (e.g., more emissions at higher pressures) or on the rate
29
at which gas is injected or removed (e.g., leaks in gas handling infrastructure).
California Natural Gas Methane Underground Storage Mass Mass Stored Methane (Gg)
12,000 10,000 8,000 6,000 4,000 2,000 0 Jan-1990
Jan-1994
Jan-1998
Jan-2002
Jan-2006
Jan-2010
Jan-2014
Year
Figure 1. The monthly total mass storage of NG methane in California (assuming 95% CH4 composition.) The black curve is a 12-month running average. Despite a large seasonal variation it is clear that storage masses have been increasing at about 1.5% per annum (~120 Gg/yr) since the turn of the century [1]. 30
Previous work has measured methane emissions from natural gas related facilities, with three
31
studies particularly relevant to our current work. First, a study of methane emissions from 45 US
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compressor stations (all outside California), found that roughly 10% of the stations emitted 50%
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of the methane emissions and the lowest 50% of emitting sites only contributed to 10% of the
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emissions, citing equipment malfunctions (e.g., leaky isolation valves and compressor vents) as
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major fugitive leak sources. [10]. Second, a study of three refineries (in Utah, Indiana, and
36
Illinois), average emissions ranged from 360-830 kg/hr, as compared with a range of 4 to 51
37
kg/hr reported by industry to the US-EPA [11]. Third, a natural gas injection and recovery well
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at the Aliso Canyon gas storage facility failed in November, 2015, releasing approximately 97
39
Gg CH4 before being repaired in February, 2016 [11], equivalent to roughly half of total annual
40
oil and gas related methane emissions (~ 220 Gg CH4/yr) estimated by the California Air
41
Resources Board (CARB) [5].
42
In this study, we describe facility level measurements of CH4 emissions for a subset of natural
43
gas infrastructure in California including gas storage facilities, petroleum refineries (which use
44
NG for power), an oil and gas production field, a gas fired power plant, and several natural gas
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processing or compression stations. We begin with a methods section describing sites we
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observed and airborne instrumentation, the mass-balance approach to estimate emissions and
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sources of uncertainty in the estimates. In results, we describe the emissions estimated for the
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different facilities and, where we collected multiple measurements over time, estimates of the
49
mean emissions and their variability. As part of the results and discussion, we also compare
50
measured emissions with annual average emissions reported by industry to the US-EPA and
51
CARB for a subset of the facilities, though note that the facility reported emissions should be
52
distinguished from official inventories for national or state level emissions. 2. MEASUREMENT SITES and METHODS
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2.1 Measurement Sites Observed in this Study
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A total of 24 facilities were measured in the course of this airborne study on 34 individual days
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spanning 27 months from June, 2014 to September, 2016 (see table S1). Eight storage facilities,
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three refineries, and seven compressor stations were measured for methane and ethane (after
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September, 2014). Ethane measurements provide not only an unambiguous marker of fossil fuel
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sources, but further establish a quantitative measure of the ratio of ethane to methane that can be
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compared with pipeline gas supplied by utilities for regional source apportionment. McDonald
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storage, Rodeo refinery, and Kirby storage which were measured eleven, seven, and seven times
61
respectively, have enough data sets that we can begin to estimate variations over time. These
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facilities use (storage facilities may use gas to power compressor engines) and emit natural gas
63
during their operation, making them of key interest when attempting to quantify GHG emissions
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from California’s natural gas infrastructure. The facilities were sampled on randomly chosen
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days (during favorable meteorological conditions), without communication with facility
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operators. As such, we are not aware of site status or operations conditions at the time of
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sampling. In addition, we measured the Elk Hills and Los Medanos power plants and the
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Belridge South petroleum production field in the Southernwestern San Joaquin valley, though
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note that the Los Medanos plant is co-located with underground gas storage. As described below,
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while Belridge South was sampled three times, two samples were considered incomplete due to
71
cloud cover limiting the aircraft's ability to climb (11/3/15), and another with very low and
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meandering wind (6/17/14). Therefore, we report only one complete sampling of Belridge South
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and one for Elk Hills power station, preventing us from making any assessment of variability in
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emissions for those sites. 2.2 Cylindrical Mass-balance Emission Measurements.
