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Determining the contribution of mo single atoms components in moO_(2)nanocatalyst in transfer hydrogenation

Nano Research 2023年第2期16卷 2302-2310页

作者： Ze-Nan Hu Yongjian Ai Yan Zhao Yiming Wang Kelong Ding Wenhui Zhang Rongxiu Guo Xinyue Zhang Xiangbin Cai Ning Wang Jianshe Hu Qionglin Liang Hongyang Liu Fei Huang Limin Wu Jiangwei Zhang Hong-bin Sun School of Environmental Engineering and Chemistry Luoyang Institute of Science and TechnologyLuoyang 471023China Department of Chemistry Northeastern UniversityShenyang 110819China moE Key Laboratory of Bioorganic Phosphorus Chemistry&Chemical Biology Beijing Key Lab of Microanalytical Methods&InstrumentationDepartment of ChemistryCenter for Synthetic and Systems BiologyTsinghua UniversityBeijing 100084China College of Energy Material and Chemistry Inner Mongolia UniversityHohhot 010021China Department of Physics and Center for Quantum Materials Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong SARChina Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China

Nanocatalysts are likely to contain undetected single-atom components,which may have been ignored but have significant effect in catalytic reactions.Herein,we report a catalyst composed of mo single atoms(SAs)and moO_(2)nanoparticles(NPs)(moSAs-moO_(2)@NC),which is an exact model to understand how the SAs contribute to the nanocatalyst.Both experimental results and the density functional theory calculations reveal that mo SAs on nitrogen-doped carbon provides the reaction zone for nitro reduction,while moO_(2)is the active site for decomposing hydrazine hydrate to produce H*.Thanks to the synergy between mo SAs and moO_(2)NPs,this catalyst exhibits noble metal-like catalytic activity(100%conversion at 4 min)for the dechlorination-proof transfer hydrogenation.Additionally,the hydrogen migration on the catalyst is verified by the electrochemical tests in the absence of a hydrogen source.This work provides a model for further study on the coexistence of single atoms in nanoparticle catalysts.

关键词： synergistic effect mo single atoms moO_(2)nanocatalyst transfer hydrogenation nitroarenes

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An in-situ NH_(4)^(+)-etched strategy for anchoring atomic mo site on ZnIn_(2)S_(4) hierarchical nanotubes for superior hydrogen photocatalysis

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Science China Chemistry 2021年第10期64卷 1716-1722页

作者： Yuguang Chao Weiyu Zhang Peng Zhou Hui Chen Shiyu Lu Menggang Li Qinghua Zhang Lin Gu Shaojun Guo School of Materials Science and Engineering Peking UniversityBeijing 100871China Institute of Physics Chinese Academy of SciencesBeijing 100190China Beijing Innovation Center for Engineering Science and Advanced Technology(BIC-ESAT) College of EngineeringPeking UniversityBeijing 100871China

Atomic sites co-catalyst (ASC) on photocatalytic materials possesses an attractive prospect to promote charge carrier separation and tune surface reaction kinetics,yet the synthesis of earth-abundant ASC under low temperature remains a great challenge.Here,a novel in-situ NH_(4)^(+)-etched strategy to anchor atomic mo sites on ZnIn_(2)S_(4)hierarchical nanotubes (HNTs) with abundant mesopores under mild conditions for promoting charge carrier separation and enhancing light multi-reflections is developed for efficient photocatalytic H_(2) evolution.Density functional theory calculations and linear sweep voltammetry demonstrate that the well-defined mo-S_(2)O_(1) sites with distinctive coordination configuration and electronic property contribute to the enhanced separation of photo-generated charge carriers and reduced Gibbs free energy for H_(2) evolution.Consequently,the well-defined moSA-ZIS HNTs present an excellent photocatalytic activity with a rate of 29.9μmol h^(-1)(5.98 mmol g^(-1)h^(-1)),which is 7.3 times higher than that of ZnIn_(2)S_(4)nanosheets (NSs),to be among the best ZnIn_(2)S_(4)-based photocatalysts.The present strategy breaks the high-temperature limitation of conventional top-down thermal dissociation/emitting approach for anchoring non-noble metal atomic sites on catalyst support.

关键词： in-situ NH_(4)^(+)-etched hierarchical nanotubes mo single atoms photocatalytic H_(2)evolution

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