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DOE OSTI2013

Volumetrics of CO{sub 2} Storage in Deep Saline Formations

Concern about the role of greenhouse gases in global climate change has generated interest in sequestering CO{sub 2} from fossil-fuel combustion in deep saline formations. Pore space in these formations is initially filled with brine, and space to accommodate injected CO{sub 2} must be generated by displacing brine, and to a lesser extent by compression of brine and rock. The formation volume required to store a given mass of CO{sub 2} depends on the storage mechanism. We compare the equilibrium volumetric requirements of three end-member processes: CO{sub 2} stored as a supercritical fluid (structural or stratigraphic trapping); CO{sub 2} dissolved in pre-existing brine (solubility trapping); and CO{sub 2} solubility enhanced by dissolution of calcite. For typical storage conditions, storing CO{sub 2} by solubility trapping reduces the volume required to store the same amount of CO{sub 2} by structural or stratigraphic trapping by about 50%. Accessibility of CO{sub 2} to brine determines which storage mechanism (structural/stratigraphic versus solubility) dominates at a given time, which is a critical factor in evaluating CO{sub 2} volumetric requirements and long-term storage security.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

High-Performance Rh 2 P Electrocatalyst for Efficient Water Splitting

The search for active, stable, and cost-efficient electrocatalysts for hydrogen production via water splitting could make a substantial impact on energy technologies that do not rely on fossil fuels. Here we report the synthesis of rhodium phosphide electrocatalyst with low metal loading in the form of nanocubes (NCs) dispersed in high-surface-area carbon (Rh2P/C) by a facile solvo-thermal approach. The Rh2P/C NCs exhibit remarkable performance for hydrogen evolution reaction and oxygen evolution reaction compared to Rh/C and Pt/C catalysts. The atomic structure of the Rh2P NCs was directly observed by annular dark-field scanning transmission electron microscopy, which revealed a phosphorus-rich outermost atomic layer. Combined experimental and computational studies suggest that surface phosphorus plays a crucial role in determining the robust catalyst properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2019

SO 2 -Induced Selectivity Change in CO 2 Electroreduction

Electrochemical conversion of carbon dioxide (CO 2 ) to value-added chemicals has attracted much attention in recent years as a potential alternative to fossil resources. Although significant works have studied the influence of impurities in the electrolyte (e.g. metal ions), few studies have been performed to understand the influence of gaseous impurities in CO 2 electroreduction. Herein, we study the effects of sulfur dioxide (SO 2 ) on Ag-, Sn-, and Cu-catalyzed CO 2 electrolysis in a flow-cell electrolyzer in near-neutral electrolyte, representing a broad range of CO 2 reduction catalysts. We show that the presence of SO 2 impurity reduces the efficiency of converting CO 2 due to the preferential reduction of SO 2 . In the case of Ag and Sn, the effect of SO 2 impurity was reversible and the catalytic activities of both catalysts were recovered. On the contrary, a shift in selectivity toward formate accompanied with a suppression of multi-carbon (C 2+ ) products was observed on Cu catalyst, demonstrating that Cu is highly sensitive to SO 2 impurity. Furthermore, our results suggest that CO 2 obtained from direct air capture technologies or biorefineries could be more suitable for Cu-catalyzed CO 2 electrolysis as these CO 2 sources would be relatively cleaner (SO 2 -free) than fossil-derived sources such as power plants and can be directly coupled with distributed renewable energy sources such as wind and solar.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2012

The influence of internal model variability in GEOS-5 on interhemispheric CO 2 exchange