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To quantify facility emissions a cylindrical flight pattern was employed to measure gas
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concentration gradients and wind velocities and then calculated facility emissions as the
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divergence of mass flux within the flight cylinder using Gauss’s Theorem as described by
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Conley et al. [12]. Using this mass balance (or conservative scalar budget) approach, the
79
emissions from a site, E, can be expressed as: 1 =
′ ∙
80
where the outer integral represents the vertical extent of the cylindrical flight pattern which
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extends from the lowest safe altitude, zmin, to the maximum flight altitude, zmax, where there is no
82
indication of a plume crossing. Due to FAA regulations, the minimum safe altitude the aircraft
83
can be flown is 500 feet above ground level (AGL) or approximately 150 m. As of October
84
2015, special permission was granted to Scientific Aviation, Inc. by the FAA to fly as low as 200
85
feet (60 m) AGL over unpopulated areas. This lower limit allows a greater altitude range of
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measurements which improves accuracy and reduces error as discussed in Section 2.3. The
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integrand in Eq. 1 is the path integral representing the dot product of the horizontal advective
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. Here c' represents the fluctuating methane flux, c'uh, and the vector normal of the flight path,
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or ethane density multiplied by uh, the horizontal wind vector. Details of the method are
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explicated in Conley et al. [12]. The benefit of using closed loops as opposed to traditional
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horizontal transects is that emissions can be assumed to be coming from a confined regional
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source, therefore individual wells, refineries, and storage facilities can be accurately quantified in
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a manner that minimizes confusion with other surrounding sources. When calculating emissions,
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a flux divergence profile is generated from altitude binned averages of each flight loop around
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the source, and the total emission rate is calculated as the integral under this curve (Eq. 1). In
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order to average over natural turbulent variability of each loop's flux divergence, the
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measurements are first averaged in altitude bins of approximately 100 m depth. The orange
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diamonds shown in Figure 2 represent each loop flown and the blue circles represent a binned
99
average that consists of loops in a specified altitude segment. The bottom altitude bin is then
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extrapolated to the ground with a vertical line, which is shown to be sufficiently accurate by
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Conley et al. [12] in a certain range of distances downwind of the source. Further discussion of
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the errors associated with this extrapolation are taken up in Section 2.3.
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Figure 2. (left) Flux divergence profiles that are created from each loop's flight data (orange
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diamonds) to estimate the total emission strength and its associated error. Solid blue circles are
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the binned averages, and the light blue line extending down from the lowest point is the
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extrapolated flux divergence representing the “ground contribution term”, which is assumed
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based on LES simulations. (right) The standard deviation measured on each loop around the
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source. The data is from the McDonald Storage Facility May 18th, 2016.
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The aircraft and instrumentation utilized for this study is described in detail by Conley et
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al., [12] and reviewed briefly here. The aircraft is a Mooney TLS M20 high performance single
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engine aircraft modified for air sampling. Primary instruments used for this campaign were the
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Picarro methane and carbon dioxide cavity ring down spectrometer and an Aerodyne ethane gas
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analyzer. The Picarro samples the air every 0.55 seconds and has a lag time of 9 to 12 seconds,
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where the Aerodyne samples the air every 0.81 seconds and has a lag time of 5 to 9 seconds. The
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lag time depends primarily on the size of the inlet lines and the sampling flow rate of the air.
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This was verified routinely by performing “breath tests,” where a person would abruptly blow
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into the inlet and the delay in instrument response would be timed. The tubes were modified
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once during the campaign which altered the lag time and was considered when making estimates.
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Data from the gas analyzers were interpolated onto a GPS time stamp for analysis. True wind
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velocities in the meridional and zonal directions are computed from the difference of the aircraft
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velocity relative to the ground (from the GPS), and the velocity of the aircraft relative to
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surrounding air (measured with pressure sensors) [12].
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2.3 Uncertainty Estimation
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In order to verify the accuracy of the cylindrical mass balance method, controlled releases
125
of known source strength were sampled on several occasions and the analysis is reported by
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Conley et. al. [12]. From those tests accuracies of the measurements are thought to be 15% or
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better with an average accuracy of 6%. We note that the controlled release experiments were
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generally sampled under optimal conditions, and took place over the course of the field results
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discussed here while continual improvements were being made to the sampling technique. Thus,
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the average error representative of the estimates reported in this study are likely greater than the
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results of the controlled releases and reported in Conley et al. [12]. In this paper, we estimate the
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uncertainty under less ideal flight conditions, and include parameterization for 1) the number of
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loops flown, 2) the proximity to the source, 3) the variability of the wind during the observation,
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and 4) a binning error introduced by estimating emissions in a finite set of altitude intervals.
