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Energy and the Environment
Vehicle-based methane surveys for finding natural gas leaks and estimating their size: validation and uncertainty Zachary Weller, Joseph Robert Roscioli, W. Conner Daube, Brian K. Lamb, Thomas Ferrara, Paul E. Brewer, and Joseph C. von Fischer Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.8b03135 • Publication Date (Web): 20 Sep 2018 Downloaded from http://pubs.acs.org on September 21, 2018
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Vehicle-based methane surveys for finding natural gas leaks and estimating their size: Validation and uncertainty Zachary D. Weller,∗,†,‡ Joseph R. Roscioli,¶ W. Conner Daube,¶ Brian K. Lamb,§ Thomas W. Ferrara,k Paul E. Brewer,⊥ and Joseph C. von Fischer† 1
†Department of Biology, Colorado State University, Fort Collins CO 80523 USA ‡Department of Statistics, Colorado State University, Fort Collins CO 80523 USA ¶Aerodyne Research Incorporated, Billerica, MA 01821 USA §Laboratory for Atmospheric Research, Department of Civil & Environmental Engineering, Washington State University, Pullman, WA 99164 USA kGHD Services Incorporated, Niagara Falls, NY 14304 USA ⊥Smithsonian Environmental Research Center, Edgewater, MD 21037 USA E-mail:
[email protected] 2
Abstract
3
Managing leaks in urban natural gas (NG) distribution systems is important for
4
reducing methane emissions and costly waste. Mobile surveying technologies have
5
emerged as a new tool for monitoring system integrity, but this new technology has
6
not yet been widely adopted. Here, we establish the efficacy of mobile methane surveys
7
for managing local NG distribution systems by evaluating their ability to detect and
8
locate NG leaks and quantify their emissions. In two cities, three-quarters of leak indica-
9
tions from mobile surveys corresponded to NG leaks, but local distribution companies’
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field crews did not find most of these leaks, indicating that the national CH4 activity
11
factor for leaks in local NG distribution pipelines is underestimated by a factor of 2.4.
12
We found the median distance between mobile-estimated leak locations and actual leak
13
locations was 19 m. A comparison of emission quantification methods (mobile-based,
14
surface enclosure, and tracer-ratio) found that the mobile method over-estimated leak
15
magnitude for the smallest leaks, but accurately estimated size for the largest leaks that
16
are responsible for the majority of total emissions. Across leak sizes, mobile methods
17
adequately rank relative emission rates for repair prioritization, and they are easily
18
deployed and offer efficient spatial coverage.
19
1
Introduction
20
Repairing natural gas (NG) leaks in urban distribution systems has significant environmental,
21
economic, and public safety benefits. Methane (CH4 ) is the primary component of NG
22
and is the second most important anthropogenic greenhouse gas 1 in large part because it
23
has a global warming potential 86 times greater than CO2 over a 20-year period. 2 The
24
economic burdens of lost gas from distribution pipelines are largely carried by rate payers
25
because their rate includes the cost of lost and unaccounted-for gas. Excluding incidents
26
due to excavation or other outside force damage (e.g., motor vehicle damage), there were
27
349 reported significant gas pipeline incidents in the U.S. from January 2010 to June 2018.
28
These incidents led to 44 deaths, 244 injuries, and an estimated $161 million in direct costs; 3
29
on top of this, there were significant litigation expenses and regulatory fines to the utilities.
30
Locating and quantifying NG leaks is the first step in increasing the efficacy of NG distri-
31
bution pipeline repair and replacement efforts. New high-sensitivity, mobile CH4 monitoring
32
platforms offer a novel approach compared to traditional walking surveys for detecting and
33
quantifying NG leaks in low-pressure distribution systems and have been deployed using a
34
diversity of transport vehicles including cars, aircraft, or walking. 4 Data from these mobile
35
sensors can be used to detect and map locations with elevated CH4 concentrations, often 2
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called leak indications. 5–7
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Data from mobile platforms have also been used to estimate NG leak rates, 8,9 and their
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ease of deployment and ability to detect leaks and quickly provide large spatial coverage
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makes them an attractive approach for prioritizing leak repairs and pipeline replacements to
40
reduce CH4 emissions. Mobile surveys can complement required Department of Transporta-
41
tion (DOT)/Pipeline and Hazardous Materials Safety Administration (PHMSA) safety-based
42
leak surveys, which are still necessary for safety assessments that produce leak grades. Yet
43
this new technology has not yet been widely deployed, in part because there have been ques-
44
tions regarding the correspondence of leak indications with NG leaks as well as the precision
45
and accuracy of estimating leak locations and emissions.
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We evaluate the efficacy of mobile CH4 surveys for detecting, locating and estimating the
47
size of NG leaks in local distribution systems. We assess the correspondence between leak
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indications and actual NG leaks using the results from mobile CH4 surveys in parts of five
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U.S. urban areas 8 and data collected during follow-up field visits to these urban areas. These
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data also provide insights into activity factors (numbers of leaks) for national CH4 emission
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inventories. Next, we compare emission rate estimates from mobile surveys to enclosure
52
and tracer quantification methods. Finally, we evaluate the results of our investigation to
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characterize the value of mobile mapping for informing infrastructure repair and replacement.