An ensemble of eight atmospheric CO 2 simulations was completed employing the National Aeronautics and Space Administration (NASA) Goddard Earth Observation System, Version 5 (GEOS–5) for the years 2000–2001, each with initial meteorological conditions corresponding to different days in January 2000 to examine internal model variability. Globally, the model runs show similar concentrations of CO 2 for the two years, but in regions of high CO 2 concentrations due to fossil fuel emissions, large differences among different model simulations appear. The phasing and amplitude of the CO 2 cycle at Northern Hemisphere locations in all of the ensemble members is similar to that of surface observations. In several southern hemisphere locations, however, some of the GEOS–5 model CO 2 cycles are out of phase by as much as four months, and large variations occur between the ensemble members. This result indicates that there is large sensitivity to transport in these regions. The differences vary by latitude—the most extreme differences in the Tropics and the least at the South Pole. Examples of these differences among the ensemble members with regard to CO 2 uptake and respiration of the terrestrial biosphere and CO 2 emissions due to fossil fuel emissions are shown at Cape Grim, Tasmania. Integration–based flow analysis of the atmospheric circulation in the model runs shows widely varying paths of flow into the Tasmania region among the models including sources from North America, South America, South Africa, South Asia and Indonesia. Furthermore, these results suggest that interhemispheric transport can be strongly influenced by internal model variability.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Climate Forcing and Trends of Organic Aerosols in the Community Earth System Model (CESM2)

The Community Earth System Model version 2 (CESM2) includes three main atmospheric configurations: the Community Atmosphere Model version 6 (CAM6) with simplified chemistry and a simplified organic aerosol (OA) scheme, CAM6 with comprehensive tropospheric and stratospheric chemistry representation (CAM6-chem), and the Whole Atmosphere Community Climate Model version 6 (WACCM6). Both, CAM6-chem and WACCM6 include a more comprehensive secondary organic aerosols (SOA) approach using the volatility basis set (vbs) scheme and prognostic stratospheric aerosols. This paper describes the different OA schemes available in the different atmospheric configurations of CESM2 and discusses differences in aerosol burden and resulting climate forcings. Derived OA burden and trends differ due to differences in OA formation using the different approaches. Regional differences in Aerosol Optical Depth with larger values using the comprehensive approach occur over SOA source regions. Stronger increasing SOA trends between 1960 and 2015 in WACCM6 compared to CAM6 are due to increasing biogenic emissions aligned with increasing surface temperatures. Using the comprehensive SOA approach further leads to improved comparisons to aircraft observations and SOA formation of ˜143 Tg/yr. We further use WACCM6 to identify source contributions of OA from biogenic, fossil fuel, and biomass burning emissions, to quantify SOA amounts and trends from these sources. Increasing SOA trends between 1960 and 2015 are the result of increasing biogenic emissions aligned with increasing surface temperatures. Biogenic emissions are at least two thirds of the total SOA burden. In addition, SOA source contributions from fossil fuel emissions become more important, with largest values over Southeast Asia. The estimated total anthropogenic forcing of OA in WACCM6 for 1995–2010 conditions is -0.43 W/m2, mostly from the aerosol direct effect.

Tilmes, S↗

DOE OSTI2021

4D Proxy Imaging of Fracture Dilation and Stress Shadowing Using Electrical Resistivity Tomography During High Pressure Injections into a Dense Rock Formation

Fluid flow through fractured rock systems is governed in large part by the distribution, interconnectivity, and size of fracture apertures. In-situ stress is one of the primary factors controlling fracture aperture, and one that is altered significantly during high-pressure fluid injections or extractions. Interactions between stress, pore pressure, aperture, and fluid flow can result in complex and evolving poroelastic behavior with significant implications regarding the predictability and risk of developing and managing deep subsurface reservoirs (geothermal, fossil energy, and geologic carbon sequestration). In saturated crystalline rocks, bulk electrical conductivity is highly sensitive to porosity, and therefore to fracture aperture size and distribution. We demonstrate the use of time-lapse 3D electrical resistivity tomography for remotely monitoring stress induced changes in aperture distribution during high pressure injections into a fractured rock system at a scale of tens of meters. Results reveal a complex and continuously evolving stress field involving aperture dilations in the natural fracture system and aperture contractions in adjacent zones of shadow stress. Results provide information about the spatiotemporal changes in the system behavior and point to the potential of electrical imaging for autonomously and remotely monitoring evolving stress conditions by proxy through changes in bulk electrical conductivity.

electrical resisitivity tomography, stress, 4D Tim↗

DOE OSTI2023

Scenario Discovery Analysis of Drivers of Solar and Wind Energy Transitions Through 2050

