Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 60, Issue 17, Pages 9311-9315Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202100244
Keywords
dehydrogenation; Lewis acids; molybdenum nitrides; porous materials
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Funding
- National Key Research and Development Program of China [2017YFA0700102]
- Natural Science Foundation of China [91845202]
- Dalian National Laboratory for Clean Energy [DNL180404]
- Strategic Priority Research Program of Chinese Academy of Sciences [XDB2000000]
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In this study, high-density Lewis acid sites were created and engineered on the surfaces of porous single-crystalline Mo2N and MoN monoliths to enhance the non-oxidative dehydrogenation of propane to propylene. The top-layer Mo ions with specific coordination structures provided effective activation of C-H bonds without overcracking of C-C bonds, resulting in propane conversion of approximately 11% and propylene selectivity of approximately 95% at 500 degrees C.
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 Mo2N 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 approximate to 11 % and a propylene selectivity of approximate to 95 % with porous single-crystalline Mo2N and MoN monoliths at 500 degrees C.
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