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Acetic acid (AA), an important commodity chemical, is produced via methanol carbonylation, emitting one ton of CO₂ per ton of product. As a sustainable alternative, we report the electrochemical oxidation of bioethanol to selectively produce AA using a novel Pdsingle bondSn alloy catalyst with nanodendritic morphology supported on nickel foam (PdSn@NF). The catalyst was synthesized via electrodeposition, and the presence of ammonium chloride in the deposition bath was found to critically affect the Pd-to-Sn ratio and, consequently, the catalyst performance. The vital role of catalyst structure, surface composition, and morphology on the activity and selectivity of PdSn@NF towards the EOR was revealed by X-ray diffractometry, emission spectroscopy, and electron microscopy. Specifically, the nanodendritic morphology of the PdSn@NF resulted in the formation of highly active undercoordinated sites, while in situ Raman spectroscopy suggested that Sn helps mitigate CO poisoning – likely a result of a lowered d-band center. Due to the strong synergy between the structural and electronic properties of PdSn@NF, ~100 % faradaic efficiency (FE) to AA at 400 mA cm−2 was achieved with lab-grade ethanol (LGE) in an H-type cell. In continuous flow operation, the FE declined due to product accumulation on active sites; however, this was mitigated by employing current pulses to remove surface-bound products. An optimized pulsing protocol restored ~100 % FE of AA for LGE and achieved ~94 % FE with bioethanol at 400 mA cm−2 despite the presence of fermentation impurities. This study underscores the promise of PdSn@NF as a highly selective and industrially relevant electrocatalyst for sustainable AA production.more » « lessFree, publicly-accessible full text available December 1, 2026
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Free, publicly-accessible full text available September 1, 2026
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Carbon reactive capture and conversion offers a sustainable route to valuable chemicals and fuels while aiding GHG reduction. Direct electrochemical conversion of capture solutions like bicarbonate avoids the energy demands...more » « lessFree, publicly-accessible full text available September 2, 2026
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Greenhouse gas emissions present a significant challenge to humanity, and utilizing renewable electricity to convert emitted CO2 into value-added products offers a promising solution; however, traditional CO2 capture and regeneration processes remain energy-intensive, restricting the overall system efficiency and decarbonization efficacy. In this study, an advanced direct reduction of captured CO2 with large current densities for formate electrosynthesis was demonstrated without the need for CO2 regeneration or compression. The bismuth nanosheet (DRM-BiNS) was synthesized by direct reduction of a Bi-based MOF, representing a new class of catalytic materials with a large surface area and interconnected pores, suitable for the direct reduction of captured CO₂. By seamlessly combining experimentation and simulation, insights into the structure-parameter-performance relation were acquired in a flow cell setting, including critical membrane-electrode distance, cell orientation, and pumping flow rate. Important flow-cell components, such as catholyte volume, electrode substrate, membrane choice, and ionomer type, were also carefully examined to enhance the cell performance. In sharp contrast to prior studies limited to current densities below 20 mA/cm² in bicarbonate-based captured CO2 solutions, this work demonstrates a remarkable current density of 300 mA/cm² with an FE to formate comparable to the case with gas-fed CO2 reduction. Moreover, the process sustained an FE above 50% at a high current density of 500 mA/cm². The DRM-BiNS catalyst exhibited outstanding selectivity, activity, and stability, significantly outperforming oxide-derived bismuth nanosheets (OD-BiNS) in captured CO2 reduction. These findings offer critical insights into the development of sustainable and scalable CO2 utilization technologies.more » « lessFree, publicly-accessible full text available July 1, 2026
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Greenhouse gas emissions present a significant challenge to humanity, and utilizing renewable electricity to convert emitted CO2 into value-added products offers a promising solution; however, traditional CO2 capture and regeneration processes remain energy-intensive, restricting the overall system efficiency and decarbonization efficacy. In this study, an advanced direct reduction of captured CO2 with large current densities for formate electrosynthesis was demonstrated without the need for CO2 regeneration or compression. The bismuth nanosheet (DRM-BiNS) was synthesized by direct reduction of a Bi-based MOF, representing a new class of catalytic materials with a large surface area and interconnected pores, suitable for the direct reduction of captured CO₂. By seamlessly combining experimentation and simulation, insights into the structure-parameter-performance relation were acquired in a flow cell setting, including critical membrane-electrode distance, cell orientation, and pumping flow rate. Important flow-cell components, such as catholyte volume, electrode substrate, membrane choice, and ionomer type, were also carefully examined to enhance the cell performance. In sharp contrast to prior studies limited to current densities below 20 mA/cm² in bicarbonate-based captured CO2 solutions, this work demonstrates a remarkable current density of 300 mA/cm² with an FE to formate comparable to the case with gas-fed CO2 reduction. Moreover, the process sustained an FE above 50% at a high current density of 500 mA/cm². The DRM-BiNS catalyst exhibited outstanding selectivity, activity, and stability, significantly outperforming oxide-derived bismuth nanosheets (OD-BiNS) in captured CO2 reduction. These findings offer critical insights into the development of sustainable and scalable CO2 utilization technologies.more » « lessFree, publicly-accessible full text available June 22, 2026
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This study examines farmers' acceptance of green ammonia produced by upcycling waste nitrogen using renewable energy. A mail survey, targeting a random sample of crop growers in Iowa, USA, found moderately high acceptance: about 50% support green ammonia as a fertilizer and 32% support green ammonia as a fuel. Support for green hydrogen is only 17% (24% opposing), demonstrating a preference of 2nd-generation over 1st-generation technologies. Ordinal logistic regression reveals social and psychological factors affecting attitude, including income, ideology, perceived benefit, ammonia usage, trust in science and technology, personal belief in reducing waste nitrogen, and social norm.more » « less
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There is a growing need to develop novel technologies that reduce reactive nitrogen concentrations in wastewater streams and decrease our reliance on fossil fuel energy required to produce N-based chemicals and fertilizers. This study conducts a techno-economic analysis (TEA) and a life cycle assessment (LCA) of the electrochemical conversion of nitrate ions (NO3–) present in wastewater to hydroxylamine (NH2OH), a valuable chemical intermediate. We employ experimental data and modeling assumptions to determine NH2OH production costs and life cycle emissions for a small-scale facility (producing 1500 kg-NH2OH/day) and a large-scale facility (producing 50,000 kg-NH2OH/day) integrated into a wastewater treatment plant. The present NH2OH production costs for the small- and large-scale facilities are estimated at $6.14/kg-NH2OH and $5.37/kg-NH2OH, respectively. The parameters dominating the electrochemical reactor cost are electrolyte, separations, and fixed cost, with their values as $1.48, $0.96, and $0.53/kg. Future cost reduction projections indicate that the present NH2OH production costs for the small- and large-scale facilities can be reduced to $2.79/kg-NH2OH and $2.06/kg-NH2OH (NH2OH market price = $1.72/kg), respectively, with improvements in the sensitivity analysis parameters. LCA results indicate that the proposed electrochemical pathway to produce NH2OH has lower life cycle impacts than the conventional pathway.more » « less
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