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At least 271 records · Page 15

Optimizing feed modulation for coupled methane and NO x conversion over Pd-Pt/Mn 0.5 Fe 2.5 O 4 /Al 2 O 3 monolith catalyst

Here the impacts of feed modulation (frequency, amplitude) and catalyst design (composition and architecture) parameters are reported for the conversion of methane and NO x over a dual-layer Pt+Pd/Al 2 O 3 + Mn 0.5 Fe 2.5 O 4 /Al 2 O 3 monolith. CH 4 and NO x conversion data show that the dual-layer catalyst outperforms single-layer samples having the same catalyst loadings, with and without spinel. Close proximity of the PGM and MFO functions in the mixed-layer catalyst lowers the CH 4 conversion at high temperature while separating the PGM and spinel layers with an intermediate Al 2 O 3 layer does not. Methane conversion enhancement is linked to its nonmonotonic dependence on O 2 . The performance gains are tied to a transient activity spike that occurs during the lean-to-rich feed transition when water is present in the feed. The transient spike is attributed to the removal of CO and H 2 products via reactions with stored O 2 in the spinel, eliminating inhibition of methane steam reforming.

03 NATURAL GAS↗

Predictive Self-Healing Seals for Gas Transmission

Damaged elastomeric diaphragms within pneumatic controllers used in the oil and gas industry lead to an unintended release of methane. Self-healing microvascular materials capable of healing various types of damage have been fabricated. These microvascular materials are designed to replace currently available commercial diaphragms found in pneumatic controllers and provide a solution to reduce unintended methane leaks. This project demonstrated the ability of these materials to reduce methane release by more than 80% in lab and pilot settings. Additionally, ML approaches successfully identified leaking systems based on training using synthetic and real data.

03 NATURAL GAS↗

Duration of O 2 Exposure Determines Dominance of Fe II vs CH 4 Production in Tropical Forest Soils

Temporal fluctuations in redox conditions influence the availability of Fe III and greenhouse gas emissions in humid upland soils. However, the impact of fluctuation duration on biogeochemical processes remains unclear. We hypothesized that rates of Fe III reduction and CH 4 production are sensitive to the duration of soil oxygenation. To test this, surface soil from the Luquillo Forest, Puerto Rico, was subjected to fluctuating redox conditions with an anoxic interval of 6 days followed by oxic intervals of either 8, 24, or 72 h. Shorter oxic intervals enhanced Fe reduction, while longer oxic intervals enhanced CH 4 emissions. As O 2 exposure decreased from 72 to 8 h, Fe reduction rates increased from 0.12 ± 0.02 to 0.26 ± 0.05 mmol kg –1 h –1 , whereas cumulative CH 4 decreased from 44.0 ± 4.7 to 12.7 ± 4.6 μmol kg –1 . 13 C-amino acid spikes were preferentially incorporated into the DNA of iron reducers (Anaeromyxobacter sp.) in the shorter oxic treatment (8 h vs 24 h), suggesting that Fe reducers are less inhibited by shorter periods of oxidation. Conversely, longer oxygen pulses appear to suppress Fe reducers more than methanogens, leading to increased CH 4 emissions. These findings highlight the role of the redox oscillation length in modulating biogeochemical processes and greenhouse gas emissions in soils.

