Knowledge Management System Of Guangzhou Institute of Energy Conversion, CAS
| In Situ Clustering of Single-Atom Copper Precatalysts in a Metal-Organic Framework for Efficient Electrocatalytic Nitrate-to-Ammonia Reduction | |
Xu, Yan-Tong1; Xie, Meng-Yuan1,3; Zhong, Huiqiong1 ; Cao, Yan1,2
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| 2022-07-06 | |
| Source Publication | ACS CATALYSIS
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| ISSN | 2155-5435 |
| Pages | 9 |
| Corresponding Author | Cao, Yan(caoyan@ms.giec.ac.cn) |
| Abstract | 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. |
| Keyword | self-reconstruction metal-organic framework single-atom electrocatalytic ammonia synthesis nitrate electroreduction |
| DOI | 10.1021/acscatal.2c02033 |
| WOS Keyword | CAUCHY WAVELET TRANSFORM ; OXIDATION ; XAFS ; CU |
| Indexed By | SCI |
| Language | 英语 |
| Funding Project | 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 Research Area | Chemistry |
| Funding Organization | 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 Subject | Chemistry, Physical |
| WOS ID | WOS:000830920800001 |
| Publisher | AMER CHEMICAL SOC |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://ir.giec.ac.cn/handle/344007/37040 |
| Collection | 中国科学院广州能源研究所 |
| Corresponding Author | Cao, Yan |
| Affiliation | 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 |
| First Author Affilication | GuangZhou Institute of Energy Conversion,Chinese Academy of Sciences |
| Recommended Citation 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. |
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