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At least 361 records · Page 20

Upgrading Biogas through in situ Conversion of Carbon Dioxide to Biomethane in Anaerobic Digesters

Organic waste streams generated by wastewater treatment plants, agricultural operations, and food processing industries represent an important yet underutilized opportunity for renewable energy production in the United States. Through anaerobic digestion, these waste streams can produce biogas, a mixture primarily composed of methane (CH4) and carbon dioxide (CO2), that can be upgraded to pipeline-quality natural gas. However, most existing upgrading technologies remove CO2 from biogas rather than utilizing it, leaving a significant portion of the potential energy unused. This project investigates a novel biological upgrading approach that converts CO2 into additional CH4 by supplying hydrogen (H2) to specialized microorganisms capable of performing hydrogenotrophic methanation. The main challenges associated with biological biogas upgrading are related to hydrogen supply, gas-liquid mass transfer, and process stability. First, due to the high cost of hydrogen gas, it is preferable that H2 be produced on-site using renewable energy sources such as wind or solar power. Second, hydrogen has low solubility in liquids, which limits its availability to microorganisms and requires strategies to improve gas dissolution and transfer within the reactor. Third, process inhibition may occur as a result of increased pH caused by CO2 consumption or elevated H2 partial pressure, both of which can negatively affect methanogenic activity. Although research in these areas has advanced during the course of this project, these challenges have not yet been fully resolved. To date, the biological systems that have achieved the highest methane concentrations are typically ex-situ reactors, where operational conditions can be more easily controlled. For this reason, the findings of the present project remain highly relevant. The project goal was to develop an innovative system that can accomplish biogas upgrading via biological conversion of CO2 to CH4, in a novel hybrid approach that combines the advantages of both in-situ and ex-situ systems. The proposed system employs a three-phase upflow anaerobic bioreactor with H2 delivery through a gas-permeable membrane, enabling efficient hydrogen transfer and microbial conversion. Under optimized operating conditions, the system achieved 99% H2 consumption and 90% CO2 conversion. A subsequent gas cleaning stage was implemented to further improve gas quality and meet target purity standards. The upgraded gas composition reached 97.7% CH4, 2.2% CO2, and 0.97% O2, while H2S concentrations remained below detection limits. In addition, a flue gas-driven inorganic thermoelectric generator (TEG) system was designed and experimentally validated as a potential source of electricity for H2 production. The system consisted of six TEG modules connected in series and achieved an open-circuit voltage of 4.5 V and a maximum power output of 224 mW at a temperature difference of approximately 53.5 °C, demonstrating effective conversion of waste heat into electrical power under simulated flue gas conditions. Finally, a comprehensive techno-economic analysis was completed to evaluate the capital and operating costs associated with the proposed system. The results provide important insights to guide future scale-up, optimization, and potential deployment of integrated biological biogas upgrading technologies.

09 BIOMASS FUELS↗

Why Terminology Matters for Successful Rollout of Carbon Dioxide Utilization Technologies

To realize their full sustainability potential, carbon dioxide utilization technologies (carbon capture and utilization/CCU) presently require policy support. Consequently, they require acceptance among a variety of stakeholders in industry, policy making, and in the public sphere alike. While CO 2 utilization is already a topic of discourse among these stakeholders, there is a lack of common terminology to describe such technologies. On the contrary: The present article shows that terminology in the field of CO 2 utilization technologies is currently used inconsistently, and that different designations such as CCU, CCUS, or CDR convey different meanings and contexts. These ambiguities may cause communication problems with regard to policy making, funding proposals, and especially in public discourse. In order to initiate and accompany a goal-oriented and knowledge-based debate on CO 2 utilization technologies in the future, actors in the field are asked to question their own choices of terminology and to assess its accuracy. Acronyms and technical abbreviations are the chief cause of potential misunderstandings, and so should be avoided whenever possible or else include a brief explanation. Consistent and precise use of terminology will facilitate transparent dialogue concerning CO 2 utilization in the future.