54 ENVIRONMENTAL SCIENCES↗

Potential State Regulatory Pathways to Facilitate Low-Carbon Fuels

States and the federal government are increasingly engaged in the challenges around decarbonizing the electric grid. In particular, regulators, consumers, stakeholders, and utilities recognize the need to carefully consider the role natural gas will play in a decarbonized future. A variety of technology and policy options to reduce greenhouse gas emissions associated with natural gas use are available, including energy efficiency programs, demand reduction tools, strategic electrification, and strategies to reduce emissions from natural gas production, transportation, and consumption. Low-carbon fuels – mainly renewable natural gas (RNG) and clean hydrogen – are being considered an important component of decarbonization goals. RNG and hydrogen may be able to meaningfully reduce emissions from processes independent of geologic natural gas, displacing emissions of methane, a powerful greenhouse gas. Although RNG and hydrogen are not cost-competitive today with geologic natural gas and are smaller in scale and potential than other decarbonization options, they can be explored as potential critical tools to decarbonize sectors that are difficult to electrify or shift off of natural gas entirely, such as air travel, industrial processes, maritime transport, long-distance trucking, space heating on cold days, and railroads (Nadel, 2022). The role of this report is to provide informational context for state utility regulators to understand the impacts of and challenges associated with broader integration of low-carbon fuels, followed by examples of state regulatory actions taken to date to facilitate the development of low-carbon fuels. Setting clear guidance to calculate the environmental benefits of low-carbon fuels and continuing federal and state investments in research and development to reduce costs relative to fossil fuels will be important steps to take to signal the desire to grow the market for these fuels. State public utility commissions may play a key role in setting regulatory frameworks for low-carbon fuels and ensuring that ratepayer funds, if utilized, are done so to further the public interest. This report is intended to summarize decisions that states have made to date on low-carbon fuels. In the spirit of understanding the current market and sharing information, this report provides success stories, and lessons learned across states as regulators implement varying strategies to achieve decarbonization objectives while maintaining their focus on affordability, safety, and reliability of the energy system. The report begins with an introduction of the role of natural gas in the U.S. economy (Section I) and background information on natural gas use, decarbonization, and low-carbon fuels (Section II). Next, the report describes the current market by discussing the scale of current production, emissions intensity, resource potential, and costs of low-carbon fuels compared to geologic natural gas (Section III). Following these sections, the report describes four strategies states have employed to facilitate low-carbon fuels: opening exploratory dockets, approving voluntary tariffs for customers, approving interconnection tariffs for producers, and considering portfolio-wide procurement targets (Section IV). This section lists states that have taken actions in each category, citing utility filings, commission decisions, stakeholder comments, and other relevant sources. Finally, the report concludes with suggested questions regulators may wish to consider regarding low-carbon fuels, in the interest of preparing to make decisions in the future (Section V). These questions include: Are there existing regulatory or technical barriers to voluntary purchases of low-carbon fuels? Can customers work with utilities to procure low-carbon fuels; are producers able to interconnect projects without significant barriers to entry? Should the infrastructure and/or commodity costs of low-carbon fuels be socialized among all ratepayers, or borne solely by the large commercial and industrial (C&I) customers currently driving the market? Should regulated natural gas and/or electric utilities own and operate low-carbon fuel production? How should regulators consider the unique decarbonization potential of low-carbon fuels, particularly for hard-to-abate sectors, in decision-making? Is additional direction or clarity from state policymakers needed? What no-regrets approaches can help facilitate both near-term RNG development and long-term development of hydrogen and other zero-carbon fuels? We collectively wish to express our gratitude to the U.S. Department of Energy, Office of Fossil Energy and Carbon Management, for supporting this report and other technical assistance resources for state regulators on natural gas topics. State regulators operate under a variety of policy environments, and states have vastly different types of energy resources, infrastructure, and customers. While there is no optimal regulatory, policy, or technological solution that will be successful in every state, state regulators can benefit by exchanging lessons learned with their peers across the country. We look forward to continued engagement with our fellow commissioners, commission staff, NARUC, the U.S. Department of Energy, and other stakeholders to develop sound regulation in the public interest.

