气候变化领域集成服务门户(CCPortal): Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal

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DOI	10.1039/c8ee01481g
	Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal
	Han Y.; Wang Y.; Xu R.; Chen W.; Zheng L.; Han A.; Zhu Y.; Zhang J.; Zhang H.; Luo J.; Chen C.; Peng Q.; Wang D.; Li Y.
发表日期	2018
ISSN	17545692
起始页码	2348
结束页码	2352
卷号	11 期号:9
英文摘要	Adjusting the electronic structure of the active center is a highly effective strategy for improving the performance of catalysts. Herein, we report an atomically dispersed catalyst (FeCl1N4/CNS), which realized for the first time a great improvement of the ORR by controlling the electronic structure of the central metal with a coordinated chlorine. The half-wave potential of FeCl1N4/CNS is E1/2 = 0.921 V, which is the highest among the reported values for non-precious metal electrocatalysts and far exceeds that of FeN4/CN and commercial Pt/C in alkaline solution. Besides an exceptionally high kinetic current density (Jk) of 41.11 mA cm-2 at 0.85 V, it also has a good methanol tolerance and outstanding stability. Experiments and DFT demonstrated that the near-range interaction with chlorine and the long-range interaction with sulfur of Fe modulated the electronic structure of the active site, thus resulting in a great improvement of the ORR in alkaline media. The present findings could open new avenues for the design of superior electrocatalysts. © 2018 The Royal Society of Chemistry.
英文关键词	Chlorine; Design for testability; Electrocatalysts; Electrolytic reduction; Oxygen; Alkaline solutions; Half-wave potential; Kinetic currents; Long range interactions; Methanol tolerance; Non-precious metals; Oxygen Reduction; Structure engineering; Electronic structure; catalyst; electronic equipment; engineering; experimental study; metal; oxygen; performance assessment
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/190136
作者单位	Department of Chemistry, Tsinghua University, Beijing, 100084, China; School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710000, China; Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100084, China; School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore; Center for Electron Microscopy, Tianjin University of Technology, Tianjin, 300384, China
推荐引用方式 GB/T 7714	Han Y.,Wang Y.,Xu R.,et al. Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal[J],2018,11(9).
APA	Han Y..,Wang Y..,Xu R..,Chen W..,Zheng L..,...&Li Y..(2018).Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal.Energy & Environmental Science,11(9).
MLA	Han Y.,et al."Electronic structure engineering to boost oxygen reduction activity by controlling the coordination of the central metal".Energy & Environmental Science 11.9(2018).