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Specifically, we assess the ability of mobile CH4 surveys to rank NG pipeline leaks by leak rate
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as the basis for prioritizing repairs among Grade 3 (non-hazardous) leaks in order to reduce
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CH4 emissions. The rest of the paper is organized into the following sections: materials
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and methods; evaluating the efficacy of mobile surveys for detecting and locating leaks using
58
data from on the ground site visits; emission rate rankings and emission factor comparisons
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among mobile, enclosure and tracer methods; and the value of mobile mapping for informing
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infrastructure repair and replacement.
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2
Materials and Methods
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2.1
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The mobile survey instrumentation and method is described in detail in von Fischer et al. 8
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Briefly, we installed Picarro high-precision CH4 analyzers in three Google Street View (GSV)
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cars and a functionally similar Los Gatos high-precision CH4 analyzer in a fourth. All CH4
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analyzers measured atmospheric CH4 concentrations at approximately 2 Hz with a response
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time (1/e) of 1 to 2 s. A pump drew air to the instrument via a polyethylene sampling
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manifold mounted on the front bumper. The GSV vehicles were also outfitted with a global
69
positioning system (GPS) to record vehicle location and speed and an anemometer to record
70
wind speed and direction.
Mobile Survey Instruments and Methodology
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We used an updated data processing algorithm relative to von Fischer et al. 8 that yields
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as a key data product a leak indication which consists of an estimated leak location and
73
emission rate. For the mobile method, a leak indication corresponds to a location where
74
elevated CH4 concentrations (exceeding 110% of background levels) are detected during two
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or more mobile traverses. These two traverses typically occur on different days, as we require
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a targeted mapping area to be surveyed twice, where a second pass of the area is conducted
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after the entire area is surveyed once. 8 See the supporting information (SI), Section 6, for
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further details about our updated algorithm.
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We deployed GSV cars equipped with CH4 analyzers for sampling in several U.S. cities
80
using the survey protocols described in von Fischer et al. 8 The cities included parts of Los
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Angeles serviced by the NG distribution company Southern California Gas (SoCal Gas), and
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four other urban areas anonymized to comply with non-disclosure agreements with local gas
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distribution companies (LDCs). We refer to these anonymized cities/LDCs as A, B, C, and
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D.
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Our mobile surveys resulted in hundreds of leak indications with corresponding location
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and emissions estimates. In each city we shared leak indication information with the LDCs
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in the form of GPS locations and a categorical estimate of leak size. In the cases reported
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here, LDCs visited the locations and reported their findings at each location. The leak sizes
89
were categorized as small (0-1.6 g min−1 ), medium (1.6-26 g min−1 ) and large (>26 g min−1 ).
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These bins were based on the range of controlled CH4 releases used to calibrate an algorithm
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for estimating leak rates from the mobile survey. For comparison, these bins represent an
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estimated 94%, 2.4%, and 26 g min−1 ) Total, All Leak Indications
137
LDC A, % no leak found LDC B, % no leak found 88% 85% 77% 50% 0% 50% 86% 80%
indications and NG leaks, as indicated by the results of the survey crews’ investigation:
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• mobile mapping may have a high incidence of false positives for NG leaks. These could
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arise from elevated CH4 readings from sources besides NG leaks (e.g., biological source,
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NG-powered vehicle exhaust),
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• mobile mapping had instrument error, leading to elevated CH4 levels that are spurious,
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• the LDC survey crews’ high false negative rate (i.e., failure to find leaks that are
143
present) for finding NG leaks is a result of either equipment that was not sufficiently
144
sensitive or inadequate search effort
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• leak indications were associated with leaks that were ignored because they were too small to be graded as leaks, and/or
146
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• the locations of the leak indications provided by the mobile platforms were not close enough to actual leak locations for the survey crews to find them.
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149
Below we explore each of these possibilities.
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3.2
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In cities A and B we visited a random subset of approximately 30 of the mobile-based leak
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indication locations where LDC survey crews did not discover a NG leak. A representative of
Follow-up Site Visits
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CH4 (ppm) 5 4 3
Figure 1: A representative map for our ground search to follow up on leak indications from the mobile platform that were not found by a LDC. The above image is from Google, map data: Google Imagery 2018. This map was accessible on a cell phone during our leak indication visits. The colored points represent elevated CH4 concentrations measured during the mobile survey. The white square is the estimated leak location based on the mobile CH4 measurements. The blue triangle is the location where we ultimately found a NG leak.
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the LDC crew joined us at each of the leak indication locations that we visited, and we spent
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a maximum of 30 minutes collaboratively surveying each location for a NG leak or other
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CH4 emitting source. We used data from the mobile survey and a portable, high-sensitivity
156
Los Gatos Research CH4 analyzer to direct our search. Figure 1 provides an example of the
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maps we used during the location visits. While our CH4 analyzer was sensitive to just a few
158
parts-per-billion (ppb) departures from background, LDCs often use hand-held sensors with
159
parts-per-million (ppm) level sensitivities. Thus, there was more than an order of magnitude
160
difference in the sensitivity of instruments used to measure CH4 levels.
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We categorized the findings from our visit to each leak indication location (Table 2).