03 NATURAL GAS↗

Methane Integrated Monitoring and Measurement System Design

Methane (CH 4 ), an abundant greenhouse gas, is the second largest contributor to global warming after carbon dioxide (CO 2 ). In comparison to CO 2 , CH 4 has a larger warming effect over a much shorter lifetime. While technologies to radically reduce global carbon dioxide emissions are materializing, rapid reductions in methane emissions are needed to limit near-term warming. Methane is primarily emitted as a byproduct from agricultural activities and energy extraction/utilization and is currently monitored via bottom-up (i.e., activity level) or top-down (via airborne or satellite retrievals) approaches. However, significant methane leaks remain undetected, and emission rates are challenging to characterize with current monitoring frameworks. In this report, we study methane leaks from oil and gas infrastructure using a tiered monitoring approach that combines bottom-up and top-down approaches in an integrated framework. We describe the individual advantages of bottom-up and top-down sensors in both stationary and mobile settings before characterizing how a fully integrated framework can improve predictions and uncertainties of potential leak locations and their emission rates. Further, we study the impact of different atmospheric (wind) conditions on integrated methane monitoring and develop a probabilistic approach to optimal sensor placement, thereby shortening detection times and improving monitoring capabilities. Last, we discuss how biogenic flux modeling can be used to improve assessment of background methane concentrations needed to fully assess the sensitivity of a tiered monitoring system.

54 ENVIRONMENTAL SCIENCES↗

Seasonal variation in methane ebullition in a temperate hydropower reservoir impacts annualized estimates

Estimates of ebullitive methane (CH4) emissions from reservoirs are highly uncertain, often based on spatial and temporal upscaling from a limited number of sampling sites and periods. While some of these estimates may adjust for seasonal variation in temperature, they rarely account for drawdown and the resulting changes in site depth and the areal extent of the reservoir. In Douglas Reservoir (Tennessee, USA), we conducted monthly sampling of 20 sites over 1 year to capture temporal and spatial variation in CH4 ebullition. We then compared various approaches for obtaining annualized, whole-reservoir ebullition estimates. CH4 ebullition fluxes were zero-inflated and highly skewed, with fluxes rising appreciably above zero in July and peaking in autumn. Estimates that did not account for drawdown overestimated annualized rates by 20%, though with high uncertainty. Seasonal variability and hotspots strongly influence annualized ebullition estimates and are important to account for in inventories and global upscaling.

Cardall, Anna [Brigham Young University]↗

An experimental and kinetic modeling study of the pyrolysis of isoprene, a significant biogenic hydrocarbon in naturally occurring vegetation fires

Isoprene dominates the carbon flux emitted by vegetation and constitutes 40% of non-methane biogenic emissions worldwide. Despite pyrolysis experiments at temperatures above 1000 K showing a link between isoprene combustion and aromatic species formation, comprehensive mechanistic research on isoprene is scarce in the literature. Here, in this work, we carry out an experimental and theoretical study to build, for the first time, a chemical kinetic model describing isoprene pyrolysis. The formation of polycyclic aromatic hydrocarbon (PAH) precursor species, often observed in vegetation fire plumes, is partially explained by isoprene pyrolysis experiments and theoretical modeling. Molecular dynamics (MD) simulations unveil reaction pathways from allylic isoprenyl radicals to allene and cyclopentadiene (CPD) intermediates, two relevant species detected in the experiments. Rate constants for these identified pathways are calculated using variational transition state theory to update the kinetic model, which is validated against single-pulse shock tube (SPST), and jet-stirred reactor (JSR) experimental data in the temperature range of 850–1690 K. The kinetic model presents satisfactory agreement with the SPST experimental data, and a reaction pathway analysis shows that association of propargyl radicals results in benzene formation. The JSR pathway analysis also identifies the prominent reactions for CPD, benzene, styrene, and toluene formation. Our model does not reproduce the CPD experimental profiles, indicating that additional studies are necessary. Overall, our findings advance the understanding of isoprene pyrolysis and its related atmospheric pollutants in naturally occurring vegetation fires where smoldering and oxygen-deficient combustion processes are present.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Microbial functional genes commonly respond to elevated carbon dioxide

