期刊
ACS APPLIED MATERIALS & INTERFACES
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c09241
关键词
nitrate reduction reactions; ammonia synthesis; electrocatalysts; metal-organic frameworks; Cu clusters
资金
- Qilu Young Scholarship Funding of Shandong University
- National Natural Science Foundation of China [22005176, 92061119]
- Natural Science Foundation of Shandong Province [ZR2020QE014, ZR2020ZD35]
- Natural Science Foundation of Jiangsu Province [BK20200228]
- Beijing NOVA program [Z201100006820066]
- Taishan Scholar Project of Shandong Province [ts201712011]
In this study, a metal cluster-conductive metal-organic framework (MOF) composite electrocatalyst Cu@CuHHTP is successfully constructed using an in situ synthetic strategy. Cu@CuHHTP exhibits superb performance for the electrocatalytic nitrate reduction reaction (NO3-RR) with a conversion rate of 85.81% and a selectivity for NH3 of 96.84%.
The electrocatalytic nitrate reduction reaction (NO3-RR) to ammonia (NH3) under ambient conditions not only has the benefit of lowering energy consumption, but also helps remove nitrate contamination. Inspired by the unique structure of nitrate/nitrite reductase with the active spheroproteins encapsulated by larger enzymes, herein, we develop an in situ synthetic strategy for the construction of metal cluster-conductive metal-organic framework (MOF) composite electrocatalysts. The metallic Cu clusters are filled into the mesopores of a conductive copper-based MOF (i.e., CuHHTP); meanwhile, CuHHTP with a porous structure provides an internal environment to limit the growth of metallic Cu clusters with an ultrasmall size (i.e., 1.5 +/- 0.2 nm) and restrains their aggregation. The obtained Cu@CuHHTP exhibits superb performance for NO3-RR. In a neutral electrolyte with 500 ppm NO3-, Cu@CuHHTP shows a high NO3- conversion of 85.81% and a selectivity for NH3 of 96.84%. N-15 isotope labeling experiments confirm that the formation of NH3 originates from the process of NO3-RR. Theoretical calculations confirm that Cu clusters are the active sites in the composite electrocatalysts, in which the proper d-band center and the accept-donate mechanism in charge transfer are the key factors for the improvement of the electrocatalytic performance.
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