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When we failed to find any elevated CH4 levels, we categorized the location as having no
163
source found. If we found elevated CH4 levels during our visit to the location, we collected
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air samples to be analyzed for CH4 and ethane concentrations. We used the results of this
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analysis to attribute elevated CH4 levels to biogenic or NG sources 16–18 . See Section S3 of 8
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Table 2: Results from the site visit to a subset of leak indications where LDCs had reported no NG leak. The data below are counts and percentages in each category. These results indicate a 72% and 68% false-negative rate, where LDCs failed to find a leak that existed within the leak indication area. Source NG, new actionable NG, recent repair evidence NG, non-actionable Biological CH4 No CH4 Source Found Other source a Totals a b
c
b
18 5 0 5 3 1 32
City A 56% Total NG: 16% 23 (72%) 0% 16% 9% 3% 100%
c
13 2 6 9 1 0 31
City B 42% Total NG: 6% 21 (68%) 19% 29% 3% 0% 100%
One leak indication corresponded to restaurant emissions on the customer side of the meter. Only half were measurable on the Heath RMLD, and two of the actionable leaks were classified as Grade 1. Three of the actionable leaks were classified as Grade 1.
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the SI for more details on the CH4 /ethane analysis. For each leak indication attributable
167
to NG, we sub-categorized the leak indication as being actionable, non-actionable, being
168
on the customer side of the meter, or having evidence of recent infrastructure repair. We
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sub-categorized the leak indication as actionable when the LDC field crew determined that
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a leak indication was the result of an active and gradable (i.e., Grade 1, 2 or 3) NG leak.
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We sub-categorized leak indications as non-actionable when elevated CH4 was due to a NG
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leak, but the soil concentrations were low enough (typically below 20% of the lower explosive
173
limit, or 10,000 ppm) for the LDC crew to not grade the leak. Finally, we sub-categorized
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leak indications that were not attributable to NG sources as being from a biological CH4
175
source or other CH4 source (end use).
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3.3
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Using the data from ground visits by both our team (Table 2) and the LDCs (Table 1), we
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estimated that 76% (95% CI: 60%, 88%) of all mobile leak indications were attributable to
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NG leaks in city A. That is, the false positive rate for the correspondence of leak indications
Correspondence Between Leak Indications and NG Leaks
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from mobile surveys with actual NG leaks is an estimated 24%. In city B an estimated 74%
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(95% CI: 59%, 86%) of our reported leak indications are attributable to NG. We calculated
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these results by considering the percentage of leak indications discovered by the LDC as NG
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leaks, and the percentage of leak indications that were not discovered by the LDC but are
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attributable to NG. See SI Section S4 for further details on how we derived these percentages.
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Weller et al. 9 explore the false negative rate of mobile CH4 surveys to estimate the number
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of leaks that go undetected.
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Based on these findings, we conclude that the majority of leak indications from mobile
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surveys corresponded to NG leaks, and that the mobile survey method had a reasonably
189
low incidence of false positives for detecting NG leaks. These results are similar to those
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of Phillips et al. 5 and Jackson et al. 6 who both found that the majority of elevated CH4
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concentrations collected by their mobile monitoring system were attributable to NG sources.
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We note that at only a very small percentage of leak indication locations did we fail to find
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any elevated CH4 concentrations with the handheld sensors that we used during our ground
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visit (3% in city A, 9% in city B), suggesting that spurious false positives from the mobile
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approach were rare.
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3.4
197
When we found a leak indication attributable to NG, we considered it a false negative leak
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report by the LDC survey crew because they had previously reported no NG leak at the
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location. As we show in Table 2, 70% (44 of 63) of the leak indications that we visited
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in cities A and B corresponded to false negative leak determinations by the survey crews.
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Of the NG leaks we found in our ground survey, the overwhelming majority (93% or 41 of
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44) were attributable to pipeline leaks, with the remaining 7% coming from metering and
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regulating devices. Thus we estimate that that the false negative rate specific to finding
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pipeline leaks is 65% (41/63).
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Leak Activity Factors
Furthermore, 11% (5/44) of these leaks, which were not initially found by the survey 10
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crews, were determined to be Grade 1 leaks by the LDC following our ground survey. Grade
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1 leaks are defined as an existing or likely hazard to people or property, 19 thus requiring
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immediate repair. In city A, there were Grade 1 leaks at two locations and in city B, there
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were Grade 1 leaks at three locations. It is important to recognize that leak grades are
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assigned on the basis of proximity to structures and potential hazard as opposed to leak
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emission rate. Small leaks can be rated as Grade 1, while larger leaks can be rated as Grade
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2 or 3 depending primarily on location.
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Ground survey effectiveness is an interaction of both equipment sensitivity and field
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crew survey protocols. In most instances in both cities, the combined efforts of the LDC
215
representative and our team found leaks within five minutes of arriving at the leak indication
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location, suggesting that field crews lack sufficiently sensitive equipment, may not have
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been meticulous in their initial on-the-ground search, or determined that that leak was not
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gradable. In city A, only half of the 18 actionable NG leaks we visited were measurable
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on the LDC’s instrument, the Heath Remote Methane Leak Detector (RMLD) which has a
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detection limit of approximately 3-5 ppm. In city B, the field crews used the Heath DPIR
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for vehicle-based survey and the Sensit Gold G2 for the walking survey and leak grading.
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The Sensit device was able to detect elevated CH4 levels at all the locations where we found
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NG leaks; our work with the DPIR was not sufficiently systematic to allow comment on its
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effectiveness.
