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There is an urgent need to develop technologies that use renewable energy to convert waste products such as carbon dioxide into hydrocarbon fuels. Carbon dioxide can be electrochemically reduced to hydrocarbons over copper catalysts, although higher efficiency is required. We have developed oxidized copper catalysts displaying lower overpotentials for carbon dioxide electroreduction and record selectivity towards ethylene (60%) through facile and tunable plasma treatments. Herein we provide insight into the improved performance of these catalysts by combining electrochemical measurements with microscopic and spectroscopic characterization techniques. Operando X-ray absorption spectroscopy and cross-sectional scanning transmission electron microscopy show that copper oxides are surprisingly resistant to reduction and copper(+) species remain on the surface during the reaction. Our results demonstrate that the roughness of oxide-derived copper catalysts plays only a partial role in determining the catalytic performance, while the presence of copper(+) is key for lowering the onset potential and enhancing ethylene selectivity.
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http://dx.doi.org/10.1038/ncomms12123 | DOI Listing |
J Colloid Interface Sci
December 2024
Pingshan Translational Medicine Center, Shenzhen Bay Laboratory, Shenzhen 518118, China. Electronic address:
Copper-based materials are promising for formaldehyde oxidation to produce hydrogen but suffer from degradation caused by soluble copper ions in alkaline electrolytes. In this report, a novel CuPd/CC alloy electrocatalyst is developed to address this issue. The catalyst drives formaldehyde oxidation at 0.
View Article and Find Full Text PDFInorg Chem
December 2024
Guizhou Provincial Key Laboratory of Green Chemical and Clean Energy Technology, School of Chemistry and Chemical Engineering, Guizhou University, Guiyang, Guizhou 550025, China.
The combination of the electrocatalytic glycerol oxidation reaction (GOR) with the cathodic hydrogen evolution reaction serves to reduce the anodic overpotential, thereby facilitating the efficient production of hydrogen. However, the GOR is confined to a narrow potential range due to the competition of the oxygen evolution reaction (OER) at high potential. Therefore, it is necessary to develop a catalyst with a high Faraday efficiency of formate (FE) over a wide potential range.
View Article and Find Full Text PDFChemistry
December 2024
Lanzhou University, College of Chemistry and Chemical Engineering, Lanzhou Tianshui south street 222, 730000, Lanzhou, CHINA.
Dual single-atom catalysts have attracted considerable research interest due to their higher metal atom loading and more flexible active sites compared to single-atom catalysts (SACs). We pioneered the one-step synthesis of sheets copper-cobalt graphitic carbon nitride dual single-atom (S-Cu/Co-g-C3N4) using folding fan-shaped aluminum foil as a template, and used them as catalysts in the epoxidation of styrene respectively. Through XAFS(X-ray Absorption Fine Structure) and other characterizations, it is found that Cu and Co single atoms are stabilized separately on g-C3N4 via coordination with nitrogen (N), hindered the ordered growth of sheets, and formed more pore structures, which not only increased more catalytically active sites, but also effectively prevented the flakes re-aggregate during the catalytic process.
View Article and Find Full Text PDFChemSusChem
December 2024
Huazhong University of Science and Technology, School of Chemistry and Chemical Engineering, Luoyu load, 430074, Wuhan, CHINA.
Electrochemical carbon dioxide reduction reaction (CO2RR) to highly value-added C2+ fuels or chemicals is a promising pathway to address environment issues and energy crisis. In the periodic table, Cu as only the candidate can convert CO2 to C2+ products such as C2H4 and C2H5OH due to the suitable absorption energy to reaction intermediate. Application of Cu is limited for its low activity and poor selectivity.
View Article and Find Full Text PDFChemistry
December 2024
Guangdong Pharmaceutical University, Guangzhou Higher Education Mega Center, 510006, Guangzhou, CHINA.
Among the various studies on CO2 utilization, the sustainable and cost-effective fixation of CO2 into cyclic carbonates remains one of the most intriguing subjects. To this end, a novel type of composite dicationic ionic liquid material, DIL@PDIL, was developed. This composite consists of a dicationic ionic liquid (DIL), DMAP[TMGH]Br, supported on a polymeric dicationic ionic liquid (PDIL), P-DVB/Im[TMGH]Br.
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