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Here, the binning error is estimated by varying the number of bins and examining the variation in
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total emissions for the different number of bins chosen. Figure S1 shows an example of the
137
derived emission estimate as a function of number of bins derived from a controlled release, and
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shows a standard deviation of approximately 10% of the mean due to different binning.
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First, we turn to the uncertainty due to not capturing horizontal efflux below the lowest
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leg of the aircraft profile. In their detailed explanation of the airborne measurement method,
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Conley et al. [12] show theoretical flux divergence profiles from LES simulations that indicate a
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nearly constant flux divergence below the lowest altitude leg but only when the distance at which
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the plume is sampled (in terms of advection time, x/U, distance divided by mean horizontal wind
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speed) is approximately one-half the large eddy turnover time (zi/w*), where zi is the atmospheric
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boundary layer (ABL) depth and w* is the convective velocity scale, an estimate of vertical wind
146
vigor in turbulent boundary layers dominated by convective forcing based on the surface
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buoyancy flux). A non-dimensional distance (X) is derived to normalize the physical distance
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from the source with the mean wind speed encountered while sampling. This allows us to more
149
accurately determine the fraction of the plume that slipped under the lowest flight leg. 2 =
∗
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While the theoretical treatment in Conley et al. [12] shows variations in the slopes of the
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near surface flux divergence profiles, we do not try to incorporate deviations from the constant
152
vertical extrapolation based on the sampling distance downwind of the source in our error
153
estimates here because the difference appears to be usually less than ~15%, and the average non-
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dimension downwind distance of 0.56 ± 0.36 is close to 0.45, the downwind distance where
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vertical extrapolation is considered ideal. Nevertheless, the fraction of the plume that has to be
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inferred below the minimum flight altitude is a function of how close the downwind leg is to the
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source, and has some bearing on the uncertainty of the emission estimate. This source of error is
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parameterized by a fraction of the emissions that are below the lowest leg, FB, scaled by the
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complement of a normal distribution centered at the optimal non-dimensional distance
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downwind of the source (X≈0.45), with expected variance of the form
161
(3)
162
where the vertical extrapolation to the surface is found to be most accurate [12]. In short, the
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fraction below can be estimated with a high degree of certainty if the non-dimensional distance is
164
close to 0.45, but this was not explicitly understood throughout the period of this study and our
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parameterization is a simple attempt to conservatively estimate this sampling shortcoming.
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/
1/3"1 − $% ∗ & '|)'*.,-| . ,
Second, we consider how our error varies with the number of loops flown around each
167
facility. Based on the analysis of flight data around controlled releases and large eddy
168
simulations Conley et al. [12] show that estimates asymptotically approach actual values and are
169
within 15-20% after approximately 20 sampling flight loops. In order to capture the general
170
behavior of this sampling limitation we use a simple logistic curve that approximates the
171
diminishing variability of the estimates as the number of loops, NL, increases, saturating after
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25-30 flight loops, as additional loops do not appear to improve the error estimate significantly.
173
The parameters in the logistic function such as the offset of 8 loops and the multiplier of 0.15
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were determined 'by eye' from the controlled release data and were chosen to generate a
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conservative estimate of the error variance associated with this under sampling of the source of
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the form
1
/ .
177
(4)
178
The third source of uncertainty we include is that due to the lack of consistency of the
123 45.67∗894:
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wind velocity during the observations. Here, we define a dimensionless wind consistency
180
parameter, WC, as the ratio of the vector mean wind speed to the average wind speed during the
181
flight sampling [12].