54 ENVIRONMENTAL SCIENCES↗

Editorial: Harmonizing life cycle analysis (LCA) and techno-economic analysis (TEA) guidelines: a common framework for consistent conduct and transparent reporting of carbon dioxide removal and CCU technology appraisal

Stabilizing the climate will require significant efforts to curb greenhouse gas emissions, manage emissions that cannot be avoided, and remove as many legacy emissions as possible [i.e., carbon dioxide (International Energy Agency, 2020; Author Collective, 2022)]. In that context, negative emissions technologies will take CO 2 from the air (Direct Air Capture) or the water (Direct Ocean Capture) and permanently remove it (Roger et al., 2021) either by sequestering the CO 2 underground or converting it to so-called Track 1 materials (Sick et al., 2021) that have lifetimes of >100 years. Shorter-lived products that decompose back into CO 2 in <100 years are categorized as Track 2 materials and will at best be carbon neutral. A carbon neutral status can also be achieved if captured CO 2 from fossil-based point sources is sequestered or used to create Track 1 materials. Conversion of CO 2 from fossil-based sources to any Track 2 material and subsequent decomposition would add new fossil-based carbon to the atmosphere, constituting an ultimately undesirable process. The overall carbon footprint of a process or product will depend on many factors associated with the carbon production, use, and disposal phases.

54 ENVIRONMENTAL SCIENCES↗

Representing Carbon Dioxide Transport and Storage Network Investments within Power System Planning Models

Carbon dioxide (CO 2 ) capture and storage (CCS) is frequently identified as a potential component to achieving a decarbonized power system at least cost; however, power system models frequently lack detailed representation of CO 2 transportation, injection, and storage (CTS) infrastructure. In this paper, we present a novel approach to explicitly represent CO 2 storage potential and CTS infrastructure costs and constraints within a continental-scale power system capacity expansion model. In addition, we evaluate the sensitivity of the results to assumptions about the future costs and performance of CTS components and carbon capture technologies. We find that the quantity of CO 2 captured within the power sector is relatively insensitive to the range of CTS costs explored, suggesting that the cost of CO 2 capture retrofits is a more important driver of CCS implementation than the costs of transportation and storage. Finally, we demonstrate that storage and injection costs account for the predominant share of total costs associated with CTS investment and operation, suggesting that pipeline infrastructure costs have limited influence on the competitiveness of CCS.

24 POWER TRANSMISSION AND DISTRIBUTION↗

Life Cycle Assessment of Innovative Carbon Dioxide Selective Membranes from Low Carbon Emission Sources: A Comparative Study

Carbon capture has been an important topic of the twenty-first century because of the elevating carbon dioxide (CO2) levels in the atmosphere. CO2 in the atmosphere is above 420 parts per million (ppm) as of 2022, 70 ppm higher than 50 years ago. Carbon capture research and development has mostly been centered around higher concentration flue gas streams. For example, flue gas streams from steel and cement industries have been largely ignored due to lower associated CO2 concentrations and higher capture and processing costs. Capture technologies such as solvent-based, adsorption-based, cryogenic distillation, and pressure-swing adsorption are under research, but many suffer from higher costs and life cycle impacts. Membrane-based capture processes are considered cost-effective and environmentally friendly alternatives. Over the past three decades, our research group at Idaho National Laboratory has led the development of several polyphosphazene polymer chemistries and has demonstrated their selectivity for CO2 over nitrogen (N2). Poly[bis((2-methoxyethoxy)ethoxy)phosphazene] (MEEP) has shown the highest selectivity. A comprehensive life cycle assessment (LCA) was performed to determine the life cycle feasibility of the MEEP polymer material compared to other CO2-selective membranes and separation processes. The MEEP-based membrane processes emit at least 42% less equivalent CO2 than Pebax-based membrane processes. Similarly, MEEP-based membrane processes produce 34–72% less CO2 than conventional separation processes. In all studied categories, MEEP-based membranes report lower emissions than Pebax-based membranes and conventional separation processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Long-Term Dynamics of Atmospheric Sulfur Dioxide in Urban and Rural Regions of China: Urbanization and Policy Impacts

High levels of sulfur dioxide (SO 2 ) due to human activities pose a serious air pollution issue in China, especially in urban agglomerations. However, limited research has investigated the impact of anthropogenic emissions on higher SO 2 concentrations in urban regions compared to rural areas in China. Here, we analyzed the trends in SO 2 concentrations from 1980 to 2021 in China using the Modern-Era Retrospective Analysis for Research and Applications, version 2 (MERRA-2) dataset. SO 2 column concentrations from the Copernicus Atmosphere Monitoring Service (CAMS) and the Ozone Monitoring Instrument (OMI) during the years 2007–2021 were also examined for validation and comparison purposes. Eight representative areas, including four urban regions (Pearl River Delta [PRD], Beijing-Tianjin-Hebei [BTH], Yangtze River Delta [YRD], and Sichuan Basin [SCB]) and four rural regions (Northeast Region [NER], Mongolian Region [MR], West Region [WR], and Tibetan Plateau Region [TR]) were selected for the analysis. Overall, a significant but fluctuating increase in SO 2 concentrations over China was observed during 1980–2021. During 1980–1997 and 2000–2010, there was an increase in SO 2 concentration, while during 1997–2000 and 2010–2021, a decreasing trend was observed. The average increase in SO 2 concentration was approximately 16 times higher in urban regions than in the rural background. We also found that SO 2 dynamics were highly associated with expansion of urban areas, population density, and gross domestic product. Nonetheless, since 2007, SO 2 concentrations have exhibited a downward trend, which is mainly attributed to the air pollution policies implemented by the Chinese government. Our findings highlight the need for further studies on the impact of SO 2 on regional climate change in China.