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Our findings suggest that the number of pipeline leaks in local distribution systems could
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be significantly greater than indicated by current NG LDC inventories that are derived using
227
traditional survey methods alone. Our data indicates that LDC crews successfully locate 35%
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of the pipeline leaks (65% false negative rate) that are found by the mobile survey method.
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Interestingly, two previous studies by the NG LDC Pacific Gas & Electric (PG&E) found that
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mobile surveys and walking surveys each find a different subset of leaks, 20,21 with relatively
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little overlap between the two approaches (5% and 12% overlap in the two studies). Like
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our study, these PG&E studies found an average 65% false negative rate (i.e., 35% find rate)
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for traditional walking surveys as compared to an average 32% false negative rate (i.e., 68%
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find rate) when using the Picarro Surveyor as the mobile platform.
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These false negative rates are approximately 4x higher than current EPA estimates, which
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assume that LDC surveys find 85% of distribution pipeline leaks. 10,22 Our results and the
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PG&E study indicate that the find rate for traditional LDC leak surveys is approximately
238
35%. If this detection rate is applied at the national scale instead of the currently assumed
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85% find rate, then the national inventory for the number of pipeline leaks in NG distribution
240
systems would increase by a factor of 2.4 (see the SI, Section S5 for details on this calculation).
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These results mirror other recent studies that estimate greater NG leakage than reported by
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the EPA 23–25 across the NG supply chain and demonstrate how mobile surveys can inform
243
national emission inventories by improving estimates of activity factors.
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3.5
Location Errors of Mobile-Based Leak Indications (ii): Utility D
(iii): Utilities C & D Combined
20 15 10
Frequency
4
0
50
100
Location Error (m)
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0
0
0
1
5
2
3
Frequency
10 5
Frequency
5
6
15
7
(i): Utility C
0
50
100
150
Location Error (m)
0
50
100
150
Location Error (m)
Figure 2: The distribution of location errors for NG leaks surveyed in areas serviced by LDCs C and D. Location error is the distance between the center of the leak indication and the location of the leak as observed during the ground visit. For 75% of the leak indications shown, the mobile location error was less than 42 m.
245
We used the leak expression GPS coordinates recorded in Cities C and D to evaluate
246
the precision of mobile-based location estimates. The average distance (error) between the
247
mobile-based leak indication locations and the actual leak expression location was 31 m. The 12
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median error was 19 m with a standard deviation of 30 m (Figure 2). This error in location
249
estimates may encompass multiple NG service lines but offers a reasonably constrained search
250
area for discovering NG leaks. The mobile-generated leak indication location is derived from
251
a weighted average of the multiple observations of elevated CH4 concentrations (see the SI
252
Section S6.1 for more details).
253
Because many NG leaks occur off the roadway where our mobile CH4 mapping efforts
254
are constrained, we expect there to be at least some location error for leaks emanating from
255
pipes off the roadway. For example, the estimated leak indication location would be placed
256
on the roadway for a leaking service line in the adjacent front yard of a home. Despite this
257
limitation, results in Figure 2 indicate that most leak indication locations are within 42 m of
258
a NG leak, a distance that corresponds to one or two lot widths in typical urban residential
259
areas.
260
4
261
In the following subsections, we compare estimated NG leak emission rates from mobile,
262
tracer-ratio, and enclosure-based methods. Our comparisons include analyses of the differ-
263
ences as well as the ratios of the estimates from the various methods. We use these two
264
comparisons to explore both the additive (differences) and multiplicative (ratios) dissimilar-
265
ities between the different methods.
266
4.1
267
Estimated emission rates from the mobile platform were significantly positively correlated
268
with rates estimated by tracer methods used by Aerodyne Research Inc. (ARI) and GHD
269
(Figure 3). The correlation with mobile-based estimates was stronger for the GHD emission
270
rates (r = 0.92, 95% CI: 0.71, 0.98, n = 10) than for ARI (r = 0.47, 95% CI: 0.22, 0.66,
271
n = 49). The combined correlation was also significantly positive (r = 0.48, 95% CI: 0.26,
Quantifying Natural Gas Emissions
Leak Flux and Ranking Estimates: Tracer Method
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0.1
0.3
1
3.2
10
Tracer Estimate, g min−1
31.6
31.6 ● ●
● ●
●
0.1
0.3
1
3.2
10
Tracer Estimate, g min−1
31.6
10
● ●● ● ● ● ● ● ● ● ●● ●● ●● ● ● ●● ● ●●
3.2
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● ●
●
1
10
●
● ●
● ●●
●
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● ●● ●●●● ●● ● ● ● ● ● ● ● ● ● ●
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0.3
●
● ●
●
●
0.1
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0.3
1
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Mobile Estimate, g min−1
● ● ●●●● ● ● ● ● ● ● ● ● ●● ● ● ●● ● ● ● ● ●● ●
3.2
3.2
● ●● ● ● ● ●
1
●
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0.3
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0.1
10
●
Mobile Estimate, g min−1
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(iii): Utilities C & D Combined
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(ii): Utility D
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0.1
Mobile Estimate, g min−1
31.6
(i): Utility C
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●
0.1
0.3
1
3.2
Utility C Utility D
10
Tracer Estimate, g min−1
31.6
Figure 3: Comparison of emission rate estimates from the mobile platform and the tracer method; lines are 1:1 lines. Figure (i) compares the flux estimates from the mobile platform to the ARI tracer method at 49 NG leaks. Figure (ii) compares the flux estimates from the mobile platform to the GHD tracer method at 10 NG leaks.