(5)
WC =
;∑= > 2∑? > ∑ @=> 2?>
where, ui and vi are the instantaneous meridional and zonal winds speeds respectively. This indicates the degree of variability in the wind direction as described by Stewart et. al [13]. Ideal winds are considered to blow consistently from the same direction during the sampling (which would yield a wind consistency value of 1.) It is generally seen that stronger winds yield a higher wind consistency and this, in principle, leads to greater precision in the emission estimates. For most cases the wind consistency parameter was above 0.8 and thus we do not expect that this was a dominant source of error in the measurements presented herein. 182 183
Taking these three terms together we estimate a generic quality factor for each emission estimate based on the sampling conditions:
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(6)
1
1
1
1
Q = @A 1 − $% ∗ & '|)'*.,-| / + A 123 45.67∗894: / + A CD /
where, Q = Quality Factor WC = Wind consistency FB = Fraction Below (fraction of estimate measured when extrapolating to the surface) X = mean non-dimensional distance from the source LN = complete loops flown around the site 184
Beyond the sampling characteristics, there is an inherent variability in the method that
185
arises from the arbitrary number of altitude bins into which loops are averaged before evaluating
186
the flux integral of Eq. 1. Emission estimates vary 11% on average, depending on the exact
187
number of altitude bins, and we include this variability into the error estimates. This was
188
determined by taking the standard deviation of the emission estimates when varying the number
189
of altitude bins from two to the number of loops flown for all of the data gathered for each
190
facility during this campaign. The binning error (BE) is then averaged to derive the mean
191
emission estimate and the relative standard deviation of this mean is added in quadrature with (1-
192
Q), an approximate measure of the relative error induced by inadequacies of sampling, to
193
determine the overall relative error estimate.
(7)
TC = E;%/ + 1 − F/ G × ||
where,
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TC = total uncertainty E = emission estimate 194 195
3. RESULTS Here, we report emission estimates for the facility observations. Individual
196
measurements of methane emissions together with 1 sigma uncertainties from Eq. 7 are reported
197
in Table S-2, and an example image of a cylindrical observation shown in Figure 3. Summary
198
statistics for methane emissions (averages and standard deviations) are then reported for
199
individual facilities in Tables 1, 2, 3. Here, average emissions from some facilities were similar
200
to 2015 emissions reported by industry to the US-EPA Greenhouse Gas Reporting Program [14]
201
and/or the California Air Resources Board Reporting Program [15], while others emitted more
202
during the observation periods than the average annual rates reported.
203
3.1 Storage Facilities. Overall the results indicated a great amount of variability in
204
emissions relative to documented estimates. As shown in Table 1, emissions were reported to the
205
US-EPA and CARB for 3 and 7 facilities, respectively. The largest storage facility of the
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campaign (82 Bcf working capacity), McDonald Island was visited 11 times and displayed
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irregular statistically significant variations in emissions. On May 12th, 2015 McDonald was
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emitting 22 ± 14 kg/hr then a few hours later it was measured at 93 ± 34 kg/hr, while the next
209
day we measured 187 ± 48 kg/hr. Despite the large variance (roughly 50% of the average)
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observed across all the samples, average emissions were 2.6 times higher than industry reporting
211
to CARB. Kirby, which was visited seven times, had an emission range from essentially 0 to
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150 +/- 51 kg/h with an average which is nine times higher than reported to CARB. Honor
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Rancho which was sampled twice measured at 835 ± 215 kg/hr and -20 ± 37 kg/hr in June and
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September of 2016 respectively, where we note that the negative value is essentially consistent
215
with zero emissions to within the measurement uncertainty. Wild Goose was sampled four times
216
and on one occasion was not emitting any detectable CH4 (< ~5 kg/hr), though the compressor
217
station was physically separated from the storage field and was observed to emit 167 +/- 42 kg/hr
218
on the one day the compressor station was measured. Due to highly variable temporal changes in
219
emissions for storage facilities, numerous samples such as were sampled from the McDonald
220
Island facility are needed for all the facilities to better understand the role of temporal variability
221
in the overall annual emissions as identified in previous studies [16]. Statistical analysis as well
222
as an in-depth look at the temporal variability for McDonald will be discussed in the following
223
section. Here, we note that the Honor Rancho storage facility is collocated with oil and gas
224
production field and the Los Medanos storage facility also contains a gas fired electricity power
225
plants, leaving some question as to what part of the measured emissions should be attributed to
226
the storage facility infrastructure. Table 1. Storage facility characteristics, and average (with standard deviation and number of measurements when N >1) measured and reported methane emissions (kg CH4/h)
