In Situ Clustering of Single-Atom Copper Precatalysts in a Metal-Organic Framework for Efficient Electrocatalytic Nitrate-to-Ammonia Reduction

doi:10.1021/acscatal.2c02033

GIEC OpenIR

	In Situ Clustering of Single-Atom Copper Precatalysts in a Metal-Organic Framework for Efficient Electrocatalytic Nitrate-to-Ammonia Reduction
	Xu, Yan-Tong 1; Xie, Meng-Yuan 1,3; Zhong, Huiqiong1 ; Cao, Yan 1,2
	2022-07-06
发表期刊	ACS CATALYSIS
ISSN	2155-5435
页码	9
通讯作者	Cao, Yan(caoyan@ms.giec.ac.cn)
摘要	When serving as a "precatalyst ", metal-organic frameworks (MOF) usually incur uncontrollable framework collapse in electrocatalysis. Herein, we report an anticollapse MOF-supported single-atom Cu precatalyst for electrocatalytic nitrate-to-ammonia reduction reaction (NARR), which can be applied in the rechargeable ammonia energy storage (RAES) technology. In situ X-ray absorption spectroscopy (XAS) revealed the association of the formation of real catalytic sites with the in situ clustering of single-atom Cu during NARR. Notably, the noncollapse MOF can afford the confined space to prevent the excessive aggregation of Cu atoms, leading to uniform ultrasmall nanoclusters (ca. 4 nm). Moreover, it achieves a maximal Faradaic efficiency toward NH3 of 85.5%, a formation rate of NH3 of 66 mu mol h(-1) cm(-2), and a specific activity of 53.43 mg(NH3) h(-1) mg(Cu)(-1) in 5 mM NO3- solution. The specific activity is found to be at least 3.3 times higher than that of other reported Cu-based catalysts. Density function theory (DFT) calculation further confirms the size effect and the host-guest interaction in facilitating the NO3- activation and the reaction energy decrease. Besides, it also exhibits a high selectivity of ammonia-to-nitrate of 93.3%, displaying great potential in RAES technology.
关键词	self-reconstruction metal-organic framework single-atom electrocatalytic ammonia synthesis nitrate electroreduction
DOI	10.1021/acscatal.2c02033
关键词[WOS]	CAUCHY WAVELET TRANSFORM ; OXIDATION ; XAFS ; CU
收录类别	SCI
语种	英语
资助项目	NSFC[22178339] ; China Postdoctoral Science Foundation[2021M690151] ; Special Research Assistant Program of the Chinese Academy of Sciences[1190000058] ; Hundred Talents Program (A) of Chinese Academy of Sciences (2019) ; Guangdong Basic and Applied Basic Research Foundation[2021A1515110069] ; Guangdong Basic and Applied Basic Research Foundation[2021000037] ; Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development[2021A1515110069] ; Basic Research Program of Guangzhou City[2021000037] ; [202102020866]
WOS研究方向	Chemistry
项目资助者	NSFC ; China Postdoctoral Science Foundation ; Special Research Assistant Program of the Chinese Academy of Sciences ; Hundred Talents Program (A) of Chinese Academy of Sciences (2019) ; Guangdong Basic and Applied Basic Research Foundation ; Guangdong Basic and Applied Basic Research Foundation ; Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development ; Basic Research Program of Guangzhou City
WOS类目	Chemistry, Physical
WOS记录号	WOS:000830920800001
出版者	AMER CHEMICAL SOC
引用统计	被引频次：54[WOS] [WOS记录] [WOS相关记录]
文献类型	期刊论文
条目标识符	http://ir.giec.ac.cn/handle/344007/37040
专题	中国科学院广州能源研究所
通讯作者	Cao, Yan
作者单位	1.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China 2.Anhui Univ, Coll Chem & Chem Engn, Hefei 230601, Peoples R China 3.Univ Sci & Technol China, Nano Sci & Technol Inst, Suzhou 215123, Peoples R China
第一作者单位	中国科学院广州能源研究所
推荐引用方式 GB/T 7714	Xu, Yan-Tong,Xie, Meng-Yuan,Zhong, Huiqiong,et al. In Situ Clustering of Single-Atom Copper Precatalysts in a Metal-Organic Framework for Efficient Electrocatalytic Nitrate-to-Ammonia Reduction[J]. ACS CATALYSIS,2022:9.
APA	Xu, Yan-Tong,Xie, Meng-Yuan,Zhong, Huiqiong,&Cao, Yan.(2022).In Situ Clustering of Single-Atom Copper Precatalysts in a Metal-Organic Framework for Efficient Electrocatalytic Nitrate-to-Ammonia Reduction.ACS CATALYSIS,9.
MLA	Xu, Yan-Tong,et al."In Situ Clustering of Single-Atom Copper Precatalysts in a Metal-Organic Framework for Efficient Electrocatalytic Nitrate-to-Ammonia Reduction".ACS CATALYSIS (2022):9.