Deep human-Earth system uncertainties and strong multi-sector dynamics make it difficult to anticipate which conditions are most likely to lead to higher or lower adoption of renewable energy, and models project a broad range of future solar and wind energy shares across future scenarios. To elucidate these dynamics, we explore a large data set of scenarios simulated from the Global Change Analysis Model (GCAM) and use scenario discovery to identify the most significant factors affecting solar and wind adoption by mid-century. We generated a data set of over 4,000 scenarios from GCAM by varying 12 different socioeconomic factors at high and low levels, including assumptions about future energy demand, resource costs, and fossil fuel emissions paths, as well as specific technology assumptions including wind and solar backup requirements and storage costs. Using scenario discovery, we assess the most important factors globally and regionally in creating high fractions of solar and wind energy and explore interconnected effects on other systems including water and non-CO 2 emissions. Globally and regionally, we found that solar and wind-related technology costs were the primary drivers of high wind and solar energy adoption, though a few regions depend heavily on other parameters like carbon capture and storage costs, population and gross domestic product trajectories, and fossil fuel costs. We also identify four key paths to high solar and wind energy by mid-century and discuss their tradeoffs in terms of other outcomes.

14 SOLAR ENERGY↗

DOE OSTI2022

Using Multiscale Ethane/Methane Observations to Attribute Coal Mine Vent Emissions in the San Juan Basin From 2013 to 2021

Abstract Source attribution of natural gas emissions from fossil fuels in New Mexico's San Juan Basin (SJB) is challenging due to source heterogeneity and emissions transience. We demonstrate that ethane (C 2 H 6 ) to methane (CH 4 ) mixing ratios can identify and separate sources over different scales using various measurement techniques. We report simultaneous CH 4 and C 2 H 6 observations near a coal mine vent and oil and gas (O&G) emission sources using ground‐based in situ measurements in 2020/2021. During these campaigns, we observed a stable coal vent C 2 H 6 :CH 4 ratio of 1.28% ± 0.11%, discernibly different than nearby O&G source ratios ranging from 0.9% to 16.8%. We analyze airborne observations of the SJB taken in 2014/2015 that exhibit similar coal vent ratios and further show the region's heterogeneity. We identify episodic O&G sources, including a gas plant source detected in 2014/2015 that is absent in our 2020/2021 data. We examine total column observations of C 2 H 6 and CH 4 made in 2013 with a solar spectrometer and find a C 2 H 6 :CH 4 ratio of 1.3% ± 0.4% for the coal vent. The stable and unique coal vent ratio relative to other O&G sources in the region is used to demonstrate that consistent attribution is possible using various measurement methods at multiple scales across many years. Finally, we demonstrate that using C 2 H 6 as a proxy for fossil CH 4 inversions can inform detailed basin‐scale inversions, provided we understand source specific changes in the C 2 H 6 :CH 4 ratio like we report in the SJB.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Radiocarbon Fingerprinting Black Carbon Source History in the Himalayas

Abstract Black carbon (BC) is considered as an important contributor to the Himalayan glaciers melt in the past few decades. However, the long‐term source apportionment of BC remains unclear. Here we present the first radiocarbon ( 14 C)‐based annual variation of BC source apportionment in an ice core spanning the period of 1959–2012 drilled from the Southeastern Tibetan Plateau, a receptor site of South Asia outflow. We find fossil fuel combustion is a major contribution (73% ± 5%), yet the biomass burning fraction ( ƒ biomass ) has grown from 24% ± 4% to 30% ± 4% since 1990. Intriguingly, we further find the ƒ biomass demonstrating a robust correlation with South Asian wildfires linked to climate oscillations. Thus, for mitigating BC impacts on Himalayan glaciers, South Asia's transition from fossil fuels to clean energy is a more efficient and urgent strategy than reducing residential biomass burning.

Wang, Mo [State Key Laboratory of Tibetan Plateau ↗

DOE OSTI2015

Impact of solar panels on global climate

Regardless of the harmful effects of burning fossil fuels on global climate1,2, other energy sources will become more important in the future because fossil fuels could run out by the early twenty-second century3 given the present rate of consumption4. This implies that sooner or later humanity will rely heavily on renewable energy sources. Here we model the effects of an idealized large-scale application of renewable energy on global and regional climate relative to a background climate of the representative concentration pathway 2.6 scenario (RCP2.6; ref. 5). We find that solar panels alone induce regional cooling by converting incoming solar energy to electricity in comparison to the climate without solar panels. The conversion of this electricity to heat, primarily in urban areas, increases regional and global temperatures which compensate the cooling effect. However, there are consequences involved with these processes that modulate the global atmospheric circulation, resulting in changes in regional precipitation.

