Isolated Indium Hydrides in CHA Zeolites: Speciation and Catalysis for Nonoxidative Dehydrogenation of Ethane
Isolated Indium Hydrides in CHA Zeolites: Speciation and Catalysis for Nonoxidative Dehydrogenation of Ethane
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DOI：
10.1021/jacs.9b13865
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发表时间：
2020-03-11
影响因子：
15
通讯作者：
Shimizu, Ken-ichi
中科院分区：
文献类型：
--
作者：
Maeno, Zen;Yasumura, Shunsaku;Shimizu, Ken-ichi
由于固体表面的复杂性和固体结构分析的困难性，研究固体材料上孤立表面层的形成、表征和功能是一项艰巨的任务。在此，我们发现了由CHA沸石支撑的氢化铟（In）物种的形成。在高温（> 773 K）下用H-2处理In交换的CHA沸石（In-CHA）形成In氧化物。原位傅里叶变换红外光谱（FTIR）和密度泛函理论（DFT）计算表明，[InH2]（+）离子位于骨架阴离子位置上是一种合理的结构。In-CHA对乙烷非氧化脱氢反应具有高选择性和稳定的催化活性。动力学和原位光谱研究以及过渡态（TS）计算表明，[InH2]（+）离子作为选择性脱氢使用In-CHA的催化活性位点。
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-2 at high temperatures (>773 K). In situ Fourier transform infrared (FTIR) spectroscopy and density functional theory (DFT) calculations revealed that an [InH2](+) 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 in situ spectroscopic studies as well as transition state (TS) calculations suggested that [InH2](+) ions serve as catalytically active sites for selective dehydrogenation using In-CHA.