272
0.66).
273
Mobile-based estimates were generally greater than tracer-based estimates, but the mag-
274
nitude of difference depended on leak size. Emissions estimates from the mobile platform
275
averaged 1.5 g min−1 larger than the tracer method relative to a mean leak rate of 2.1 g
276
min−1 . This mean difference in emissions estimates was significantly different from 0 (95%
277
CI 0.44, 2.48, n = 59), indicating a positive bias in the mobile based estimates. We found
278
that the over-estimation of small leaks led to a large and statistically significant average
279
multiplicative bias where leak emissions estimates were 4.4 times greater than tracer esti-
280
mates (p1.3 g min−1 .
311
We found a moderate, positive correlation (r = 0.43, 95% CI 0.10, 0.68, n = 33) between
312
mobile and surface enclosure estimates (Figure 5ii). The mobile rates were, on average, 1.7 g
313
min−1 greater than the enclosure rates (95% CI 1.2 to 2.2). When evaluated multiplicatively,
314
enclosure rates were, on average, only 15.4% the size of mobile based rates (Figure 5ii,
315
p < 0.001). This general pattern is retained for larger leaks where the mobile estimate is
316
>1.3 g min−1 .
317
There are several possible explanations for why the tracer and mobile methods are larger
318
than the surface enclosure estimates. If the seal on the enclosure is not sufficient, there
319
may be additional dilution which is not measured with the sampling system which would
320
lead to an underestimation of the leak rate. Similarly, if the enclosures failed to cover the
321
whole surface expression, it would lead to an underestimate of the total emission. It is also
322
possible that the ambient measurement methods are affected by nearby leaks not captured
323
with the enclosure. In cases where the surface expression of the leak is large (crosswind width
324
of 5 to 10 m), it is plausible that use of a point source for the tracer would not simulate
325
the distributed CH4 source, but previous tracer release studies using a second tracer as an
326
internal standard found no significant bias, even when the tracers are spatially separated. 26
327
In contrast to our findings, a previous surface enclosure study of controlled CH4 releases
328
agreed to within 12% of the metered release rates (see the SI) over the range 1.6 to 4.8 g
329
min−1 . Repeated enclosure measurements of the same set of actual leaks over a 3-week period
330
showed variability up to 60% from week to week. 10 In our study, most mobile measurements
331
were not conducted at the same time as the tracer ratio and enclosure measurements.
332
SoCal Gas found similar magnitudes of disagreement between enclosure estimates and
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mobile estimates of leak rates. 27 Following our mobile-based estimation of leak rates in their
334
Los Angeles service area, SoCal Gas hired GHD to conduct enclosure-based estimates of
335
leak rates. SoCal Gas shared these results with us and later made them public in a legal
336
proceeding. 28 SoCal reported that the mobile-based emissions estimates were 13 times greater
337
than the enclosure estimates, 27 which is equivalent to enclosure results averaging 7.7% the
338
size of the mobile-based emission estimates. Our results suggest that this difference emerged
339
from an overestimate of small leaks by the mobile method, as well as the underestimate of
340
rates by the enclosure method.
341
5
342
5.1
343
We have demonstrated that a large majority of leak indications from mobile CH4 monitoring
344
platforms correspond to NG leaks, that leak indication locations are sufficient for finding
345
NG leaks, and that leak flux estimates are effective for ranking leak sizes. Because NG LDC
346
field crews were unable to locate these NG leaks, our findings suggest that NG distribution
347
systems have many more leaks than LDCs are able to find using their existing leak survey
348
equipment and methods. This may partly reflect differences in how a leak is defined by
349
LDCs, the sensitivity of the instrumentation used for surveys, and/or the breadth of area
350
associated with mobile leak indications vs single address leak designations. From a public
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safety perspective, this is concerning because some of the leaks we discovered during our
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ground visit were categorized as Grade 1.
Value of Mobile Mapping for Repair Prioritization Finding Natural Gas Leaks
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These results raise questions about why field crews were unable to find leaks indicated
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by the mobile platform. We suspect differences in instruments are partly responsible. The
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Picarro and Los Gatos instruments on the mobile platform are able to measure CH4 con-
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centrations at a very high frequency (2 times per second) and are highly sensitive (detecting
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changes down to 0.001 part-per-million), while the instruments used by LDCs are generally 18
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less sensitive. It is also possible that crews using hand-held sensors are only able to detect
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leaks at ground level and may not detect small atmospheric plumes from a nearby source. We
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hypothesize that using more sensitive instruments coupled with additional training would
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reduce the false negative rate and improve leak detection.
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5.2
Prioritization Method Tracer Estimate Mobile Estimate Random Repair
0.6 0.4 0.2
Cumulative Emissions
0.8
1.0
Using Leak Size Information
Emissions Reduction Comparisons
0.0
Mobile vs. Random Mobile vs. Tracer
0
5
10
15
20
25
30
35
40
45
Leak Ranking (largest to smallest)
Figure 6: Cumulative emissions curves (CECs) from the ARI tracer and mobile quantification methods. The solid red and black lines show the estimated cumulative emissions curves and the shading shows 95% confidence intervals. Despite imprecision in the mobile estimates, the effectiveness of prioritizing leak repair for approximately the top 15% of leaks is equivalent for the mobile and tracer methods.