54 ENVIRONMENTAL SCIENCES↗

Comparing the Use of High- to Low-Cost Black Carbon and Carbon Dioxide Sensors for Characterizing On-Road Diesel Truck Emissions

The exhaust plume capture method is a commonly used approach to measure pollutants emitted by in-use heavy-duty diesel trucks. Lower cost sensors, if used in place of traditional research-grade analyzers, could enable wider application of this method, including use as a monitoring tool to identify high-emitting trucks that may warrant inspection and maintenance. However, low-cost sensors have for the most part only been evaluated under ambient conditions as opposed to source-influenced environments with rapidly changing pollutant concentrations. This study compared black carbon (BC) emission factors determined using different BC and carbon dioxide (CO 2 ) sensors that range in cost from $200 to $20,000. Controlled laboratory experiments show that traditional zero and span steady-state calibration checks are not robust indicators of sensor performance when sampling short duration concentration peaks. Fleet BC emission factor distributions measured at two locations at the Port of Oakland in California with 16 BC/CO 2 sensor pairs were similar, but unique sensor pairs identified different high-emitting trucks. At one location, the low-cost PP Systems SBA-5 agreed on the classification of 90% of the high emitters identified by the LI-COR LI-7000 when both were paired with the Magee Scientific AE33. Conversely, lower cost BC sensors when paired with the LI-7000 misclassified more than 50% of high emitters when compared to the AE33/LI-7000. Confidence in emission factor quantification and high-emitter identification improves with larger integrated peak areas of CO 2 and especially BC. This work highlights that sensor evaluation should be conducted under application-specific conditions, whether that be for ambient air monitoring or source characterization.

47 OTHER INSTRUMENTATION↗

Biological Parts for Plant Biodesign to Enhance Land-Based Carbon Dioxide Removal

A grand challenge facing society is climate change caused mainly by rising CO 2 concentration in Earth’s atmosphere. Terrestrial plants are linchpins in global carbon cycling, with a unique capability of capturing CO 2 via photosynthesis and translocating captured carbon to stems, roots, and soils for long-term storage. However, many researchers postulate that existing land plants cannot meet the ambitious requirement for CO 2 removal to mitigate climate change in the future due to low photosynthetic efficiency, limited carbon allocation for long-term storage, and low suitability for the bioeconomy. To address these limitations, there is an urgent need for genetic improvement of existing plants or construction of novel plant systems through biosystems design (or biodesign). Here, we summarize validated biological parts (e.g., protein-encoding genes and noncoding RNAs) for biological engineering of carbon dioxide removal (CDR) traits in terrestrial plants to accelerate land-based decarbonization in bioenergy plantations and agricultural settings and promote a vibrant bioeconomy. Specifically, we first summarize the framework of plant-based CDR (e.g., CO 2 capture, translocation, storage, and conversion to value-added products). Then, we highlight some representative biological parts, with experimental evidence, in this framework. Finally, we discuss challenges and strategies for the identification and curation of biological parts for CDR engineering in plants.

