Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO 2 /CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm −2...

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Veröffentlicht in:Nature communications 2020-07, Vol.11 (1), p.3685-3685, Article 3685
Hauptverfasser: Li, Jun, Xu, Aoni, Li, Fengwang, Wang, Ziyun, Zou, Chengqin, Gabardo, Christine M., Wang, Yuhang, Ozden, Adnan, Xu, Yi, Nam, Dae-Hyun, Lum, Yanwei, Wicks, Joshua, Chen, Bin, Wang, Zhiqiang, Chen, Jiatang, Wen, Yunzhou, Zhuang, Taotao, Luo, Mingchuan, Du, Xiwen, Sham, Tsun-Kong, Zhang, Bo, Sargent, Edward H., Sinton, David
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Sprache:eng
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Zusammenfassung:Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO 2 /CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm −2 ). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C 2 intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm −2 from CO electroreduction. The activity exceeds that of prior reports by a factor of 2. The electrocatalytic upgrading of CO to higher-value fuels provides a promising route to multi-carbon alcohol products. Here, the authors show that high alcohol selectivity and activity can be achieved by incorporating palladium in copper.
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-020-17499-5