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DOE OSTI2020

Recent advances in polymeric facilitated transport membranes for carbon dioxide separation and hydrogen purification

Membrane and membrane process have been widely considered as one of the best candidates for mitigating CO 2 emissions from the combustion or utilization of fossil fuels. Various amine-containing polymers constitute an important class of membranes, where the highly selective CO 2 transport is achieved by the facilitated transport mechanism. In this review, the amine–CO 2 chemistry is discussed in conjunction with the mechanism of the reaction-mediated CO 2 transport. A wide variety of amine-containing polymers are discussed based on two synthesis motifs: (a) polyamines with amino groups covalently bound to the polymer backbone and (b) small molecule amines embedded in a polymer matrix. This review concludes with the remarks on the facilitated transport membranes for post-combustion carbon capture (CO 2 /N 2 ) and hydrogen purification (CO 2 /H 2 ).

42 ENGINEERING↗

DOE OSTI2020

ToF-SIMS Analysis of Chemical Composition of Atmospheric Aerosols in Beijing

Atmospheric aerosols collected from each season in urban Beijing have been studied using time-of-flight secondary ion mass spectrometry (ToF-SIMS). The chemical composition of atmospheric aerosol particles during various atmospheric pollution levels were analyzed and distinguished by principal component analysis (PCA). The differences and sources of the components of the aerosol particles were explored. The results showed that the fine particulate matter from heavily polluted days mainly consists of inorganic salts and organic compounds, such as hydrocarbons, nitrogen- or sulfur-containing hydrocarbons, and their oxides. Samples collected from clean days in the four seasons were also analyzed. Only the samples collected in spring showed a significant difference from the other three seasons. We concluded that the main source of pollution in the Beijing urban area was fossil fuel combustion from motor vehicles.

ToF-SIMS, principal component analysis↗

DOE OSTI2024

Cu Based Dilute Alloys for Tuning the C 2+ Selectivity of Electrochemical CO 2 Reduction

Electrochemical CO 2 reduction is a promising technology for replacing fossil fuel feedstocks in the chemical industry but further improvements in catalyst selectivity need to be made. So far, only copper-based catalysts have shown efficient conversion of CO 2 into the desired multi-carbon (C 2+ ) products. This work explores Cu-based dilute alloys to systematically tune the energy landscape of CO 2 electrolysis toward C 2+ products. Selection of the dilute alloy components is guided by grand canonical density functional theory simulations using the calculated binding energies of the reaction intermediates CO*, CHO*, and OCCO* dimer as descriptors for the selectivity toward C 2+ products. Here, a physical vapor deposition catalyst testing platform is employed to isolate the effect of alloy composition on the C 2+ /C 1 product branching ratio without interference from catalyst morphology or catalyst integration. Six dilute alloy catalysts are prepared and tested with respect to their C 2+ /C 1 product ratio using different electrolyzer environments including selected tests in a 100-cm 2 electrolyzer. Consistent with theory, CuAl, CuB, CuGa and especially CuSc show increased selectivity toward C 2+ products by making CO dimerization energetically more favorable on the dominant Cu facets, demonstrating the power of using the dilute alloy approach to tune the selectivity of CO 2 electrolysis.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Sustainable Production of Biomass‐Derived Graphite and Graphene Conductive Inks from Biochar

Abstract Graphite is a commonly used raw material across many industries and the demand for high‐quality graphite has been increasing in recent years, especially as a primary component for lithium‐ion batteries. However, graphite production is currently limited by production shortages, uneven geographical distribution, and significant environmental impacts incurred from conventional processing. Here, an efficient method of synthesizing biomass‐derived graphite from biochar is presented as a sustainable alternative to natural and synthetic graphite. The resulting bio‐graphite equals or exceeds quantitative quality metrics of spheroidized natural graphite, achieving a RamanI D /I G ratio of 0.051 and crystallite size parallel to the graphene layers (L a ) of 2.08 µm. This bio‐graphite is directly applied as a raw input to liquid‐phase exfoliation of graphene for the scalable production of conductive inks. The spin‐coated films from the bio‐graphene ink exhibit the highest conductivity among all biomass‐derived graphene or carbon materials, reaching 3.58 ± 0.16 × 10 4 S m −1 . Life cycle assessment demonstrates that this bio‐graphite requires less fossil fuel and produces reduced greenhouse gas emissions compared to incumbent methods for natural, synthesized, and other bio‐derived graphitic materials. This work thus offers a sustainable, locally adaptable solution for producing state‐of‐the‐art graphite that is suitable for bio‐graphene and other high‐value products.

