气候变化领域集成服务门户(CCPortal): Efficient CO 2 to CO electrolysis on solid Ni-N-C catalysts at industrial current densities

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DOI	10.1039/c8ee02662a
	Efficient CO 2 to CO electrolysis on solid Ni-N-C catalysts at industrial current densities
	Möller T.; Ju W.; Bagger A.; Wang X.; Luo F.; Ngo Thanh T.; Varela A.S.; Rossmeisl J.; Strasser P.
发表日期	2019
ISSN	1754-5692
起始页码	640
结束页码	647
卷号	12 期号:2
英文摘要	The electrochemical CO 2 reduction reaction (CO 2 RR) to pure CO streams in electrolyzer devices is poised to be the most likely process for near-term commercialization and deployment in the polymer industry. The reduction of CO 2 to CO is electrocatalyzed under alkaline conditions on precious group metal (PGM) catalysts, such as silver and gold, limiting widespread application due to high cost. Here, we report on an interesting alternative, a PGM-free nickel and nitrogen-doped porous carbon catalyst (Ni-N-C), the catalytic performance of which rivals or exceeds those of the state-of-the-art electrocatalysts under industrial electrolysis conditions. We started from small scale CO 2 -saturated liquid electrolyte H-cell screening tests and moved to larger-scale CO 2 electrolyzer cells, where the catalysts were deployed as Gas Diffusion Electrodes (GDEs) to create a reactive three-phase interface. We compared the faradaic CO yields and CO partial current densities of Ni-N-C catalysts to those of a Ag-based benchmark, and its Fe-functionalized Fe-N-C analogue under ambient pressures, temperatures and neutral pH bicarbonate flows. Prolonged electrolyzer tests were conducted at industrial current densities of up to 700 mA cm -2 . Ni-N-C electrodes are demonstrated to provide CO partial current densities above 200 mA cm -2 and stable faradaic CO efficiencies around 85% for up to 20 hours (at 200 mA cm -2 ), unlike their Ag benchmarks. Density functional theory-based calculations of catalytic reaction pathways help offer a molecular mechanistic basis of the observed selectivity trends on Ag and M-N-C catalysts. Computations lend much support to our experimental hypothesis as to the critical role of N-coordinated metal ion, Ni-N x , motifs as the catalytic active sites for CO formation. Apart from being cost effective, the Ni-N-C powder catalysts allow flexible operation under acidic, neutral, and alkaline conditions. This study demonstrates the potential of Ni-N-C and possibly other members of the M-N-C materials family to replace PGM catalysts in CO 2 -to-CO electrolyzers. © 2019 The Royal Society of Chemistry.
语种	英语
scopus关键词	Alkalinity; Carbon dioxide; Catalysis; Catalyst selectivity; Cost effectiveness; Current density; Density functional theory; Diffusion in gases; Doping (additives); Electrocatalysts; Electrodes; Electrolysis; Electrolytes; Electrolytic cells; Iron compounds; Metal ions; Phase interfaces; Porous materials; Reduction; Silver; Silver compounds; Alkaline conditions; Catalytic active sites; Catalytic performance; Catalytic reactions; Flexible operation; Gas diffusion electrodes; Industrial electrolysis; Polymer industries; Nickel compounds; carbon; carbon dioxide; carbon monoxide; catalysis; catalyst; electrochemical method; electrokinesis; industrial technology; nickel; nitrogen; solid
来源期刊	Energy and Environmental Science
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/162685
作者单位	Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, Berlin, Germany; Department of Chemistry, University Copenhagen, Universitetsparken 5, Copenhagen, 2100, Denmark; Institute of Chemistry, National Autonomous University of Mexico, Mexico City, Mexico
推荐引用方式 GB/T 7714	Möller T.,Ju W.,Bagger A.,et al. Efficient CO 2 to CO electrolysis on solid Ni-N-C catalysts at industrial current densities[J],2019,12(2).
APA	Möller T..,Ju W..,Bagger A..,Wang X..,Luo F..,...&Strasser P..(2019).Efficient CO 2 to CO electrolysis on solid Ni-N-C catalysts at industrial current densities.Energy and Environmental Science,12(2).
MLA	Möller T.,et al."Efficient CO 2 to CO electrolysis on solid Ni-N-C catalysts at industrial current densities".Energy and Environmental Science 12.2(2019).