59 BASIC BIOLOGICAL SCIENCES↗

A new method for inferring city emissions and lifetimes of nitrogen oxides from high-resolution nitrogen dioxide observations: a model study

We present a new method to infer emissions and lifetimes of nitrogen oxides (NO x ) based on tropospheric nitrogen dioxide (NO 2 ) observations together with reanalysis wind fields for cities located in polluted backgrounds. Since the accuracy of the method is difficult to assess due to lack of “true values” that can be used as a benchmark, we apply the method to synthetic NO 2 observations derived from the NASA-Unified Weather Research and Forecasting (NU-WRF) model at a high horizontal spatial resolution of 4 km × 4 km for cities over the continental United States. We compare the inferred emissions and lifetimes with the values given by the NU-WRF model to evaluate the method. The method is applicable to 26 US cities. The derived results are generally in good agreement with the values given by the model, with the relative differences of 2 % ± 17 % (mean ± standard deviation) and 15 % ± 25 % for lifetimes and emissions, respectively. Our investigation suggests that the use of wind data prior to the satellite overpass time improves the performance of the method. The correlation coefficients between inferred and NU-WRF lifetimes increase from 0.56 to 0.79 and for emissions increase from 0.88 to 0.96 when comparing results based on wind fields sampled simultaneously with satellite observations and averaged over 9 h data prior to satellite observations, respectively. We estimate that uncertainties in NO x lifetime and emissions arising from the method are approximately 15 % and 20 %, respectively, for typical (US) cities. The total uncertainties reach up to 43% (lifetimes) and 45% (emissions) by considering the additional uncertainties associated with satellite NO 2 observations and wind data. We expect this new method to be applicable to NO 2 observations from the TROPOspheric Monitoring Instrument (TROPOMI) and geostationary satellites, such as Geostationary Environment Monitoring Spectrometer (GEMS) or the Tropospheric Emissions: Monitoring Pollution (TEMPO) instrument, to estimate urban NO x emissions and lifetimes globally.

54 ENVIRONMENTAL SCIENCES↗

High-resolution mapping of nitrogen oxide emissions in large US cities from TROPOMI retrievals of tropospheric nitrogen dioxide columns

Satellite-derived spatiotemporal patterns of nitrogen oxide (NOx) emissions can improve accuracy of emission inventories to better support air quality and climate research and policy studies. In this study, we develop a new method by coupling the chemical transport Model-Independent SATellite-derived Emission estimation Algorithm for Mixed-sources (MISATEAM) with a divergence method to map high-resolution NO x emissions across US cities using TROPOspheric Monitoring Instrument (TROPOMI) tropospheric nitrogen dioxide (NO 2 ) retrievals. The accuracy of the coupled method is validated through application to synthetic NO 2 observations from the NASA-Unified Weather Research and Forecasting (NU-WRF) model, with a horizontal spatial resolution of 4 km × 4 km for 33 large and mid-size US cities. Validation reveals excellent agreement between inferred and NU-WRF-provided emission magnitudes (R= 0.99, normalized mean bias, NMB = —0.01) and a consistent spatial pattern when comparing emissions for individual grid cells (R = 0.88 ± 0.06). We then develop a TROPOMI-based database reporting annual emissions for 39 US cities at a horizontal spatial resolution of 0.05° × 0.05° from 2018 to 2021. This database demonstrates a strong correlation (R= 0.90) with the National Emission Inventory (NEI) but reveals some bias (NMB = —0.24). There are noticeable differences in the spatial patterns of emissions in some cities. Our analysis suggests that uncertainties in TROPOMI-based emissions and potential misallocation of emissions and/or missing sources in bottom-up emission inventories both contribute to these differences.

54 ENVIRONMENTAL SCIENCES↗

Cloud processing of dimethyl sulfide (DMS) oxidation products limits sulfur dioxide (SO 2 ) and carbonyl sulfide (OCS) production in the eastern North Atlantic marine boundary layer

Dimethyl sulfide (DMS) is the major sulfur species emitted from the ocean. The gas-phase oxidation of DMS by hydroxyl radicals proceeds through the stable, soluble intermediate hydroperoxymethyl thioformate (HPMTF), eventually forming carbonyl sulfide (OCS) and sulfur dioxide (SO 2 ). Recent work has shown that HPMTF is efficiently lost to marine boundary layer (MBL) clouds, thus arresting OCS and SO 2 production and their contributions to new-particle formation and growth events. To date, no long-term field studies exist to assess the extent to which frequent cloud processing impacts the fate of HPMTF. Here, we present 6 weeks of measurements of the cloud fraction and the marine sulfur species methanethiol, DMS, and HPMTF made at the Atmospheric Radiation Measurement (ARM) research facility on Graciosa Island, Azores, Portugal. Using an observationally constrained chemical box model, we determine that cloud loss is the dominant sink of HPMTF in this region of the MBL during the study, accounting for 79 %–91 % of HPMTF loss on average. When accounting for HPMTF uptake to clouds, we calculate campaign average reductions in DMS-derived MBL SO 2 and OCS of 52 %–60 % and 80 %–92 % for the study period. Using yearly measurements of the site- and satellite-measured 3D cloud fraction and DMS climatology, we infer that HPMTF cloud loss is the dominant sink of HPMTF in the eastern North Atlantic during all seasons and occurs on timescales faster than what is prescribed in global chemical transport models. Accurately resolving this rapid loss of HPMTF to clouds has important implications for constraining drivers of MBL new-particle formation.

