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Plasmon-Induced CO 2 Conversion on Al@Cu 2 O: A DFT Study
In plasmonic catalysis, localized surface plasmon was leveraged to drive chemical reactions. This approach is promising for catalyzing many challenging reactions at relatively low temperatures and pressures. We apply density functional calculations to provide the insight for the mechanism of plasmon-induced direct CO 2 dissociation on an Al@Cu 2 O core-shell structure, which was observed in a previous experimental study. We show that the interaction of Cu 2 O with CO 2 results in the accessible antibonding states of the adsorbed CO 2 in the range of visible light. Though the intrinsic activation barrier for direct CO 2 dissociation is as high as 3.6 eV, we find that an effective reaction barrier of CO 2 dissociation under photon excitation could be reduced by 2 eV. We also show that the charge transfer is more pronounced in the final state of the dissociation due to the strong hybridization of the dissociated species with Cu 2 O. These results thus provide an explanation for the visible-light-induced direct CO 2 dissociation at relatively low temperature and under ambient pressure. This finding also shows the promising impact of plasmonic catalysis in mitigating carbon emission.
Self-Organization and Nitrogen Incorporation in Diamond-Like Carbon Microstructures Synthesized by Nonthermal Plasma
Nonthermal plasma activation of light alkanes is an encouraging decarbonization strategy to produce chemicals or fuels from abundant and/or flared carbon sources. However, prolific carbon growth on both the catalyst and electrode has limited its practicality, requiring additional knowledge of the carbon structure and growth mechanism before breakthroughs are realized. Furthermore, visual evidence is provided for nonuniform diamond-like carbon (DLC) microstructures that materialize in a coaxial dielectric barrier discharge (DBD) reactor flowing ethane and He at 278 K. Through a connection to known behaviors of DBD microdischarge patterns, the microstructure spacing was controlled by altering the applied voltage (ΔV) of the plasma or the burning voltage (U b ). Additionally, carbon valorization through nitrogen incorporation from N 2 was explored as an orthogonal solution to carbon mitigation, with N/C values >0.25 achieved and both sp 2 and sp 3 C–N bonding observed in the microstructures.
Mechanistic insights into CO 2 capture and electrochemical conversion in nonaqueous Na–CO 2 batteries
Developing efficient energy storage systems that capture and convert CO 2 is critical for mitigating carbon emissions. Here, we report a Na–CO 2 battery with ruthenium dioxide (RuO 2 ) cathode catalysts and propane-1,3-diamine (PDA) as an electrolyte additive to enhance CO 2 capture and conversion efficiency. The integration of CO 2 adsorption and electrochemical reduction facilitates activation of the inert CO 2 molecule and circumvents gas–solid–liquid ternary-phase reactions at the interface. We employed density functional theory (DFT) calculations to systematically unravel the reaction mechanisms and energetics governing CO 2 reduction, both with and without PDA. Our results reveal an energetically favorable pathway toward the formation of Na 2 CO 3 and C as final discharge products, rather than sodium oxalate (Na 2 C 2 O 4 ). The CO 2 –amine adduct facilitates charge transfer from PDA to CO 2 , which results in activation of CO 2 . The kinetics of CO 2 conversion and regeneration of PDA were found to be significantly enhanced on the RuO 2 surface compared to the bulk electrolyte. More importantly, pre-activation of CO 2 via the amine–CO 2 adduct lowers the total overpotential to 2.44 V, compared to 3.13 V without PDA. This study provides fundamental insights into CO 2 electroreduction in Na–CO 2 batteries and underscores the promise of electrolyte engineering for sustainable CO 2 utilization and high-performance energy storage.
Evaluating the stability and activity of dilute Cu-based alloys for electrochemical CO 2 reduction
Cu-based catalysts currently offer the most promising route to actively and selectively produce value-added chemicals via electrochemical reduction of CO 2 (eCO 2 R); yet further improvements are required for their wide-scale deployment in carbon mitigation efforts. Here, we systematically investigate a family of dilute Cu-based alloys to explore their viability as active and selective catalysts for eCO 2 R through a combined theoretical–experimental approach. Using a quantum–classical modeling approach that accounts for dynamic solvation effects, we assess the stability and activity of model single-atom catalysts under eCO 2 R conditions. Our calculations identify that the presence of eCO2R intermediates, such as CO*, H*, and OH*, may dynamically influence the local catalyst surface composition. Additionally, we identify through binding energy descriptors of the CO*, CHO*, and OCCO* dimer intermediates that certain elements, such as group 13 elements (B, Al, and Ga), enhance the selectivity of C 2+ species relative to pure Cu by facilitating CO dimerization. The theoretical work is corroborated by preliminary testing of eCO 2 R activity and selectivity of candidate dilute Cu-based alloy catalyst films prepared by electron beam evaporation in a zero-gap gas diffusion electrode-based reactor. Of all studied alloys, dilute CuAl was found to be the most active and selective toward C 2+ products like ethylene, consistent with the theoretical predictions. Finally, we attribute the improved performance of dilute CuAl alloys to more favorable dimerization reaction energetics of bound CO species relative to that on pure Cu. In a broader context, the results presented here demonstrate the power of our simulation framework in terms of rational catalyst design.