Environmental Sciences & Ecology↗

DOE OSTI2015

Southward shift of the northern tropical belt from 1945 to 1980

Geology↗

DOE OSTI2023

A cost comparison of various hourly-reliable and net-zero hydrogen production pathways in the United States

Hydrogen (H 2 ) as an energy carrier may play a role in various hard-to-abate subsectors, but to maximize emission reductions, supplied hydrogen must be reliable, low-emission, and low-cost. Here, we build a model that enables direct comparison of the cost of producing net-zero, hourly-reliable hydrogen from various pathways. To reach net-zero targets, we assume upstream and residual facility emissions are mitigated using negative emission technologies. For the United States (California, Texas, and New York), model results indicate next-decade hybrid electricity-based solutions are lower cost ($2.02-$2.88/kg) than fossil-based pathways with natural gas leakage greater than 4% ($2.73-$5.94/kg). These results also apply to regions outside of the U.S. with a similar climate and electric grid. However, when omitting the net-zero emission constraint and considering the U.S. regulatory environment, electricity-based production only achieves cost-competitiveness with fossil-based pathways if embodied emissions of electricity inputs are not counted under U.S. Tax Code Section 45V guidance.

08 HYDROGEN↗

DOE OSTI2026

Solventless, Ambient-Pressure Production of Bio-Based Lactones Over Earth-Abundant, Mixed Metal Oxide Catalysts for Circular Polyesters

Transitioning to a circular plastics economy will require use of renewable feedstocks, energy-efficient processes, and closed-loop recyclable polymers, such as polyesters. A key challenge lies in sustainably sourcing monomers used to make recyclable polyesters. This work presents a catalytic platform utilizing earth-abundant Cu(x)Ca(1-x)O mixed metal oxides for the oxidative dehydrocyclization of bio-based diols to lactones, which are advantaged for energy-efficient ring-opening polymerization. Operating below 200 degrees C, at ambient pressure, and without solvent, the process uses air as the sole oxidant, achieving high yields of lactones across a broad substrate scope of C4-8 diols in the liquid phase. The oxidative dehydrocyclization reaction is thermodynamically downhill due to water formation and energy-efficient compared to incumbent, non-redox pathways utilized in fossil carbon-based industrial processes for lactone production. Mechanistic studies reveal facile redox cycling of Cu2+-O(Ca2+)-Cu2+ interfacial sites unique to the developed catalyst. Techno-economic analysis and life cycle assessment estimate 40% lower energy demand and 15% lower GHG intensity per mass of butyrolactone produced compared to the fossil carbon-based route. Liquid-phase oxidative dehydrocyclization offers a promising approach for scalable lactone production from renewable, bio-based diols to enable circular polyesters.

36 MATERIALS SCIENCE↗

DOE OSTI2019

The development of molecular water oxidation catalysts

There is an urgent need to transition from fossil fuels to solar fuels $-$ not only to lower CO 2 emissions that cause global warming but also to ration fossil resources. Splitting H 2 O with sunlight emerges as a clean and sustainable energy conversion scheme that can afford practical technologies in the short-to-mid-term. A crucial component in such a device is a water oxidation catalyst (WOC). These artificial catalysts have been developed mainly over the past two decades, which is in contrast to nature’s WOCs, which have featured in its photosynthetic apparatus for more than a billion years. Recent times have seen the development of increasingly active molecular WOCs, the study of which affords an understanding of catalytic mechanisms and decomposition pathways. This Perspective offers a historical description of the landmark molecular WOCs, particularly ruthenium systems, that have guided research to our present degree of understanding.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Bio-Based Polymers with Performance-Advantaged Properties

