Supported Rhodium Catalysts for Ammonia-Borane Hydrolysis: Dependence of the Catalytic Activity on the Highest Occupied State of the Single Rhodium Atoms.
Supported Rhodium Catalysts for Ammonia-Borane Hydrolysis: Dependence of the Catalytic Activity on the Highest Occupied State of the Single Rhodium Atoms.
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DOI：
10.1002/anie.201701089
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发表时间：
2017-04
影响因子：
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通讯作者：
Liangbing Wang;Hongliang Li;Wenbo Zhang;Xiao Zhao;Jianxiang Qiu;Aowen Li;Xusheng Zheng;Zhenpeng Hu-Z
中科院分区：
文献类型：
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作者：
Liangbing Wang;Hongliang Li;Wenbo Zhang;Xiao Zhao;Jianxiang Qiu;Aowen Li;Xusheng Zheng;Zhenpeng Hu-Z
负载型金属纳米晶在制氢反应中表现出了显著的催化性能，其催化性能受其载体的影响甚至决定。因此，确定催化性能和金属-载体相互作用之间的直接关系是至关重要的。在这里，我们提供了一个定量的配置文件，探索金属支持相互作用，考虑在单原子催化剂的最高占据状态。所研究的催化剂由分散在VO 2纳米棒表面的孤立Rh原子组成。结果表明，氨-硼烷水解反应的活化能随底物的相变而变化。机理研究表明，催化性能直接取决于单个Rh原子的最高占据态，这是由衬底的能带结构决定的。其他金属催化剂，甚至与非贵金属，表现出显着的催化活性对NH3-BH 3水解，合理地设计，通过调整其最高占据状态。
Supported metal nanocrystals have exhibited remarkable catalytic performance in hydrogen generation reactions, which is influenced and even determined by their supports. Accordingly, it is of fundamental importance to determine the direct relationship between catalytic performance and metal-support interactions. Herein, we provide a quantitative profile for exploring metal-support interactions by considering the highest occupied state in single-atom catalysts. The catalyst studied consisted of isolated Rh atoms dispersed on the surface of VO2 nanorods. It was observed that the activation energy of ammonia-borane hydrolysis changed when the substrate underwent a phase transition. Mechanistic studies indicate that the catalytic performance depended directly on the highest occupied state of the single Rh atoms, which was determined by the band structure of the substrates. Other metal catalysts, even with non-noble metals, that exhibited significant catalytic activity towards NH3 BH3 hydrolysis were rationally designed by adjusting their highest occupied states.