Growth–Mortality Coordination Differs Among Xerophytic Versus Mesophytic Tree Species During Severe Drought
ABSTRACT Forest composition is changing, yet the consequences for terrestrial carbon cycling are unclear. In the eastern United States, water‐demanding “mesophytic” tree species are replacing “xerophytic” oaks (Quercusspp.) and hickories (Caryaspp.), raising concerns that forest productivity will become increasingly sensitive to more frequent and severe drought conditions predicted for the region. However, we have a limited understanding of the extent to which the mortality risk of xerophytes versus mesophytes is coordinated with their growth sensitivity during drought. Here, we evaluated growth and mortality dynamics for 20 abundant eastern United States tree species following a severe drought in the summer of 2012. We synthesized data from ~4500 forest inventory plots and used an approach that quantified relative drought responses between co‐located trees to minimize impacts from environmental heterogeneity. We found that mesophytes were just as likely to perish as co‐occurring xerophytes but were more sensitive to drought in terms of diminished growth. These findings suggest that xerophytic decline is likely to lead to reduced carbon uptake during drought and that management efforts to conserve oak‐hickory stands will be decisive to sustain the carbon mitigation potential of these forests. However, we also found that growth‐mortality relationships differed between functional groups. Among xerophytes, growth and survival during drought were decoupled. Among mesophytes, there was a high degree of coordination, where species that experienced greater mortality also experienced greater growth reductions. Therefore, mesophytes with high growth sensitivity to water deficits are likely to be the most vulnerable to drought‐driven die‐off events moving forward.
Heat Transfer, Refrigeration and Heat Pumps
The Special Issue entitled “Heat Transfer, Refrigeration and heat Pumps” accepted papers covering a wide range of topics related to heat pumps, thermal energy storage, and low-Global Warming Potential (GWP) alternative refrigerants. Heat pumps play a vital role in providing space conditioning and water heating while utilizing the energy of the environment. Since heat pumps use renewable thermal energy from the environs to provide the desired utility, they contribute to the portfolio of technologies that mitigate carbon footprint. The heat pump may be considered a truly renewable technology if the electricity it uses comes entirely from a renewable source. More accurately, a heat pump is a “low carbon technology”. These perspectives make heat pumps an indispensable option for the future in order to reduce the nocuous human impact on the environment. More efficient heat pumping technologies are being developed for the residential, commercial, and industrial sectors of the economy. Another R&D thrust is heat pumps for cold climates. Hardware components, use of low-GWP refrigerants, and identification of systemic inefficiencies are active research areas. This article is a synopsis of the papers submitted to the Special Issue.
Novel textured surfaces for superior corrosion mitigation in molten carbonate salts for concentrating solar power
Corrosion of metals in contact with molten salts used for thermal energy storage and heat transport at high temperatures is a serious impediment to the development of next-generation concentrating solar thermal systems. Toward addressing this limitation, novel multiscale fractal-textured Ni coatings on a variety of substrate alloys are presented in this study for exceptional corrosion mitigation in molten carbonate salts at a high temperature. Strongly adherent, durable, single-layer, and double-layer multiscale fractal coatings were fabricated using the electrodeposition method. Corrosion performance of the coatings on SS310, SS316, SS347, and In800H was studied in molten carbonate salt (32% Li 2 CO 3 +33% Na 2 CO 3 +35% K 2 CO 3 ) at 750 °C. Single-layer coatings are stable up to 300 h immersion, whereas double-layer coatings are stable beyond 750 h. The corrosion rate of double-layer Ni coatings on ferrous alloys was reduced by as much as 60% from that of uncoated surfaces and was about 18% below that of higher cost, high Ni content Ha230. The study represents the first-ever report of corrosion characteristics of alloys in carbonate salts at 750 °C and the first demonstration of a means of dramatically reducing corrosion in carbonate salts at a high temperature. The article is significant in that it provides a viable approach for low-cost structural alloys to be corrosion-resistant to molten carbonate heat transfer fluids and storage media in high-temperature concentrating solar thermal applications. Furthermore, the corrosion-resistant coatings provide opportunities for the use of low-cost, ferritic alloys instead of the expensive nickel-based alloys in practice.