Bio-based compounds with unique chemical functionality can be obtained through selective transformations of plant and other non-fossil, biogenic feedstocks for the development of new polymers to displace those produced from fossil carbon feedstocks. Although substantial efforts have been invested to produce bio-based polymers that are chemically identical to and directly replace those from petroleum, a long-pursued goal is to synthesize new, sustainable, bio-based polymers that either functionally replace or exhibit performance advantages relative to incumbent polymers. Owing to anthropogenic climate change and the environmental consequences of global plastics pollution, the need to realize a bio-based materials economy at scale is critical. To that end, in this Review we describe the concept of performance-advantaged, bio-based polymers (PBPs), highlighting examples wherein superior performance is facilitated by the inherent chemical functionality of bio-based feedstocks. We focus on PBPs with C–O and C–N inter-unit chemical bonds, as these are often readily accessible from bio-based feedstocks, which are heteroatom-rich relative to petroleum-derived feedstocks. Finally, we outline guiding principles and challenges to aid progress in the development of PBPs.

bio-based feedstock↗

DOE OSTI2018

Impaired photosynthesis and increased leaf construction costs may induce floral stress during episodes of global warming over macroevolutionary timescales

Global warming events have coincided with turnover of plant species at intervals in Earth history. As mean global temperatures rise, the number, frequency and duration of heat-waves will increase. Ginkgo biloba was grown under controlled climatic conditions at two different day/night temperature regimes (25/20 °C and 35/30 °C) to investigate the impact of heat stress. Photosynthetic CO 2 -uptake and electron transport were reduced at the higher temperature, while rates of respiration were greater; suggesting that the carbon balance of the leaves was adversely affected. Stomatal conductance and the potential for evaporative cooling of the leaves was reduced at the higher temperature. Furthermore, the capacity of the leaves to dissipate excess energy was also reduced at 35/30 °C, indicating that photo-protective mechanisms were no longer functioning effectively. Leaf economics were adversely affected by heat stress, exhibiting an increase in leaf mass per area and leaf construction costs. This may be consistent with the selective pressures experienced by fossil Ginkgoales during intervals of global warming such as the Triassic - Jurassic boundary or Early Eocene Climatic Optimum. The physiological and morphological responses of the $G$. biloba leaves were closely interrelated; these relationships may be used to infer the leaf economics and photosynthetic/stress physiology of fossil plants.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2019

The Impact of Future Fuel Consumption on Regional Air Quality in Southeast Asia

Aerosols emitted from fossil fuel burning can cause air quality and human health issues. In this sensitivity study, we examine the impact of fossil fuel aerosols on air quality in Southeast Asia under five different hypothetical fuel consumption scenarios. These scenarios reflect air pollutant outcomes of implementations of certain idealized policies in the power generation, industry, and residential sectors. Analyses based on comparison among the modeling results from these scenarios reveal the sectors that should be targeted by air pollution mitigation policy. The results reveal that in Southeast Asia, sulfate could be decreased by 25% if coal were to be replaced by natural gas in the power generation and industry sectors. Black carbon concentration would reduce 42% overall if biofuel were replaced by natural gas in the residential sector. Shipping emissions are especially critical for the urban air quality in Singapore: fine particular matters (PM 2.5 ) could be dramatically cut by 69% in Singapore by merely eliminating shipping emissi

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Mechanisms of soft tissue and protein preservation in Tyrannosaurus rex

Abstract The idea that original soft tissue structures and the native structural proteins comprising them can persist across geological time is controversial, in part because rigorous and testable mechanisms that can occur under natural conditions, resulting in such preservation, have not been well defined. Here, we evaluate two non-enzymatic structural protein crosslinking mechanisms, Fenton chemistry and glycation, for their possible contribution to the preservation of blood vessel structures recovered from the cortical bone of a Tyrannosaurus rex (USNM 555000 [formerly, MOR 555]). We demonstrate the endogeneity of the fossil vessel tissues, as well as the presence of type I collagen in the outermost vessel layers, using imaging, diffraction, spectroscopy, and immunohistochemistry. Then, we use data derived from synchrotron FTIR studies of the T. rex vessels to analyse their crosslink character, with comparison against two non-enzymatic Fenton chemistry- and glycation-treated extant chicken samples. We also provide supporting X-ray microprobe analyses of the chemical state of these fossil tissues to support our conclusion that non-enzymatic crosslinking pathways likely contributed to stabilizing, and thus preserving, these T. rex vessels. Finally, we propose that these stabilizing crosslinks could play a crucial role in the preservation of other microvascular tissues in skeletal elements from the Mesozoic.

59 BASIC BIOLOGICAL SCIENCES↗