Facility Name Gill Ranch Honor Rancho Kirby La Goleta Lodi Los Medanos* McDonald Pleasant Creek Princeton
Working Storage (Bcf) 20 24 15 22 9 18 82 2 11
Min
Max
Avg. (Std. Dev, N)
US-EPA (2015)
CARB (2015)
5 -21 -10 24 22 8 -
59 835 150 38 461 24 -
33 (27, 3 ) 407 (605, 2) 55 (54, 7) 215 -90 33 (7, 3) 223 (144, 11) 16 (9, 4) 43
55 2 -
63 15 1 3 49 -
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Wild Goose** 75 -3 105 35 (61, 3) *Los Medanos contains both gas storage and power generation
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** Excludes measurement of compressor near Wild Goose storage field 227
3.2 Refineries. By far the greatest discrepancies between reported and measured methane
228
emissions were found for the three refineries that were sampled a total of 15 times, with results
229
shown in Table 2. On average the three refineries emitted roughly an order of magnitude as
230
much methane than reported to US-EPA or CARB. Here, Benicia had average measured
231
emissions of 382 kg/hr over the seven visits, between 12 and 4 times that reported US-EPA and
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CARB respectively. Martinez refinery, sampled thrice, emitted an average of 260 kg/hr ,
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between two and four times the reported values. Last, Rodeo, was visited five times had an
234
average emission of 306 kg/hr (albeit with a large) that was roughly 30 times that reported.
235
Unlike storage facilities, the refineries were consistently observed to emit significantly more than
236
the annual average emission rate reported to the US-EPA and CARB. Here, we note that our
237
observations do now allow us to determine what portion of methane emissions come directly
238
from petroleum feed stocks or products and what portion come from natural gas used for heat
239
and power at the facilties. Table 2. Measured and reported methane emissions with statistics as above for refineries (kg CH4/hr)
Facility Name Benicia Martinez Rodeo
Min 220 239 23
Max 700 283 527
Average US(Std.Dev, EPA N) (2015) 382 (185, 7) 30 260 (22, 3) 138 306 (206, 5) 11
CARB (2015)
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Figure 3. Observed CH4 mixing ratios for loops surrounding Benicia refinery, on May 23rd, 2016. Downwind CH4 of the flight pattern show clear enhancements relative to the upwind. The mean wind direction is shown by the black arrow in lower left. 240
3.3 Power Plants, Production Fields, and Processing/Compressor Stations. The
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majority of natural gas used in California is transported from out of state in transmission lines
242
that require compression and so nine compressor stations were observed once each in this study,
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with results shown in Table 3. Here, methane emission varied significantly, from barely
244
observable at the Hanford compressor to over 230 kg/hr measured at the Blythe compressor
245
station. On the basis of these limited observations, about half the compressor stations appeared to
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emit more than the annual averages reported, but having only one observation each prevents us
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from drawing strong conclusions about average emissions from any individual facility.
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Table 3. Measured and reported methane emissions for compressor, oil production, power
249
stations (kg CH4/hr)
250
Min
Max
Avg (Std. Dev)
US-EPA (2015)
CARB (2015)
Compressor
-
-
235
6
58
Burney
Compressor
-
-
73
-
49
Hanford
Compressor
-
-
3
13
-
Mettler
Compressor
-
-
93
10
8
Moreno
Compressor
-
-
43
44
11
Needles
Compressor
-
-
12
-
44
Newberry
Compressor
-
-
72
1
-
Panoche
Compressor
-
-
158
-
1
Wild Goose
Compressor
-
-
167
-
51
Elk Hills
Gas Processing & Power Plant
334
533
433 (141, 2)
16
23
Belridge South
Oil Field
63
1953
827 (996, 3)
-
-
Facility Name
Facility Type
Blythe
In addition to the compressor stations, the Belridge South oil production and processing
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field was observed three times, but for reasons described below only one set of measurements are
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valid. Emissions from the combination of a gas processing station and a power plant at Elk Hills
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were observed twice. Because of its comparatively large size the Belridge South field required
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15 minutes to loop once, requiring at least three hours to obtain even 12 loops. Here, emissions
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ranged from 63 to 1,953 kg/h, with only one of the measurements meeting the above
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requirements and emissions roughly consistent with an estimate of production and processing
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emissions derived from a bottom up mapping of oil and gas related methane emissions reported
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by Jeong et al. [17]. Because of its smaller size both observations of the Elk Hills gas processing
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and power plant were made with many loops and yielded comparatively consistent methane
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emissions estimates that were within a factor of two emissions reported to CARB, but appear
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higher than those reported to US-EPA.
