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https://hdl.handle.net/2440/139501
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dc.contributor.author | Lin, J. | - |
dc.contributor.author | Wang, Y. | - |
dc.contributor.author | Tian, W. | - |
dc.contributor.author | Zhang, H. | - |
dc.contributor.author | Sun, H. | - |
dc.contributor.author | Wang, S. | - |
dc.date.issued | 2023 | - |
dc.identifier.citation | ACS Catalysis, 2023; 13(17):11711-11722 | - |
dc.identifier.issn | 2155-5435 | - |
dc.identifier.issn | 2155-5435 | - |
dc.identifier.uri | https://hdl.handle.net/2440/139501 | - |
dc.description.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. | - |
dc.description.statementofresponsibility | Jingkai Lin, Yantao Wang, Wenjie Tian, Huayang Zhang, Hongqi Sun, and Shaobin Wang | - |
dc.language.iso | en | - |
dc.publisher | American Chemical Society (ACS) | - |
dc.rights | © 2023 American Chemical Society | - |
dc.source.uri | http://dx.doi.org/10.1021/acscatal.3c02076 | - |
dc.subject | ammonia to hydrogen | - |
dc.subject | ambient ammonia splitting | - |
dc.subject | single-atom photocatalysis | - |
dc.subject | catalyst panel | - |
dc.subject | structure−activity relationship | - |
dc.title | Macroporous Carbon-Nitride-Supported Transition-Metal Single-Atom Catalysts for Photocatalytic Hydrogen Production from Ammonia Splitting | - |
dc.type | Journal article | - |
dc.identifier.doi | 10.1021/acscatal.3c02076 | - |
dc.relation.grant | http://purl.org/au-research/grants/arc/DP200103206 | - |
dc.relation.grant | http://purl.org/au-research/grants/arc/DE220101074 | - |
pubs.publication-status | Published online | - |
dc.identifier.orcid | Lin, J. [0000-0001-6409-0146] | - |
dc.identifier.orcid | Tian, W. [0000-0002-9896-1154] | - |
dc.identifier.orcid | Wang, S. [0000-0002-1751-9162] | - |
Appears in Collections: | Chemical Engineering publications |
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