Maeno Zen, Yasumura Shunsaku, Wu Xiaopeng, Huang Mengwen, Liu Chong, Toyao Takashi, Shimizu Ken-Ichi
Institute for Catalysis, Hokkaido University, N-21, W-10, Sapporo 001-0021, Japan.
Elements Strategy Initiative for Catalysts and Batteries, Kyoto University, Katsura, Kyoto 615-8520, Japan.
J Am Chem Soc. 2020 Mar 11;142(10):4820-4832. doi: 10.1021/jacs.9b13865. Epub 2020 Mar 2.
The study of the formation, characterization, and functionality of isolated surface hydrides on solid materials is a formidable task because of the complexity of solid surfaces and the difficulty of analyzing structures in solids. Herein, we found the formation of indium (In) hydride species supported by CHA zeolites. The In hydrides were formed by treatment of an In-exchanged CHA zeolite (In-CHA) with H at high temperatures (>773 K). Fourier transform infrared (FTIR) spectroscopy and density functional theory (DFT) calculations revealed that an [InH] ion on a framework anionic site is a plausible structure. In-CHA exhibited high selectivity and durable catalytic activity for the nonoxidative dehydrogenation of ethane for at least 90 h. Kinetic and spectroscopic studies as well as transition state (TS) calculations suggested that [InH] ions serve as catalytically active sites for selective dehydrogenation using In-CHA.
由于固体表面的复杂性以及分析固体结构的困难，研究固体材料上孤立表面氢化物的形成、表征和功能是一项艰巨的任务。在此，我们发现了由CHA沸石负载的铟（In）氢化物物种的形成。通过在高温（>773 K）下用H处理铟交换的CHA沸石（In-CHA）形成了In氢化物。傅里叶变换红外（FTIR）光谱和密度泛函理论（DFT）计算表明，骨架阴离子位点上的[InH]离子是一种合理的结构。In-CHA在乙烷的非氧化脱氢反应中表现出高选择性和持久的催化活性，至少持续90小时。动力学和光谱研究以及过渡态（TS）计算表明，[InH]离子是使用In-CHA进行选择性脱氢的催化活性位点。