Chemistry↗

DOE OSTI2022

Codesigning Alloy Compositions of CdSe y Te 1− y Absorbers and Mg x Zn 1− x O Contacts to Increase Solar Cell Efficiency

Thin‐film solar cells such as CdTe are a major commercial photovoltaic technology, with more than 25 GW installed worldwide and levelized costs of electricity competitive with fossil fuels. Further progress may result from integrating CdSe y Te 1− y absorbers with Mg x Zn 1− x O contacts, but the device efficiency is difficult to maximize due to coupled dependence on chemical composition of both alloys. Herein, a high‐throughput approach is demonstrated to codesign chemical compositions in alloyed Mg x Zn 1− x O/CdSe y Te 1− y thin‐film solar cells, using combinatorial libraries of PV devices with orthogonal composition gradients in CdSe y Te 1− y absorbers and Mg x Zn 1− x O contacts. It is found that the solar cell performance is a strong and coupled function of both elemental compositions, with efficiency up to 17.7% ( V OC = 836 mV, fill factor = 69%, J SC = 30.6 mA cm −2 ) at atomic compositions of Mg/(Mg + Zn) ≈18% and average Se/(Se + Te) ≈4%. These performance trends among >100 devices are explained by >100 ns lifetime of photoexcited charge carriers at the Mg x Zn 1− x O/CdSe y Te 1− y interface where strong Se accumulation is also observed. This study reports the optimal compositions of the commercially relevant Mg x Zn 1− x O/CdSe y Te 1− y solar cells and demonstrates a general approach to codesigning performance of alloyed thin‐film solar cells and other optoelectronic devices.

14 SOLAR ENERGY↗

DOE OSTI2016

What can molecular simulation do for global warming?

Carbon capture is necessary to reduce CO 2 emissions from burning fossil fuels, which has led to global warming. Molecular simulations offer chemical insights and design principles for new separation media and for understanding the separation process. In this review, we summarize recent applications of simulation methods from ab initio and density functional theory to classical molecular dynamics and Grand canonical Monte Carlo in understanding ionic liquids and porous carbonaceous materials for CO 2 separation, especially the postcombustion CO 2 / N 2 separation. We highlight design and simulation of the porous two‐dimensional ( 2D ) materials as the highly selective membranes for CO 2 separation. Simulated structure–property relationships for the materials are discussed in connection to the corresponding chemisorption, physisorption, or membrane process. In chemisorption, the focus is on reducing the heat of reaction with CO 2 ; in physisorption, the key is to increase the binding strength via CO 2 ‐philic groups; in membrane process, the key is to increase solubility for ionic‐liquid membranes and to control pore size for 2D materials. Challenges and opportunities for simulating emerging materials are also discussed. WIREs Comput Mol Sci 2016, 6:173–197. doi: 10.1002/wcms.1241 This article is categorized under: Structure and Mechanism > Computational Materials Science Electronic Structure Theory > Density Functional Theory Molecular and Statistical Mechanics > Molecular Interactions

Tian, Ziqi↗

DOE OSTI2015

Interdisciplinary research in climate and energy sciences

Due to the complex nature of climate change, interdisciplinary research approaches involving knowledge and skills from a broad range of disciplines have been adopted for studying changes in the climate system as well as strategies for mitigating climate change (i.e., greenhouse gas emissions reductions) and adapting to its impacts on society and natural systems. Harnessing of renewable energy sources to replace fossil fuels is widely regarded as a long-term mitigation strategy that requires the synthesis of knowledge from engineering, technology, and natural and social sciences. In this study, we examine how the adoption of interdisciplinary approaches has evolved over time and in different geographic regions. We conducted a comprehensive literature survey using an evaluation matrix of keywords, in combination with a word cloud analysis, to evaluate the spatiotemporal dynamics of scholarly discourse about interdisciplinary approaches to climate change and renewable energy research and development (R&D). Publications that discuss interdisciplinary approaches to climate change and renewable energy have substantially increased over the last 60 years; it appears, however, that the nature, timing, and focus of these publications vary across countries and through time. Over the most recent three decades, the country-level contribution to interdisciplinary research for climate change has become more evenly distributed, but this was not true for renewable energy research, which remained dominated by the United Sates and a few other major economies. The research topics have also evolved: Water resource management was emphasized from 1990s to 2000s, policy and adaptation were emphasized from the 2000s to 2010 – 2013, while vulnerability became prominent during the most recent years (2010 – 2013). Lastly, our analysis indicates that the rate of growth of interdisciplinary research for renewable energy lags behind that for climate change, possibly because knowledge emanating from climate change science has motivated the subsequent upswing in renewable energy R&D.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Estimating the impacts of natural gas power generation growth on solar electricity development: PJM's evolving resource mix and ramping capability