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The mobile-based leak rate estimates are useful for prioritizing leak repair and pipeline
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replacement, despite uncertainty in estimates of absolute leak emission rates. To illustrate
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the relative benefit of using mobile quantification as compared with tracer methods and a
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random repair approach, we constructed cumulative emission curves for each approach. We
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construct the cumulative emission curves by first ranking the leaks from largest to smallest 19
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based on estimated emission rate, then computing the proportion of the estimated total
369
emissions attributable to the largest x leaks (Figure 6 for city C). We computed the uncer-
370
tainty in the cumulative emissions curves using a bootstrap approach. See SI Section S7 for
371
more details on the bootstrap analysis.
372
The tracer-based cumulative emission curve for city C indicates that the top 9 leaks
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(18% of leaks) account for an estimated 67% (64%-71%) of the total emissions (Figure 6).
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Other NG leak studies have similarly found that a small proportion of leaks account for the
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majority of emissions. 9,29,30 When compared to the tracer-based cumulative emission curve,
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it is clear that the mobile approach does an effective job of characterizing the emissions,
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while also being much quicker and much lower cost than the tracer method. Despite the
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uncertainty in both the tracer ratio and mobile flux estimates, the mobile-based cumulative
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emission curve is not significantly different from the tracer curve for the largest leaks (i.e.,
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top 9). However, a gap emerges between the tracer and mobile curves due to the aforemen-
381
tioned over-estimate of small leaks by the mobile approach. Both tracer and mobile-based
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curves lie well above the random repair line, indicating that the mobile-based rankings offers
383
an effective approach, in terms of spatial coverage and acceptable quantification accuracy,
384
for reducing NG system leakage. This efficacy results from the mobile-based rankings suc-
385
cessfully identifying the largest leaks, which contribute disproportionately to total emissions.
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Further improvements in mobile leak rate estimation methodologies will increase precision
387
and accuracy and therefore the efficacy of ranking leaks for repairs, but it is clear that cur-
388
rent precision is more than sufficient for effectively characterizing the population of leaks
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and cost-effective prioritization within leak repair and pipeline replacement programs such
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that large reductions in methane emissions can be achieved quickly and easily.
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In light of differences among quantification methods, there remain open questions about
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the accurate quantification of NG leak emission rates. For example, evidence here suggests
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that the surface enclosure method tends to under-estimate leak rates compared to estimates
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obtained from downwind ambient measurements and this may be more problematic at higher
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leak rates. Further work is required to test both approaches in complex urban environments
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and for the type of dispersed surface expressions associated with below ground pipeline leaks.
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Likewise, it appears that mobile methods over-estimate the size of small leaks. Understanding
398
these discrepancies and their associated uncertainties is important for an accurate accounting
399
of emissions from and management of NG distribution systems, yet they do not undercut the
400
value of mobile methods for detecting and ranking leaks for effective system management.
401
Finally, mobile surveys are not a substitute for the regular walking surveys conduct
402
by LDCs. Previous work has revealed that some NG leaks are detected only by mobile
403
surveying but not by walking surveys, and vice-versa. 20,21 Of course, the process of grading
404
leaks for safety requires boots on the ground, but the co-deployment of vehicle-based surveys
405
can help find more leaks and also provides space- and time-effective monitoring. Currently,
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mobile surveys cannot substitute for walking leak surveys, because mobile surveys can fail to
407
detect NG leaks under some environmental conditions and at some locations. 9 Despite these
408
limitations, mobile surveys are a powerful new tool available for effectively and responsibly
409
managing NG distribution systems.
410
Acknowledgement
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This work was funded by grants from the Alfred P Sloan Foundation and Robertson Foun-
412
dations to the Environmental Defense Fund. The authors thank Steven P. Hamburg, Ramon
413
Alvarez, and Jennifer Hoeting for helpful feedback that improved the manuscript. The au-
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thors also thank Duck Keun Yang and Sam Chamberlain for helping with data collection
415
and management.
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Supporting Information Available
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The following file is available online as supporting information:
21
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• Supporting Information for Vehicle-based methane surveys for finding nat-
419
ural gas leaks and estimating their size: validation and uncertainty. The SI
420
contains further information on data collection, processing, and analysis.
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References
422
(1) Boucher, O.; Friedlingstein, P.; Collins, B.; Shine, K. P. The indirect global warming
423
potential and global temperature change potential due to methane oxidation. Environ.
424
Research Letters 2009, 4, 044007.
425
(2) Myhre, G.; Shindell, D.; BrÂŐon, F.-M.; Collins, W.; Fuglestvedt, J.; Huang, J.;
426
Koch, D.; Lamarque, J.-F.; Lee, D.; Mendoza, B.; Nakajima, T.; Robock, A.;
427
G. Stephens, T. T.; Zhang, H. In Climate change 2013: The Physical Science Basis.
428
Contribution of working group I to the fifth assessment report of the intergovernmen-
429
tal panel on climate change; Stocker, T., Qin, D., Plattner, G., Tignor, M., Allen, S.,
430
Boschung, J., Nauels, A., Xia, Y., Bex, B., Midgley, B., Eds.; Cambridge University
431
Press, 2013.
