Macroporous Carbon-Nitride-Supported Transition-Metal Single-Atom Catalysts for Photocatalytic Hydrogen Production from Ammonia Splitting
Date
2023
Authors
Lin, J.
Wang, Y.
Tian, W.
Zhang, H.
Sun, H.
Wang, S.
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Journal article
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ACS Catalysis, 2023; 13(17):11711-11722
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Jingkai Lin, Yantao Wang, Wenjie Tian, Huayang Zhang, Hongqi Sun, and Shaobin Wang
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Abstract
Ammonia (NH3) splitting to hydrogen (H2) is a promising route for on-site production of green hydrogen energy; however, the application is limited due to high-cost noblemetal-based catalysts and high operating temperature of the endothermic nature. Herein, we develop a series of macroporous carbon nitride-supported single-atom transition metal (TMsMCN, TMs: Co, Mn, Fe, Ni, Cu) catalyst panels for solar light-driven photocatalytic gaseous NH3 splitting. Under ambient reaction conditions, the optimized Ni-MCN shows an H2 production rate of 35.6 μmol g−1 h−1 , much superior to that of MCN and other TMs-MCN. Such enhanced photoactivity is attributed to the presence of Ni−N4 sites, which improve the optical properties, accelerate charge carrier separation/ transfer, and boost NH3 splitting kinetics of the catalysts. Density functional theory calculations further reveal that the Ni−N4 sites can effectively modify the electronic structure of the carbon nitride. Compared with other metal sites, the Ni−N4 site possesses moderate NH3 binding strength and the lowest energy barrier to facilitate the formation of key intermediates *NH + *H. These findings provide valuable guidelines for the rational design of single-atom catalysts toward energy- and cost-effective photocatalytic NH3 splitting for H2 production.
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© 2023 American Chemical Society