Abstract Expansion of distributed solar photovoltaic (PV) and natural gas‐fired generation capacity in the United States has put a renewed spotlight on methods and tools for power system planning and grid modernization. This article investigates the impact of increasing natural gas‐fired electricity generation assets on installed distributed solar PV systems in the Pennsylvania–New Jersey–Maryland (PJM) Interconnection in the United States over the period 2008–2018. We developed an empirical dynamic panel data model using the system‐generalized method of moments (system‐GMM) estimation approach. The model accounts for the impact of past and current technical, market and policy changes over time, forecasting errors, and business cycles by controlling for PJM jurisdictions‐level effects and year fixed effects. Using an instrumental variable to control for endogeneity, we concluded that natural gas does not crowd out renewables like solar PV in the PJM capacity market; however, we also found considerable heterogeneity. Such heterogeneity was displayed in the relationship between solar PV systems and electricity prices. More interestingly, we found no evidence suggesting any relationship between distributed solar PV development and nuclear, coal, hydro, or electricity consumption. In addition, considering policy effects of state renewable portfolio standards, net energy metering, differences in the PJM market structure, and other demand and cost‐related factors proved important in assessing their impacts on solar PV generation capacity, including energy storage as a non‐wire alternative policy technique. This article is categorized under: Photovoltaics > Economics and Policy Fossil Fuels > Climate and Environment Energy Systems Economics > Economics and Policy

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2019

Recent In Situ/Operando Characterization of Lithium-Sulfur Batteries

To address the ever-increasing energy demand due to the increase in the population and at the same time depleting fossil fuel reserves, new energy storage systems, such as batteries, are being developed. Among various battery systems, Li-S batteries have comparatively high theoretical energy density and lower cost, making Li-S batteries very promising for next-generation secondary batteries. However, the current energy density and capacity decay with cycling of Li-S batteries do not fulfill the industrialization needs. To overcome the drawbacks of Li-S batteries and improve its performance, better mechanism understanding is necessary. A great deal of ex situ characterization research has been conducted making a lot of progress in the understanding of the working mechanism. Considering the complexity of the intermediate lithium polysulfides and the inherent multi-electron reaction pathways, advanced in situ/operando techniques are highly required. In this chapter, recent progress of a few typical in situ/operando characterization techniques used in Li-S battery studies is reviewed. These techniques provide more in-depth understanding of Li-S batteries in different aspects and could be enlightening for other energy storage systems too.

Yang, Yan↗

DOE OSTI2023

Energy Transition: Challenges and Opportunities for the Oil & Gas Industry

The energy sector has been experiencing a massive but gradual shift in recent years toward renewable and low-carbon energy sources. The future of fossil fuels lies in the ability of the industry to adapt to the market, environment, and social trends within the energy transition framework. In this chapter, we review the challenges that the oil and gas industry will be facing in the coming years. We then explore opportunities and growth areas that this transition provides to the industry. This chapter focuses on three areas of digitization and modernization, developing innovative low-carbon fuels, and harnessing underground and offshore facilities and expertise.

blockchain technology↗

DOE OSTI2023

Modeling Farmers’ Adoption Potential to New Bioenergy Crops: An Agent-Based Approach

The use of fossil fuels is the primary source of greenhouse gas emissions but there are alternatives to these especially in the form of biofuels, fuels derived from bioenergy crops. This paper aims to determine farmers’ potential adoption rates of newly introduced bioenergy crops with a specific example of carinata in the state of Georgia. The determination is done using an agent-based modeling technique with two principal assumptions—farmers are profit maximizer and they are influenced by neighboring farmers. Two diffusion parameters (traditional and expansion) are followed along with two willingness (high and low) scenarios to switch at varying production economics to carinata and other prominent traditional field crops (cotton, peanuts, corn) in the study region. We find that a contract prices around $9, $8 and $7 can be a viable option for encouraging farmers to adopt carinata in low, average, and high profit conditions, respectively. Expansion diffusion (that diffuses all over the geographical area), rather than centered to the few places like traditional diffusion at the early stage of adoption in conjunction with higher willingness conditions influences higher adoption rates in the short-term. As such, the model can be used to understand the behavioral economics of carinata in Georgia and beyond, as well as offering a potential tool to study similar bioenergy crops.