432
(3) PHMSA, Distribution, Transmission & Gathering, LNG, and Liquid Accident and
433
Incident Data. 2018; https://www.phmsa.dot.gov/pipeline/library/data-stats/
434
pipelineincidenttrends.
435
(4) Eapi, G. R.; Sabnis, M. S.; Sattler, M. L. Mobile measurement of methane and hydrogen
436
sulfide at natural gas production site fence lines in the Texas Barnett Shale. J. Air &
437
Waste Manag. Assoc. 2014, 64, 927–944.
438
(5) Phillips, N. G.; Ackley, R.; Crosson, E. R.; Down, A.; Hutyra, L. R.; Brondfield, M.;
439
Karr, J. D.; Zhao, K.; Jackson, R. B. Mapping urban pipeline leaks: Methane leaks
440
across Boston. Environ. Pollut. 2013, 173, 1–4.
22
ACS Paragon Plus Environment
Page 22 of 27
Page 23 of 27
Environmental Science & Technology
441
(6) Jackson, R. B.; Down, A.; Phillips, N. G.; Ackley, R. C.; Cook, C. W.; Plata, D. L.;
442
Zhao, K. Natural gas pipeline leaks across Washington, DC. Environ. Sci. & Technol.
443
2014, 48, 2051–2058.
444
(7) Gallagher, M. E.; Down, A.; Ackley, R. C.; Zhao, K.; Phillips, N.; Jackson, R. B. Natural
445
gas pipeline replacement programs reduce methane leaks and improve consumer safety.
446
Environ. Sci. & Technol. Letters 2015, 2, 286–291.
447
(8) von Fischer, J. C.; Cooley, D.; Chamberlain, S.; Gaylord, A.; Griebenow, C. J.; Ham-
448
burg, S. P.; Salo, J.; Schumacher, R.; Theobald, D.; Ham, J. Rapid, Vehicle-Based
449
Identification of Location and Magnitude of Urban Natural Gas Pipeline Leaks. Envi-
450
ron. Sci. & Technol. 2017, 51, 4091–4099.
451
(9) Weller, Z. D.; Hoeting, J. A.; von Fischer, J. C. A Calibration-Capture-Recapture Model
452
for Inferring Natural Gas Leak Population Characteristics Using Data From Google
453
Street View Cars. to appear, Environmetrics 2018, https://doi.org/10.1002/env.2519 .
454
(10) Lamb, B. K.; Edburg, S. L.; Ferrara, T. W.; Howard, T.; Harrison, M. R.; Kolb, C. E.;
455
Townsend-Small, A.; Dyck, W.; Possolo, A.; Whetstone, J. R. Direct measurements
456
show decreasing methane emissions from natural gas local distribution systems in the
457
United States. Environ. Sci. & Technol. 2015, 49, 5161–5169.
458
(11) Allen, D. T.; Torres, V. M.; Thomas, J.; Sullivan, D. W.; Harrison, M.; Hendler, A.;
459
Herndon, S. C.; Kolb, C. E.; Fraser, M. P.; Hill, A. D. Measurements of methane
460
emissions at natural gas production sites in the United States. Proc. Natl. Acad. Sci.
461
U.S.A. 2013, 110, 17768–17773.
462
(12) Mitchell, A. L.; Tkacik, D. S.; Roscioli, J. R.; Herndon, S. C.; Yacovitch, T. I.; Mar-
463
tinez, D. M.; Vaughn, T. L.; Williams, L. L.; Sullivan, M. R.; Floerchinger, C. Measure-
464
ments of methane emissions from natural gas gathering facilities and processing plants:
465
Measurement results. Environ. Sci. & Technol. 2015, 49, 3219–3227. 23
ACS Paragon Plus Environment
Environmental Science & Technology
466
(13) Lamb, B. K.; McManus, J. B.; Shorter, J. H.; Kolb, C. E.; Mosher, B.; Harriss, R. C.;
467
Allwine, E.; Blaha, D.; Howard, T.; Guenther, A. Development of atmospheric tracer
468
methods to measure methane emissions from natural gas facilities and urban areas.
469
Environ. Sci. & Technol. 1995, 29, 1468–1479.
470
(14) Shorter, J. H.; McManus, J. B.; Kolb, C. E.; Allwine, E. J.; Siverson, R.; Lamb, B. K.;
471
Mosher, B. W.; Harriss, R. C.; Howard, T.; Lott, R. A. Collection of leakage statistics
472
in the natural gas system by tracer methods. Environ. Sci. & Technol. 1997, 31, 2012–
473
2019.
474
(15) Lamb, B. K.; Cambaliza, M. O.; Davis, K. J.; Edburg, S. L.; Ferrara, T. W.; Flo-
475
erchinger, C.; Heimburger, A. M.; Herndon, S.; Lauvaux, T.; Lavoie, T. Direct and
476
indirect measurements and modeling of methane emissions in Indianapolis, Indiana.
477
Environ. Sci. & Technol. 2016, 50, 8910–8917.
478
(16) Yacovitch, T. I.; Herndon, S. C.; Roscioli, J. R.; Floerchinger, C.; McGovern, R. M.;
479
Agnese, M.; PeÌĄtron, G.; Kofler, J.; Sweeney, C.; Karion, A. Demonstration of an
480
ethane spectrometer for methane source identification. Environ. Sci. & Technol. 2014,
481
48, 8028–8034.