Atmospheric CO 2 concentration is increasing, largely due to anthropogenic activities. Previous studies of individual free-air CO 2 enrichment (FACE) experimental sites have shown significant impacts of elevated CO 2 (eCO 2 ) on soil microbial communities; however, no common microbial response patterns have yet emerged, challenging our ability to predict ecosystem functioning and sustainability in the future eCO 2 environment. Here we analyzed 66 soil microbial communities from five FACE sites, and showed common microbial response patterns to eCO 2 , especially for key functional genes involved in carbon and nitrogen fixation (e.g., pcc/acc for carbon fixation, nifH for nitrogen fixation), carbon decomposition (e.g., amyA and pulA for labile carbon decomposition, mnp and lcc for recalcitrant carbon decomposition), and greenhouse gas emissions (e.g., mcrA for methane production, norB for nitrous oxide production) across five FACE sites. Also, the relative abundance of those key genes was generally increased and directionally associated with increased biomass, soil carbon decomposition, and soil moisture. In addition, a further literature survey of more disparate FACE experimental sites indicated increased biomass, soil carbon decay, nitrogen fixation, methane and nitrous oxide emissions, plant and soil carbon and nitrogen under eCO 2 . A conceptual framework was developed to link commonly responsive functional genes with ecosystem processes, such as pcc/acc vs. soil carbon storage, amyA/pulA/mnp/lcc vs. soil carbon decomposition, and nifH vs. nitrogen availability, suggesting that such common responses of microbial functional genes may have the potential to predict ecosystem functioning and sustainability in the future eCO 2 environment.

59 BASIC BIOLOGICAL SCIENCES↗

Observation-constrained kinetic modeling of isoprene SOA formation in the atmosphere

Isoprene has the largest global non-methane hydrocarbon emission, and the oxidation of isoprene plays a crucial role in the formation of secondary organic aerosol (SOA). Two primary processes are known to contribute to SOA formation from isoprene oxidation: (1) the reactive uptake of isoprene-derived epoxides on acidic or aqueous particle surfaces and (2) the absorptive gas–particle partitioning of low-volatility oxidation products. In this study, we developed a new multiphase condensed isoprene oxidation mechanism that includes these processes with key molecular intermediates and products. The new mechanism was applied to simulate isoprene gas-phase oxidation products and SOA formation from previously published chamber experiments under a variety of conditions and atmospheric observations during the Southern Oxidant and Aerosol Studies (SOAS) field campaign. Our results show that SOA formation from most of the chamber experiments is reasonably reproduced using our mechanism, except when the concentration ratios of initial nitric oxide to isoprene exceed ~ 2, the formed SOA is significantly underpredicted. The SOAS simulations also reasonably agree with the measurements regarding the diurnal pattern and concentrations of different product categories, while the total isoprene SOA remains underestimated. The molecular compositions of the modeled SOA indicate that multifunctional low-volatility products contribute to isoprene SOA more significantly than previously thought, with a median mass contribution of ~ 57 % to the total modeled isoprene SOA. However, this contribution is intricately intertwined with IEPOX-derived SOA (IEPOX: isoprene-derived epoxydiols), posing challenges for their differentiation using bulk aerosol composition analysis (e.g., the aerosol mass spectrometer with positive matrix factorization). Furthermore, the SOA from these pathways may vary greatly, mainly dependent on the volatility estimation and treatment of particle-phase processes (i.e., photolysis and hydrolysis). Our findings emphasize that the various pathways to produce these low-volatility species should be considered in models to more accurately predict isoprene SOA formation. The new condensed isoprene chemical mechanism can be further incorporated into regional-scale air quality models, such as the Community Multiscale Air Quality Modelling System (CMAQ), to assess isoprene SOA formation on a larger scale.

