Efficient electrochemical N-2 fixation by doped-oxygen-induced phosphorus vacancy defects on copper phosphide nanosheets

doi:10.1039/c9ta13135c

	Efficient electrochemical N-2 fixation by doped-oxygen-induced phosphorus vacancy defects on copper phosphide nanosheets
	Jin, Meng 1,2; Zhang, Xian 1; Han, Miaomiao 1; Wang, Haojie 1; Wang, Guozhong 1; Zhang, Haimin 1
刊名	JOURNAL OF MATERIALS CHEMISTRY A
	2020-03-28
卷号	8
ISSN号	2050-7488
DOI	10.1039/c9ta13135c
通讯作者	Zhang, Xian(zhangxian158229@163.com) ; Zhang, Haimin(zhanghm@issp.ac.cn)
英文摘要	Anion vacancy defect-engineered catalysts have exhibited impressive activity in the electro/photocatalytic N-2 reduction reaction (NRR) because of their advantages in N-2 adsorption and activation. However, most studies have concentrated on oxygen vacancy defects because of their low formation energy. Sulfur, nitrogen, and phosphorus anion vacancy defects with higher formation energies are rarely reported. Herein, utilizing a doped-oxygen-induced strategy, partially electrochemically reduced oxygen-doped Cu3P nanosheets (RO-Cu3P) with rich surface phosphorus vacancies were successfully synthesized and could be employed as highly catalytically active species for the electrochemical NRR process. It is noteworthy that both ammonia and hydrazine were detected in the NRR tests, indicating that the reduction process followed a proposed alternating pathway. An ammonia yield of 28.12 mu g h(-1) cm(-2) with a high faradaic efficiency of 17.5% was achieved under ambient conditions for the RO-Cu3P/CFC electrode with abundant phosphorus vacancies, about 3.4 times higher than that for a prepared pure Cu3P/CFC electrode. It is believed that the RO-Cu3P species with abundant surface phosphorus vacancies are the most likely active species for NRR, as confirmed by both control experiments and density functional theory calculations. This work provides a promising strategy to design and construct efficient NRR catalysts with anion vacancy defects for good theoretical and experimental guidance.
资助项目	Anhui Provincial Natural Science Foundation[1908085QB83] ; China Postdoctoral Science Foundation[2019M652224]
WOS关键词	NITROGEN-FIXATION ; ELECTROREDUCTION ; REDUCTION ; CATALYSTS ; CATHODE ; AMMONIA ; CLOTH ; CU3P
WOS研究方向	Chemistry ; Energy & Fuels ; Materials Science
语种	英语
出版者	ROYAL SOC CHEMISTRY
WOS记录号	WOS:000526703800012
资助机构	Anhui Provincial Natural Science Foundation ; China Postdoctoral Science Foundation
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/103707]
专题	中国科学院合肥物质科学研究院
通讯作者	Zhang, Xian; Zhang, Haimin
作者单位	1.Chinese Acad Sci, Anhui Key Lab Nanomat & Nanotechnol, CAS Ctr Excellence Nanosci,Key Lab Mat Phys, Ctr Environm & Energy Nanomat,Inst Solid State Ph, Hefei 230031, Peoples R China 2.Univ Sci & Technol China, Hefei 230026, Peoples R China
推荐引用方式 GB/T 7714	Jin, Meng,Zhang, Xian,Han, Miaomiao,et al. Efficient electrochemical N-2 fixation by doped-oxygen-induced phosphorus vacancy defects on copper phosphide nanosheets[J]. JOURNAL OF MATERIALS CHEMISTRY A,2020,8.
APA	Jin, Meng,Zhang, Xian,Han, Miaomiao,Wang, Haojie,Wang, Guozhong,&Zhang, Haimin.(2020).Efficient electrochemical N-2 fixation by doped-oxygen-induced phosphorus vacancy defects on copper phosphide nanosheets.JOURNAL OF MATERIALS CHEMISTRY A,8.
MLA	Jin, Meng,et al."Efficient electrochemical N-2 fixation by doped-oxygen-induced phosphorus vacancy defects on copper phosphide nanosheets".JOURNAL OF MATERIALS CHEMISTRY A 8(2020).