气候变化领域集成服务门户(CCPortal): Selective CO2 reduction to C3 and C4 oxyhydrocarbons on nickel phosphides at overpotentials as low as 10 mV

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DOI	10.1039/c8ee00936h
	Selective CO2 reduction to C3 and C4 oxyhydrocarbons on nickel phosphides at overpotentials as low as 10 mV
	Calvinho K.U.D.; Laursen A.B.; Yap K.M.K.; Goetjen T.A.; Hwang S.; Murali N.; Mejia-Sosa B.; Lubarski A.; Teeluck K.M.; Hall E.S.; Garfunkel E.; Greenblatt M.; Dismukes G.C.
发表日期	2018
ISSN	17545692
起始页码	2550
结束页码	2559
卷号	11 期号:9
英文摘要	We introduce five nickel phosphide compounds as electro-catalysts for the reduction of carbon dioxide in aqueous solution, that achieve unprecedented selectivity to C3 and C4 products (the first such report). Three products: formic acid (C1), methylglyoxal (C3), and 2,3-furandiol (C4), are observed at potentials as low as +50 mV vs. RHE, and at the highest half-reaction energy efficiencies reported to date for any >C1 product (99%). The maximum selectivity for 2,3-furandiol is 71% (faradaic efficiency) at 0.00 V vs. RHE on Ni2P, which is equivalent to an overpotential of 10 mV, with the balance forming methylglyoxal, the proposed reaction intermediate. P content in the series correlates closely with both the total C products and product selectivity, establishing definitive structure-function relationships. We propose a reaction mechanism for the formation of multi-carbon products, involving hydride transfer as the potential-determining step to oxygen-bound intermediates. This unlocks a new and more energy-efficient reduction route that has only been previously observed in nickel-based enzymes. This performance contrasts with simple metallic catalysts that have poor selectivity between multi-carbon products, and which require high overpotentials (>700 mV) to achieve comparable reaction rates. © 2018 The Royal Society of Chemistry.
英文关键词	Carbon dioxide; Catalyst selectivity; Energy efficiency; Phosphorus compounds; Reaction intermediates; Reaction rates; Solutions; Faradaic efficiencies; Hydride transfers; Maximum selectivity; Metallic catalysts; Nickel phosphide; Product selectivities; Reaction mechanism; Structure-function relationship; Nickel compounds; aqueous solution; carbon dioxide; catalysis; catalyst; chemical reaction; efficiency measurement; enzyme; enzyme activity; formic acid; nickel; organic compound; performance assessment; reduction
语种	英语
来源期刊	Energy & Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/190126
作者单位	Department of Chemistry and Chemical Biology, Rutgers, State University of New Jersey, 610 Taylor Road, Piscataway, NJ 08854, United States; Waksman Institute of Microbiology, Rutgers, State University of New Jersey, 190 Frelinghuysen Road, Piscataway, NJ 08854, United States
推荐引用方式 GB/T 7714	Calvinho K.U.D.,Laursen A.B.,Yap K.M.K.,et al. Selective CO2 reduction to C3 and C4 oxyhydrocarbons on nickel phosphides at overpotentials as low as 10 mV[J],2018,11(9).
APA	Calvinho K.U.D..,Laursen A.B..,Yap K.M.K..,Goetjen T.A..,Hwang S..,...&Dismukes G.C..(2018).Selective CO2 reduction to C3 and C4 oxyhydrocarbons on nickel phosphides at overpotentials as low as 10 mV.Energy & Environmental Science,11(9).
MLA	Calvinho K.U.D.,et al."Selective CO2 reduction to C3 and C4 oxyhydrocarbons on nickel phosphides at overpotentials as low as 10 mV".Energy & Environmental Science 11.9(2018).