482
(17) McKain, K.; Down, A.; Raciti, S. M.; Budney, J.; Hutyra, L. R.; Floerchinger, C.;
483
Herndon, S. C.; Nehrkorn, T.; Zahniser, M. S.; Jackson, R. B. Methane emissions from
484
natural gas infrastructure and use in the urban region of Boston, Massachusetts. Proc.
485
Natl. Acad. Sci. U.S.A. 2015, 112, 1941–1946.
486
(18) Karion, A.; Sweeney, C.; Kort, E. A.; Shepson, P. B.; Brewer, A.; Cambaliza, M.; Con-
487
ley, S. A.; Davis, K.; Deng, A.; Hardesty, M. Aircraft-based estimate of total methane
488
emissions from the Barnett Shale region. Environ. Sci. & Technol. 2015, 49, 8124–8131.
489
(19) California Public Utilities Commission, Survey of Natural Gas Leakage Abate-
490
ment Best Practices. 2015; https://www.socalgas.com/regulatory/documents/ 24
ACS Paragon Plus Environment
Page 24 of 27
Page 25 of 27
Environmental Science & Technology
491
r-15-01-008/R.15-01-008%20SED%20Report%20Survey%20of%20Natural%20Gas%
492
20Leakage%20Abatement%20Practices%20031815%20Rpt%20Only.pdf.
493
494
(20) Clark, T.; Conley, E.; Kerans, M.; Piazza, M. Picarro Surveyor Leak Detection Study: Diablo Side-by-Side Study. Pacific Gas and Electric 2012, Internal Study Report.
495
(21) Kerans, M.; Clark, T.; Conley, E.; Crosson, E.; Piazza, M. Picarro Surveyor Leak De-
496
tection Study: Sacramento Side-by-Side Study. Pacific Gas and Electric 2012, Internal
497
Study Report.
498
(22) Campbell, L. M.; Campbell, M. V.; Epperson, D. L. Methane Emissions from the
499
Natural Gas Industry, Volume 9: Underground Pipeline. 1996; https://www.epa.gov/
500
sites/production/files/2016-08/documents/9_underground.pdf.
501
(23) Miller, S. M.; Wofsy, S. C.; Michalak, A. M.; Kort, E. A.; Andrews, A. E.; Biraud, S. C.;
502
Dlugokencky, E. J.; Eluszkiewicz, J.; Fischer, M. L.; Janssens-Maenhout, G. Anthro-
503
pogenic emissions of methane in the United States. Proc. Natl. Acad. Sci U.S.A. 2013,
504
110, 20018–20022.
505
(24) Wunch, D.; Toon, G. C.; Hedelius, J. K.; Vizenor, N.; Roehl, C. M.; Saad, K. M.;
506
Blavier, J.-F. L.; Blake, D. R.; Wennberg, P. O. Quantifying the loss of processed
507
natural gas within California’s South Coast Air Basin using long-term measurements
508
of ethane and methane. Atmosph. Chem. and Physics 2016, 16, 14091.
509
(25) Alvarez, R. A.; Zavala-Araiza, D.; Lyon, D. R.; Allen, D. T.; Barkley, Z. R.;
510
Brandt, A. R.; Davis, K. J.; Herndon, S. C.; Jacob, D. J.; Karion, A. Assessment
511
of methane emissions from the US oil and gas supply chain. Science 2018, eaar7204.
512
(26) Roscioli, J.; Yacovitch, T.; Floerchinger, C.; Mitchell, A.; Tkacik, D.; Subramanian, R.;
513
Martinez, D.; Vaughn, T.; Williams, L.; Zimmerle, D. Measurements of methane emis-
514
sions from natural gas gathering facilities and processing plants: measurement methods.
515
Atmos. Meas. Techniques 2015, 8, 2017. 25
ACS Paragon Plus Environment
Environmental Science & Technology
516
(27) Newton, E. Southern California Gas Company’s Verification Study of the Methane
517
Mapping of Four California Cities by the Environmental Defense Fund and Colorado
518
State University. Online, 2016; https://socalgas.com/regulatory/documents/
519
r-15-01-008/EDF_4-Cities_Methane_Mapping_Report_Final_081916.pdf.
520
(28) Hovsepian, M. Supplemental Replay Comments of Southern California Gas Company
521
(U 904 G) and San Diego Gas and Electric Company (U 902 G) On Best Practices
522
Recommendations. 2015; http://docs.cpuc.ca.gov/PublishedDocs/Efile/G000/
523
M166/K474/166474903.PDF.
524
(29) Brandt, A. R.; Heath, G.; Kort, E.; O’sullivan, F.; Pétron, G.; Jordaan, S.; Tans, P.;
525
Wilcox, J.; Gopstein, A.; Arent, D. Methane leaks from North American natural gas
526
systems. Science 2014, 343, 733–735.
527
(30) Balcombe, P.; Anderson, K.; Speirs, J.; Brandon, N.; Hawkes, A. The natural gas sup-
528
ply chain: the importance of methane and carbon dioxide emissions. ACS Sustainable
529
Chem. & Eng. 2016, 5, 3–20.
26
ACS Paragon Plus Environment
Page 26 of 27
Page 27 of 27
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