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作者机构:Key Laboratory of Optoelectronic Materials Chemistry and Physics Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Key Laboratory of Design & Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 China Advanced Energy Science and Technology Guangdong Laboratory 29 Sanxin North Road Huizhou Guangdong 116023 China
出 版 物:《Angewandte Chemie》
年 卷 期:2021年第133卷第17期
学科分类:081704[工学-应用化学] 08[工学] 0817[工学-化学工程与技术]
主 题:dehydrogenation Lewis acids molybdenum nitrides porous materials
摘 要:The non-oxidative dehydrogenation of propane to propylene plays an important role in the light-olefin chemical industry. However, the conversion and selectivity remain a fundamental challenge at low temperatures. Here we create and engineer high-density Lewis acid sites at well-defined surfaces in porous single-crystalline Mo 2 N and MoN monoliths to enhance the non-oxidative dehydrogenation of propane to propylene. The top-layer Mo ions with unsaturated Mo-N 1/6 and Mo-N 1/3 coordination structures provide high-density Lewis acid sites at the surface, leading to the effective activation of C−H bonds without the overcracking of C−C bonds during the non-oxidative dehydrogenation of propane. We demonstrate a propane conversion of ≈11 % and a propylene selectivity of ≈95 % with porous single-crystalline Mo 2 N and MoN monoliths at 500 °C.