54 ENVIRONMENTAL SCIENCES↗

Methane Hydrates in Alaska

This paper was prepared for the National Petroleum Council's Study on Natural Gas GHG Emissions. Natural gas is the largest primary energy produced in the United States and its use is growing. Yet getting this gas to homes and businesses creates greenhouse gas emissions. That’s why reducing emissions from America’s natural gas is an urgent priority that requires collaborative solutions. The National Petroleum Council brought together a diverse group of stakeholders with the expertise to analyze this complex issue and identify ways to reduce natural gas GHG emissions for all future supply and demand scenarios. The result: actionable consensus on ensuring a lower-emission natural gas system. The study’s research charts a course forward to meaningfully reduce emissions from the natural gas system, contributing significantly to the United States’ ability to achieve its climate goals. The report concludes that through the implementation of existing policies, voluntary commitments, technologies, and market mechanisms, a 63% reduction in methane emissions can be achieved by 2030. The report went further to identify an additional pathway that methane emissions decrease by 70% and carbon dioxide emissions reduce by 33% through 2050.

03 NATURAL GAS↗

Evaluating the feasibility of using downwind methods to quantify point source oil and gas emissions using continuously monitoring fence-line sensors

The dependable reporting of methane (CH 4 ) emissions from point sources, such as fugitive leaks from oil and gas infrastructure, is important for profit maximization (retaining more hydrocarbons), evaluating climate impacts, assessing CH 4 fees for regulatory programs, and validating CH 4 intensity in differentiated gas programs. Currently, there are disagreements between emissions reported by different quantification techniques for the same sources. It has been suggested that downwind CH 4 quantification methods using CH 4 measurements on the fence line of production facilities could be used to generate emission estimates from oil and gas operations at the site level, but it is currently unclear how accurate the quantified emissions are. To investigate the accuracy of downwind methods, this study uses fence-line simulated data collected during controlled-release experiments as input for a non-standard closed-path eddy covariance (EC), the Gaussian plume inverse model (GPIM), and the backward Lagrangian stochastic (bLs) model in a range of atmospheric conditions. This study's EC attempt was unsuccessful due to data collection and instrumentation issues, resulting in invalid results characterized by underestimated emissions, large negative fluxes, and cospectra/ogives that deviated from their ideal shapes. Consequently, the EC results could not be compared with the GPIM and bLS model. The bLs model demonstrated the highest accuracy for single-release single-point emissions, though it exhibited greater uncertainty than GPIM under multi-release conditions. Across the GPIM and bLs model, the most reliable quantification was achieved with 15 min averaging and a narrow 5° wind sector range. Although EC was limited in this context, future studies should consider employing a standard EC system and further optimizing GPIM and bLs approaches – particularly for complex multi-source scenarios – to enhance quantification accuracy and reduce uncertainty.

03 NATURAL GAS↗

High-throughput methane pyrolysis for low-cost, emissions-free hydrogen

Palo Alto Research Center (PARC) and its partners will explore a targeted molten metal as a catalyst in a methane pyrolysis mist reactor to convert natural gas into hydrogen and solid carbon at a low cost without carbon dioxide emissions. The technology could augment or replace current H 2 production methods, while simultaneously sequestering carbon in high value materials.

08 HYDROGEN↗

Industry Partnerships & Their Role In Reducing Natural Gas Supply Chain Greenhouse Gas Emissions – Phase 2