54 ENVIRONMENTAL SCIENCES↗

Using atmospheric observations to quantify annual biogenic carbon dioxide fluxes on the Alaska North Slope

The continued warming of the Arctic could release vast stores of carbon into the atmosphere from high-latitude ecosystems, especially from thawing permafrost. Increasing uptake of carbon dioxide (CO 2 ) by vegetation during longer growing seasons may partially offset such release of carbon. However, evidence of significant net annual release of carbon from site-level observations and model simulations across tundra ecosystems has been inconclusive. To address this knowledge gap, we combined top-down observations of atmospheric CO 2 concentration enhancements from aircraft and a tall tower, which integrate ecosystem exchange over large regions, with bottom-up observed CO 2 fluxes from tundra environments and found that the Alaska North Slope is not a consistent net source nor net sink of CO 2 to the atmosphere (ranging from ₋6 to +6 Tg C yr -1 for 2012–2017). Our analysis suggests that significant biogenic CO 2 fluxes from unfrozen terrestrial soils, and likely inland waters, during the early cold season (September–December) are major factors in determining the net annual carbon balance of the North Slope, implying strong sensitivity to the rapidly warming freeze-up period. At the regional level, we find no evidence of the previously reported large late-cold-season (January–April) CO 2 emissions to the atmosphere during the study period. Despite the importance of the cold-season CO 2 emissions to the annual total, the interannual variability in the net CO 2 flux is driven by the variability in growing season fluxes. During the growing season, the regional net CO 2 flux is also highly sensitive to the distribution of tundra vegetation types throughout the North Slope. This study shows that quantification and characterization of year-round CO 2 fluxes from the heterogeneous terrestrial and aquatic ecosystems in the Arctic using both site-level and atmospheric observations are important to accurately project the Earth system response to future warming.

54 ENVIRONMENTAL SCIENCES↗

Annual carbon dioxide flux over seasonal sea ice in the Canadian Arctic

Continuous measurements of carbon dioxide (CO 2 ) flux were collected from a 10 m eddy covariance tower in a coastal-marine environment in the Canadian Arctic Archipelago over the course of a 17-month period. The extended length of data collection resulted in a unique dataset that includes measurements from two spring melt and summer seasons and one autumn freeze-up. These field observations were used to verify findings from previous theoretical and laboratory experiments investigating air-sea gas exchange in connection with sea ice. The results corroborated previous findings showing that thick ice cover under winter conditions acts as a barrier to gas exchange. In the spring, CO 2 fluxes were downward (uptake) in both the presence of melt ponds and during ice break-up. However, diurnal cycles were present throughout the early spring melt period, corresponding to the opposing influences of freezing and melting at the ice surface. Fluxes measured during melt periods confirmed previous laboratory tank measurements that showed a gas transfer coefficient of melting ice of 0.4 mol m −2 d −1 atm −1 . Open water CO 2 fluxes showed outgassing in early summer and uptake in mid-to-late summer, tied closely to trends in surface water temperature and its effect on the partial pressure of CO 2 in the water. The autumn period of the field campaign represents the first eddy covariance CO 2 fluxes measured over naturally forming sea ice. Our measurements showed mean upward fluxes (outgassing) of 1.1±1.5 mmol m −2 d −1 associated with the freezing of ice – the same order of magnitude found by previous laboratory tank experiments. However, peak flux periods during ice formation had measured fluxes that were a factor of 3 higher than the tank experiments, suggesting the importance of natural conditions (e.g., wind) on air-ice gas exchange. Conducting an Arctic-wide extrapolation we estimate CO 2 outgassing from the freezing period to be a counterbalance equivalent to 5 to 15 % of the magnitude of the estimated Arctic CO 2 sink. Overall, there was no evidence of dramatically enhanced gas exchange in marginal ice conditions as proposed by previous studies. Although the different seasons showed active CO 2 exchange, there was a balance between upward and downward fluxes at this specific location, resulting in a small net CO 2 uptake over the annual cycle of −0.3 g C m −2 .

54 ENVIRONMENTAL SCIENCES↗