Macroporous Carbon-Nitride-Supported Transition-Metal Single-Atom Catalysts for Photocatalytic Hydrogen Production from Ammonia Splitting

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dc.contributor.authorLin, J.
dc.contributor.authorWang, Y.
dc.contributor.authorTian, W.
dc.contributor.authorZhang, H.
dc.contributor.authorSun, H.
dc.contributor.authorWang, S.
dc.date.issued2023
dc.description.abstractAmmonia (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.statementofresponsibilityJingkai Lin, Yantao Wang, Wenjie Tian, Huayang Zhang, Hongqi Sun, and Shaobin Wang
dc.identifier.citationACS Catalysis, 2023; 13(17):11711-11722
dc.identifier.doi10.1021/acscatal.3c02076
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.orcidLin, J. [0000-0001-6409-0146]
dc.identifier.orcidTian, W. [0000-0002-7503-5481] [0000-0002-9896-1154]
dc.identifier.orcidWang, S. [0000-0002-1751-9162]
dc.identifier.urihttps://hdl.handle.net/2440/139501
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.relation.granthttp://purl.org/au-research/grants/arc/DP200103206
dc.relation.granthttp://purl.org/au-research/grants/arc/DE220101074
dc.rights© 2023 American Chemical Society
dc.source.urihttps://doi.org/10.1021/acscatal.3c02076
dc.subjectambient ammonia splitting
dc.subjectammonia to hydrogen
dc.subjectcatalyst panel
dc.subjectsingle-atom photocatalysis
dc.subjectstructure−activity relationship
dc.titleMacroporous Carbon-Nitride-Supported Transition-Metal Single-Atom Catalysts for Photocatalytic Hydrogen Production from Ammonia Splitting
dc.typeJournal article
pubs.publication-statusPublished

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