This analysis is the product of collaboration between Our Nation’s Energy Future (ONE Future) and the United States (U.S.) Department of Energy (DOE) National Energy Technology Laboratory (NETL). This analysis is an update to Phase 1 of the collaboration between ONE Future and NETL. Phase 1 had three objectives: 1. Calculate a greenhouse gas (GHG) emission profile representative of ONE Future’s supply chain, including methane (CH 4 ) emission rates. 2. Compare ONE Future’s emission profile to the emission profile for the U.S. natural gas supply chain. 3. Evaluate specific emission reduction opportunities. Phase 2 has two key enhancements over Phase 1: 1. The reporting year of the data is updated from 2016 to 2017. 2. The emission profiles and the specific emission reduction opportunities are regionalized for the ONE Future supply chain. The ONE Future supply chain is based on data provided by ONE Future members for all their U.S. onshore assets. ONE Future’s data are mostly representative of their participation in the Greenhouse Gas Reporting Program (GHGRP) administered by the Environmental Protection Agency (EPA) and is supplemented by ONE Future facilities that are not required to report to GHGRP. The U.S. scenario is based on NETL’s life cycle analysis (LCA) of natural gas extraction and power generation, which also uses data from the GHGRP (but does not include non-GHGRP facilities). In addition to the data from these sources, NETL accounted for uncertainty due to data variability, data limitations, and variability in liquids unloading frequency and event duration. This report is a re-issue of the 2020 study (published on July 28, 2020). It revises the device count in the mitigation strategy “pipeline pump-down before maintenance” in the Marginal Abatement Cost (MAC) Analysis section of the report (Section 7). Please see the addendum for more details on this revision and resultant changes. This revision does not change most of our conclusions and recommendations. It only changes the total methane reduced from all the mitigation opportunities (low cost and high cost) from 6.5 Bcf CH 4 /yr to 4.8 Bcf CH 4 /yr.

03 NATURAL GAS↗

Dilemma of organic matter input to mitigate climate impact of rice paddies

Soil can act as either a source or sink of atmospheric carbon (C). Organic matter application can sequester carbon dioxide (CO 2 ) through negative emission technologies. However, in rice paddies, organic matter application can significantly increase methane (CH 4 ) emissions, offsetting potential climate benefits. Here, we compared the effects of organic matter types on net climate impact by quantifying annual gaseous fluxes and soil C stock changes with CO 2 equivalents. All organic amendments increased CH 4 emissions (7–30 Mg CO 2 -eq. ha −1 ) compared with the no organic matter treatment (NPK). However, the increases in soil C stock (9–11 Mg CO 2 -eq. ha −1 ) were insufficient to shift the system from a net C source to a net sink, even when combined with water management strategies. In contrast, biochar increased CH 4 emissions but enhanced soil C stock, leading to a net negative emission effect without compromising rice productivity. Given that rice paddies account for about 11 % of anthropogenic CH 4 emissions, organic matter application requires careful evaluation to avoid exacerbating climatic impacts.

Climate impact↗

Lagged Wetland CH 4 Flux Response in a Historically Wet Year

While a stimulating effect of plant primary productivity on soil carbon dioxide (CO 2 ) emissions has been well documented, links between gross primary productivity (GPP) and wetland methane (CH 4 ) emissions are less well investigated. Determination of the influence of primary productivity on wetland CH 4 emissions (FCH 4 ) is complicated by confounding influences of water table level and temperature on CH 4 production, which also vary seasonally. Here, in this work, we evaluate the link between preceding GPP and subsequent FCH 4 at two fens in Wisconsin using eddy covariance flux towers, Lost Creek (US-Los) and Allequash Creek (US-ALQ). Both wetlands are mosaics of forested and shrub wetlands, with US-Los being larger in scale and having a more open canopy. Co-located sites with multi-year observations of flux, hydrology, and meteorology provide an opportunity to measure and compare lag effects on FCH4 without interference due to differing climate. Daily average FCH4 from US-Los reached a maximum of 47.7 ηmol CH 4 m -2 s -1 during the study period, while US-ALQ was more than double at 117.9 ηmol CH 4 m -2 s -1 . The lagged influence of GPP on temperature-normalized FCH4 (T air -FCH 4 ) was weaker and more delayed in a year with anomalously high precipitation than a following drier year at both sites. FCH 4 at US-ALQ was lower coincident with higher stream discharge in the wet year (2019), potentially due to soil gas flushing during high precipitation events and lower water temperatures. Better understanding of the lagged influence of GPP on FCH 4 due to this study has implications for climate modeling and more accurate carbon budgeting.

59 BASIC BIOLOGICAL SCIENCES↗