Study of alkaline carbonate cooling to mitigate Ex-Vessel molten corium accidents
To mitigate adverse effects from molten corium following a reactor pressure vessel failure (RPVF), some new reactor designs employ a core catcher and a sacrificial material (SM), such as ceramic or concrete, to stabilize the molten corium and avoid containment breach. Existing reactors cannot easily be modified to include these SMs but could be modified to allow injectable cooling materials. Current reactor designs are limited to using water to stabilize the corium, but this can create other issues such as reaction of water with the concrete forming hydrogen gas. Here the novel SM proposed is a granular carbonate mineral that can be used in existing light water reactor plants. The granular carbonate will decompose when exposed to heat, inducing an endothermic reaction to quickly solidify the corium in place and producing a mineral oxide and carbon dioxide. Corium spreading is a complex process strongly influenced by coupled chemical reactions, including decay heat from the corium, phase change, and reactions between the concrete containment and available water. A recently completed Sandia National Laboratories laboratory directed research and development (LDRD) project focused on two research areas: experiments to demonstrate the feasibility of the novel SM concept, and modeling activities to determine the potential applications of the concept to actual nuclear plants. Small-scale experiments using lead oxide (PbO) as a surrogate for molten corium demonstrate that the reaction of the SM with molten PbO results in a fast solidification of the melt due to the endothermic carbonate decomposition reaction and the formation of open pore structures in the solidified PbO from CO 2 released during the decomposition. A simplified carbonate decomposition model was developed to predict thermal decomposition of carbonate mineral in contact with corium. This model was incorporated into MELCOR, a severe accident nuclear reactor code. A full-plant MELCOR simulation suggests that by the introduction of SM to the reactor cavity prior to RPVF ex-vessel accident progression, e.g., core-concrete interaction and core spreading on the containment floor, could be delayed by at least 15 h; this may be enough for additional accident management to be implemented to alleviate the situation.
Mitigating the soil carbon deficit of annual agriculture with perennial bioenergy crops in the U.S. Midwest
Maize ( Zea mays L.) is the dominant bioenergy feedstock in the US Midwest but its cultivation since the early 1800s has incurred substantial losses in soil organic carbon (SOC). We quantified differences in SOC stocks under perennial bioenergy crops of Panicum virgatum L. (switchgrass) and Miscanthus x giganteus Greef et Deuter (miscanthus) planted on former maize and soybean fields relative to maize-based annual cropping and native prairie. Comparisons were made at seven locations across Illinois, USA, spanning a range of climate and soil types. Across sites, SOC stocks to 1-m depth on an equivalent soil mass basis were 146 Mg C ha −1 under prairie, 107 Mg C ha −1 under miscanthus, 97.9 Mg C ha −1 under switchgrass, and 87.7 Mg C ha −1 under maize. Higher SOC demonstrates the potential of perennial bioenergy crops to rebuild the SOC deficit accrued under nearly two centuries of maize-based annual cropping. SOC stock increased in the first 5 years under mature bioenergy crops at four out of seven sites. Carbon isotope (δ 13 C) analyses of surface depths confirmed short-term increases in SOC to be derived from miscanthus and switchgrass. Stocks of SOC could be increased over time under miscanthus or switchgrass cultivation even with annual harvesting, though our measured rates of SOC accumulation were lower than previous estimates for Illinois and varied by site.