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Section 3.6 Analysis of Variability. We next examine the significance of observed temporal
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variability for the four facilities which were measured 5 or more times. Under the assumption
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that the observations were normally distributed and the average of estimated uncertainties
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captures the measurement related variation in the observations, we evaluate F statistics, as the
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ratio of observed variance in emissions to the average of the estimated uncertainties. We then
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computed the corresponding probabilities, p, that one would exceed the observed values of F,
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given the number of samples collected for N-1 degrees of freedom. As shown in Table 4, the F-
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statistics and p-values of exceeding F is significant at the p < 0.05 for three (Benicia, McDonald
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and Kirby). Table 4. F-test results for facilities sampled more than once
Facility Name
Benicia
Facility Type
Refinery
Average Estimate (kg/hr)
Variance
382
29412
(kg/hr)2
Average Uncertainty squared
Average F ratio
(kg/hr)2
(-)
11080
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2.65
prob (-)
0.03
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Kirby
Storage
55.4
2500
586
4.27
0.00
McDonald
Storage
223
18906
2455
7.70
0.00
Rodeo
Refinery
306
34040
17408
1.96
0.11
Based on the F-test results it appears that emissions at a majority of the sites we sampled
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repeatedly were more variable than expected based on the estimated errors. McDonald Island
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was sampled 11 times and was observed to have the largest and most variable emissions
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observed during this two-year campaign. The cause of such a high variance is uncertain at the
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time, but is likely due to intentional venting during maintenance operations reported for the site
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(PG&E private communication).
277 278
Section 3.7 Discussion This work quantifies methane emissions from a sampling of California natural gas
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facilities. A total of 24 unique sites were sampled, with ten storage facilities, three refineries,
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seven compressor stations, an oil production field, and the combination of gas processing and
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nearby power plant.
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The storage facilities were measured frequently and differed by less than a factor of 2
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from available reporting. One exception was the McDonald Island storage facility that exhibited
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large and variable emissions, likely associated with maintenance operations at the site. We note
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that although the average of measurements was within a factor of two of the average reported,
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high variability was observed, suggesting the need for additional measurements, perhaps at other
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times of day when operations might differ. Here we also note that the CO2 emissions were
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generally below the limit of detection, consistent with there being much smaller combustion than
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for the refineries or power stations.
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Three petroleum refineries were found to be the largest methane emitters, with emissions
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roughly an order of magnitude larger than that reported to the US-EPA or CARB during the 15
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samplings. These observations are similar to those reported previously where three refineries in
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three different states showed emissions that were on average eight-fold higher than reported [16].
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Because of the large discrepancies, we also compared measured and reported carbon dioxide
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emissions CO2 emissions, which for the refineries are roughly 1,000 times greater than the
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methane emissions. Unlike methane, Table 5 shows that the average CO2 emissions measured
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during the flights agree with reporting to within 50% for all three facilities, suggesting that the
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measurements might reasonably be expected to approximate average from these facilities and
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hence that methane emissions are likely under-reported. In addition, CO2 emissions from the Elk
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Hills power station were measured to be quite similar on both days of observation, and quite
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consistent with annual reporting to CARB, though lower than annual reporting to US-EPA. To
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the best of our understanding, differences in which components are included in reporting may
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provide an explanation for the differences in emissions reporting to the two agencies. Table 5. Measured and reported carbon dioxide emissions (Mg CO2 /hr) for the subset of facilities with clearly measurable emissions.
Facility Benicia Martinez Rodeo Elk Hills
Min -4 155 152 133
Max
Average
445 275 407 140
285 223 235 137
Std.Dev 157 62 105 5
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US EPA (2015) 341 386 168 231
CARB (2015) 323 468 150 231
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The emissions measured at the nine compressor stations were in the same range as
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storage facilities. While we were generally not able to separate compressor emissions from
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subsurface leakage, this raises the likelihood that a significant fraction of methane emitted from
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storage facilities may be associated with compressors. In one case, emissions measured at Wild
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Goose subsurface storage were physically separated from the Wild Goose compressor and
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smaller than the single measurement of Wild Goose compressor emissions. Since compressor
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stations are expected to emit variable amounts of methane depending on their operation and
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maintenance operations, this suggests a value in coordinating some fraction of measurements
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with site operators.
