气候变化领域集成服务门户(CCPortal): Fe1N4-O1site with axial Fe-O coordination for highly selective CO2reduction over a wide potential range

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DOI	10.1039/d1ee00569c
	Fe1N4-O1site with axial Fe-O coordination for highly selective CO2reduction over a wide potential range
	Chen Z.; Huang A.; Yu K.; Cui T.; Zhuang Z.; Liu S.; Li J.; Tu R.; Sun K.; Tan X.; Zhang J.; Liu D.; Zhang Y.; Jiang P.; Pan Y.; Chen C.; Peng Q.; Li Y.
发表日期	2021
ISSN	17545692
起始页码	3430
结束页码	3437
卷号	14 期号:6
英文摘要	On the path to deploying the electrochemical CO2reduction reaction (CO2RR) to CO, the narrow potential range under the high Faraday efficiency of CO (FECO) still blocks its ultimate practical viability. Engineering the electronic structureviaheteroatom doping is supposed to be efficient. However, a feasible synthesis and precise control are still challenging. Here, we propose a fast-pyrolyzing and controllable-activation strategy to construct an O-rich carbonaceous support and atomically dispersed FeN4site with axial O coordination (Fe1N4-O1), which was confirmed by aberration-corrected electron microscopy and X-ray absorption spectroscopy. A wide potential range of 310 mV (−0.56 V to −0.87 Vvs.RHE) could be achieved when FECOwas continuously maintained at nearly 100%, which exceeded the existing results to the best of our knowledge. DFT calculations revealed that the superior performance originated from the axial O-coordination induced electronic localization enhancement, which could facilitate the desorption of CO and increase the energy barrier for the competitive hydrogen evolution reaction. © The Royal Society of Chemistry 2021.
英文关键词	Coordination reactions; Hydrogen evolution reaction; Iron compounds; X ray absorption spectroscopy; Aberration-corrected electron microscopy; Carbonaceous supports; DFT calculation; Electronic localization; Faraday efficiency; Potential range; Precise control; Pyrolyzing; Nitrogen compounds; absorption; activation energy; carbon dioxide; chemical bonding; correction; desorption; electrochemistry; hydrogen; iron; 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/190646
作者单位	Department of Chemistry, Tsinghua University, Beijing, 100084, China; School of Electronics Science and Engineering, University of Electronic Science and Technology of China, Chengdu, 610054, China; Chemistry and Chemical Engineering Guangdong Laboratory, Shantou, 515031, China
推荐引用方式 GB/T 7714	Chen Z.,Huang A.,Yu K.,et al. Fe1N4-O1site with axial Fe-O coordination for highly selective CO2reduction over a wide potential range[J],2021,14(6).
APA	Chen Z..,Huang A..,Yu K..,Cui T..,Zhuang Z..,...&Li Y..(2021).Fe1N4-O1site with axial Fe-O coordination for highly selective CO2reduction over a wide potential range.Energy & Environmental Science,14(6).
MLA	Chen Z.,et al."Fe1N4-O1site with axial Fe-O coordination for highly selective CO2reduction over a wide potential range".Energy & Environmental Science 14.6(2021).