Self-re-adhering alkali-activated cement composite and its ability to mitigate corrosion of carbon steel in 300 °C hydrothermal environment
Cement-steel interface is a weak point of cement sheath integrity under the environments of high-temperature geothermal wells. This paper presents carbon steel (CS) adherence behaviors of 300 °C-autoclaved alkali-activated Calcium-Aluminate-Cement (CAC)/fly ash F (FAF) (Thermal Shock Resistant Cement, TSRC), granulated blast furnace slag (GBFS)/SiO 2 , and Ordinary Portland Cement (OPC)/SiO 2 blends. The composites’ ability to preserve the bond under the conditions of thermal shock (TS) and strong acid attack (pH 0.6 H 2 SO 4 /brine at 90 °C) as well as their ability to recover the damaged bond and provide steel corrosion protection after additional short-time 5-day curing at 300 °C were evaluated. GBFS/SiO 2 sheath underwent catastrophic failure in the first TS cycle; OPC/SiO 2 lost 78 % and TSRC 51 % of the bond strength in 6 cycles. Only TSRC-CS bond survived 30 days of strong acid exposure; OPC/SiO 2 bond failed after 18 days and GBFS/SiO 2 after 20 days. Addition of micro-glass fibers (MGF) to TSRC further improved its bond strength and CS corrosion protection. Samples of TSRC-CS cured for 30 days at 300 °C before the bond damage recovered 49 % of the damaged bond strength after additional short-time curing. The CS protected by the re-adhered TSRC showed low corrosion rate of 0.13 mm/year (TSRC-MGF), 0.2 mm/year (TSRC) vs. 0.64 mm/year for OPC/SiO 2 protected CS.
MELCOR Study of Alkaline Carbonate Cooling to Mitigate Ex-Vessel Molten Corium Accidents.
Abstract not provided.
Potential of soil carbon sequestration to mitigate climate change
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Soil microbiome interventions for carbon sequestration and climate mitigation
Mitigating climate change in soil ecosystems involves complex plant and microbial processes regulating carbon pools and flows. Here, we advocate for the use of soil microbiome interventions to help increase soil carbon stocks and curb greenhouse gas emissions from managed soils. Direct interventions include the introduction of microbial strains, consortia, phage, and soil transplants, whereas indirect interventions include managing soil conditions or additives to modulate community composition or its activities. Approaches to increase soil carbon stocks using microbially catalyzed processes include increasing carbon inputs from plants, promoting soil organic matter (SOM) formation, and reducing SOM turnover and production of diverse greenhouse gases. Marginal or degraded soils may provide the greatest opportunities for enhancing global soil carbon stocks. Among the many knowledge gaps in this field, crucial gaps include the processes influencing the transformation of plant-derived soil carbon inputs into SOM and the identity of the microbes and microbial activities impacting this transformation. As a critical step forward, we encourage broadening the current widespread screening of potentially beneficial soil microorganisms to encompass functions relevant to stimulating soil carbon stocks. Moreover, in developing these interventions, we must consider the potential ecological ramifications and uncertainties, such as incurred by the widespread introduction of homogenous inoculants and consortia, and the need for site-specificity given the extreme variation among soil habitats. Incentivization and implementation at large spatial scales could effectively harness increases in soil carbon stocks, helping to mitigate the impacts of climate change.
The Plant a Trillion Trees Campaign to Reduce Global Warming – Fleshing Out the Concept
The campaign to plant a trillion trees provided an easily understood approach to reduce the threat of global warming. However, focusing on trees does not consider that a maturing forest releases carbon (C) from dying trees offsetting C intake from growth of other trees, and results in only a one-time carbon storage benefit. Under sustainable management that harvests before forest growth slows down, forest C is transferred to wood products that substitute for fossil fuel (FF)- intensive products, reducing the carbon dioxide (CO 2 ) emissions with every harvest. Sustainably managed forests maintain growth by replanting (or regenerating), sustaining the C stored in products, as well as avoiding FF-intensive product emissions with every harvest. This paper addresses the question: Could planting more trees significantly reduce atmospheric CO 2 ; and if so, how? Survey data from many wood-producing mills show life cycle inventory (LCI) data on C that has been tracked through every stage of processing for many different wood products specific to each United States (USA) supply region, as well as C displacement measurements when substituting wood for FFintensive products. Results show that more and better-managed forest lands and more efficient product uses provide significant opportunities to reduce CO 2 emissions, especially in highly productive forest regions.