Ullah, Kazi↗

DOE OSTI2025

Climate models project increasing precipitation in the US Southwest in 2024–2100

We analyzed the measured precipitation in the southwestern US and found that, from 1900 to 2024, precipitation decreased at an average rate of − 1.2 cm per year per 100 years. The most significant precipitation decreases occurred in the three-month period from February to April. At the same time, precipitation during the southwestern monsoon season (July, August, and September) remained relatively stable. The ensemble mean of all CMIP6 (Coupled Model Intercomparison Project phase 6) climate models, along with the regression model incorporating anthropogenic aerosol (AER) and Pacific Decadal Oscillation (PDO) as predictors, projects precipitation to increase from 2024 to 2100. This projected precipitation increase relies on the anticipated decrease in emissions of anthropogenic aerosols, which is associated with the transition from fossil fuel burning to renewable and nuclear energy sources.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2019

Molecular dynamics of combustion reactions in supercritical carbon dioxide. Part 4: boxed MD study of formyl radical dissociation and recombination

Fossil fuel oxy-combustion is an emergent technology where habitual nitrogen diluent is replaced by high pressure (supercritical) carbon dioxide. The supercritical state of CO2 increases the efficiency of the energy conversion and the absence of nitrogen from the reaction mixture reduces pollution by NOx. However, the effects of a supercritical environment on elementary reactions kinetics are not well understood at present. We used boxed molecular dynamics simulations at the QM/MM theory level to predict the kinetics of dissociation/recombination reaction HCO• + [M] ↔ H• + CO + [M], an important elementary step in many combustion processes. A wide range of temperatures (400–1600 K) and pressures (0.3–1000 atm) were studied. Potentials of mean force were plotted and used to predict activation free energies and rate constants. Based on the data obtained, extended Arrhenius equation parameters were fitted and tabulated. The apparent activation energy for the recombination reaction becomes negative above 30 atm. As the temperature increased, the pressure effect on the rate constant decreased. While at 400 K the pressure increase from 0.3 atm to 300 atm accelerated the dissociation reaction by a factor of 250, at 1600 K the same pressure increase accelerated this reaction by a factor of 100.

Biochemistry & Molecular Biology↗

DOE OSTI2018

Geochemical and isotopic evidence on the recharge and circulation of geothermal water in the Tangshan Geothermal System near Nanjing, China: implications for sustainable development

Geothermal resources are practical and competitive clean-energy alternatives to fossil fuels, and study on the recharge sources of geothermal water supports its sustainable exploitation. In order to provide evidence on the recharge source of water and circulation dynamics of the Tangshan Geothermal System (TGS) near Nanjing (China), a comprehensive investigation was carried out using multiple chemical and isotopic tracers (δ{sup 2}H, δ{sup 18}O, δ{sup 34}S, {sup 87}Sr/{sup 86}Sr, δ{sup 13}C, {sup 14}C and {sup 3}H). The results confirm that a local (rather than regional) recharge source feeds the system from the exposed Cambrian and Ordovician carbonate rocks area on the upper part of Tangshan Mountain. The reservoir temperature up to 87 °C, obtained using empirical as well as theoretical chemical geothermometers, requires a groundwater circulation depth of around 2.5 km. The temperature of the geothermal water is lowered during upwelling as a consequence of mixing with shallow cold water up to a 63% dilution. The corrected {sup 14}C age shows that the geothermal water travels at a very slow pace (millennial scale) and has a low circulation rate, allowing sufficient time for the water to become heated in the system. This study has provided key information on the genesis of TGS and the results are instructive to the effective management of the geothermal resources. Further confirmation and even prediction associated with the sustainability of the system could be achieved through continuous monitoring and modeling of the responses of the karstic geothermal reservoir to hot-water mining.

58 GEOSCIENCES↗

DOE OSTI2021

Integrated energy-water-land nexus planning in the Colorado River Basin (Argentina)