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This work is an initial sampling and only captures total emissions without resolving the sub-
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facility components responsible for the majority of emissions. In order to improve annual
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average emission estimates and capture variations, future measurements of California natural gas
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facilities are needed. Here, it will be important to both measure facilities either more frequently
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using the methods described here, continuously (e.g., fenceline monitoring), and apply methods
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that provide sufficient spatial resolution (e.g., infrared plume imaging) to identify and remediate
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emissions from the components responsible for emissions. ACKNOWLEDGEMENTS
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This analysis was supported by the California Energy Commission’s Natural Gas Research
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Program under contracts 500-12-006 and 500-13-005. IF is supported in part by the California
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Agricultural Experiment Station, USDA National Institute of Food and Agriculture project #CA-
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D-LAW-2229-H. Work by MLF was performed at LBNL under U.S. Department of Energy
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Contract No. DE-AC02-05CH11231. The statements and conclusions in this paper are those of
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the authors and not necessarily those of the California Energy Commission. The views and
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opinions of authors expressed herein do not necessarily state or reflect those of the United States
328
Government or any agency thereof, or The Regents of the University of California. Ernest
329
Orlando Lawrence Berkeley National Laboratory is an equal opportunity employer nor do
330
references herein to any specific commercial product, process, or service by its trade name,
331
trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement,
332
recommendation, or favoring by the United States Government or any agency thereof, or The
333
Regents of the University of California.
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Supporting Information: Supporting information includes a table summarizing all the facilities
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measured, including facility type, location, and number of times each was measured, a second
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table reporting measured data for each facility and observation date, and a figure showing the
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variation in estimated emission as a function of the number of vertical bins used to average
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observations for an example measurement during a controlled release test.
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REFERENCES [1] U.S. Energy Information Administration, U.S. Natural Gas Total Consumption. Web. 02 June, 2017. https://www.eia.gov/dnav/ng/hist/n9140us2a.htm [2] "Global Warming Potentials." Global Warming Potentials. United Nations, 2014. Web. 04 July 2015. http://unfccc.int/ghg_data/items/3825.php [3] Alvarez, R. A.; Pacala, S. W.; Winebrake, J. J.; Chameides, W. L.; Hamburg, S. P. Greater focus needed on methane leakage from natural gas infrastructure. Proceedings of the National Academy of Sciences 2012, 109 (17), 6435–6440. [4] U.S. Environmental Protection Agency, Inventory of U.S. Greenhouse Gas Emissions and Sinks from 1990-2015. https://www.epa.gov/ghgemissions/inventory-us-greenhousegas-emissions-and-sinks (accessed 14 June 2017). [5] "Methane (CH4)." CH4. Air Resources Board, 6 May 2015. Web. 03 Feb. 2016. https://www.arb.ca.gov/cc/inventory/background/ch4.htm [6] "Supply and Demand of Natural Gas in California." California Natural Gas Data, Facts, & Statistics. California Energy Commission, n.d. Web. 03 Feb. 2016. http://www.energy.ca.gov/almanac/naturalgas_data/overview.html [7] Brandt, A. R.; Heath, G. A.; Kort, E. A.; O'sullivan, F.; Petron, G.; Jordaan, S. M.; Tans, P.; Wilcox, J.; Gopstein, A. M.; Arent, D.; et al. Methane Leaks from North American Natural Gas Systems. Science 2014, 343 (6172), 733–735. [8] "California Underground Natural Gas Storage Capacity." California Underground Natural Gas Storage Capacity. US Energy Administration, n.d. Web. 03 Feb. 2016. https://www.eia.gov/dnav/ng/ng_stor_cap_dcu_SCA_a.htm [9] Subramanian, R.; Williams, L. L.; Vaughn, T. L.; Zimmerle, D.; Roscioli, J. R.; Herndon, S. C.; Yacovitch, T. I.; Floerchinger, C.; Tkacik, D. S.; Mitchell, A. L.; et al. Methane Emissions from Natural Gas Compressor Stations in the Transmission and Storage
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