The role of oxygen in stimulating methane production in wetlands
Methane (CH 4 ), a potent greenhouse gas, is the second most important greenhouse gas contributor to climate change after carbon dioxide (CO 2 ). The biological emissions of CH 4 from wetlands are a major uncertainty in CH 4 budgets. Microbial methanogenesis by Archaea is an anaerobic process accounting for most biological CH 4 production in nature, yet recent observations indicate that large emissions can originate from oxygenated or frequently oxygenated wetland soil layers. To determine how oxygen (O 2 ) can stimulate CH 4 emissions, we used incubations of Sphagnum peat to demonstrate that the temporary exposure of peat to O 2 can increase CH 4 yields up to 2000-fold during subsequent anoxic conditions relative to peat without O 2 exposure. Geochemical (including ion cyclotron resonance mass spectrometry, X-ray absorbance spectroscopy) and microbiome (16S rDNA amplicons, metagenomics) analyses of peat showed that higher CH 4 yields of redox-oscillated peat were due to functional shifts in the peat microbiome arising during redox oscillation that enhanced peat carbon (C) degradation. Novosphingobium species with O 2 -dependent aromatic oxygenase genes increased greatly in relative abundance during the oxygenation period in redox-oscillated peat compared to anoxic controls. Acidobacteria species were particularly important for anaerobic processing of peat C, including in the production of methanogenic substrates H 2 and CO 2 . Higher CO 2 production during the anoxic phase of redox-oscillated peat stimulated hydrogenotrophic CH 4 production by Methanobacterium species. The persistence of reduced iron (Fe(II)) during prolonged oxygenation in redox-oscillated peat may further enhance C degradation through abiotic mechanisms (e.g., Fenton reactions). The results indicate that specific functional shifts in the peat microbiome underlie O 2 enhancement of CH 4 production in acidic, Sphagnum-rich wetland soils. They also imply that understanding microbial dynamics spanning temporal and spatial redox transitions in peatlands is critical for constraining CH 4 budgets; predicting feedbacks between climate change, hydrologic variability, and wetland CH 4 emissions; and guiding wetland C management strategies.
Revisiting “Additional Carbon”: Tracking Atmosphere–Ecosystem Carbon Exchange to Establish Mitigation and Negative Emissions From Bio-Based Systems
Climate stabilization plans rely heavily on advanced bioenergy and bioproducts for substitution of fossil-based energy sources and materials, and increasingly, for negative emissions via the direct sequestration of biogenic carbon. Yet, there remain persistent, largely unresolved critiques of bioenergy assessment methodology, particularly in the areas of land use and biogenic carbon accounting. The concept of “additional carbon” calls for evaluating the climate performance of bio-based systems by whether feedstock production creates measurable new local agro-ecosystem uptake of carbon from the atmosphere. This concept is challenging to operationalize for first-generation biofuels, and has largely been advanced as a negative critique. However, carbon additionality is more straightforward to establish—and less critical to overall system mitigation performance—in advanced bioenergy systems. In this Perspective, I review the additional carbon critique, and why it is analytically challenging to address in first-generation biofuel systems based on conventional food crops with large existing markets. Next, I make a case that carbon additionality (1) is more readily achievable with cellulosic feedstocks, (2) is more directly observable for dedicated biomass crops, and (3) is not a strict requirement for achieving net mitigation in carbon-negative bio-based systems. I end by discussing how centering atmosphere–ecosystem carbon exchanges in bio-based system assessment could create new opportunities for enterprise-scale performance monitoring and verification, augmenting and diversifying the current reliance on model-based life-cycle assessment approaches.
A bioenergy-focused versus a reforestation-focused mitigation pathway yields disparate carbon storage and climate responses
Limiting global warming to 2 °C requires urgent action on land-based mitigation. This study evaluates the biogeochemical and biogeophysical implications of two alternative land-based mitigation scenarios that aim to achieve the same radiative forcing. One scenario is primarily driven by bioenergy expansion (SSP226Lu-BIOCROP), while the other involves re/afforestation (SSP126Lu-REFOREST). We find that overall, SSP126Lu-REFOREST is a more efficient strategy for removing CO2 from the atmosphere by 2100, resulting in a net carbon sink of 242 ~ 483 PgC with smaller uncertainties compared to SSP226Lu-BIOCROP, which exhibits a wider range of -78 ~ 621 PgC. However, SSP126Lu-REFOREST leads to a relatively warmer planetary climate than SSP226Lu-BIOCROP, and this relative warming can be intensified in certain re/afforested regions where local climates are not favorable for tree growth. Despite the cooling effect on a global scale, SSP226Lu-BIOCROP reshuffles regional warming hotspots, amplifying summer temperatures in vulnerable tropical regions such as Central Africa and Southeast Asia. Our findings highlight the need for strategic land use planning to identify suitable regions for re/afforestation and bioenergy expansion, thereby improving the likelihood of achieving the intended climate mitigation outcomes.