Integrated energy-water-land (EWL) planning promotes synergies and avoids conflicts in ways that sector-specific planning approaches cannot. Many important decisions that influence emerging EWL nexus issues are implemented at regional (e.g., large river basin, electricity grid) and sub-regional (e.g., small river basin, irrigation district) scales. However, actual implementation of integrated planning at these scales has been limited. Simply collecting and visualizing data and interconnections across multiple sectors and sub-regions in a single modeling platform is a unique endeavor in many regions. This study introduces and applies a novel approach to linking together multiple sub-regions in a single platform to characterize and visualize EWL resource use, EWL system linkages within and among sub-regions, and the EWL nexus implications of future policies and investments. This integrated planning methodology is applied in the water-stressed Colorado River Basin in Argentina, which is facing increasing demands for agricultural and fossil fuel commodities. Guided by stakeholders, this study seeks to inform basin planning activities by characterizing and visualizing (1) the basin’s current state of EWL resources, (2) the linkages between sectors within and among basin sub-regions, and (3) the EWL nexus implications of planned future agricultural development activities. Results show that water scarcity, driven in part by human demands that have historically reached 60% of total surface water supply, poses a substantial constraint to economic development in the basin. The Colorado basin has the potential to serve as a testbed for crafting novel and generalizable sub-regional EWL planning approaches capable of informing the EWL planning dialogue globally.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Combining biotechnology with sustainability: feasibility of bioenergy sorghum in generating high-value bioproducts

Biofuels generated through fermentation of plant-derived lignocellulosic biomass are currently not competitive with fossil fuels. Here, a framework is described for the engineering of valuable coproducts to improve the economic feasibility of biofuel production. To accomplish this goal, the desirable traits of the bioenergy crop Sorghum bicolor are harnessed via modern engineering approaches. A robust analysis is provided to highlight the scientific basis, costs, regulatory challenges, and lucrative nature of coproduct development. Sustainable biofuel production could also have far-reaching societal impacts, especially in the context of our rapidly changing global climate. This perspective suggests that the path to profitable biofuel production is attainable and encourages consideration of similar approaches by the biotechnology industry.

09 BIOMASS FUELS↗

DOE OSTI2014

Spatially resolved estimation of ozone-related mortality in the United States under two representative concentration pathways (RCPs) and their uncertainty

We report that the spatial pattern of the uncertainty in air pollution-related health impacts due to climate change has rarely been studied due to the lack of high-resolution model simulations, especially under the Representative Concentration Pathways (RCPs), the latest greenhouse gas emission pathways. We estimated future tropospheric ozone (O 3 ) and related excess mortality and evaluated the associated uncertainties in the continental United States under RCPs. Based on dynamically downscaled climate model simulations, we calculated changes in O 3 level at 12 km resolution between the future (2057 and 2059) and base years (2001–2004) under a low-to-medium emission scenario (RCP4.5) and a fossil fuel intensive emission scenario (RCP8.5). We then estimated the excess mortality attributable to changes in O 3 . Finally, we analyzed the sensitivity of the excess mortality estimates to the input variables and the uncertainty in the excess mortality estimation using Monte Carlo simulations. O 3 -related premature deaths in the continental U.S. were estimated to be 1312 deaths/year under RCP8.5 (95 % confidence interval (CI): 427 to 2198) and ₋2118 deaths/year under RCP4.5 (95 % CI: ₋3021 to ₋1216), when allowing for climate change and emissions reduction. The uncertainty of O 3 -related excess mortality estimates was mainly caused by RCP emissions pathways. Finally, excess mortality estimates attributable to the combined effect of climate and emission changes on O 3 as well as the associated uncertainties vary substantially in space and so do the most influential input variables. Spatially resolved data is crucial to develop effective community level mitigation and adaptation policy.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

DOE OSTI2019

The role of methane in future climate strategies: mitigation potentials and climate impacts

This study examines model-specific assumptions and projections of methane (CH 4 ) emissions in deep mitigation scenarios generated by integrated assessment models (IAMs). For this, scenarios of nine models are compared in terms of sectoral and regional CH 4 emission reduction strategies, as well as resulting climate impacts. The models’ projected reduction potentials are compared to sector and technology-specific reduction potentials found in literature. Significant cost-effective and non-climate policy related reductions are projected in the reference case (10–36% compared to a “frozen emission factor” scenario in 2100). Still, compared to 2010, CH 4 emissions are expected to rise steadily by 9–72% (up to 412 to 654 Mt CH 4 /year). Ambitious CO 2 reduction measures could by themselves lead to a reduction of CH 4 emissions due to a reduction of fossil fuels (22–48% compared to the reference case in 2100). However, direct CH 4 mitigation is crucial and more effective in bringing down CH 4 (50–74% compared to the reference case). Given the limited reduction potential, agriculture CH 4 emissions are projected to constitute an increasingly larger share of total anthropogenic CH 4 emissions in mitigation scenarios. Enteric fermentation in ruminants is in that respect by far the largest mitigation bottleneck later in the century with a projected 40–78% of total remaining CH 4 emissions in 2100 in a strong (2 °C) climate policy case.

54 ENVIRONMENTAL SCIENCES↗