Modulating Lattice Oxygen in Dual-Functional Mo-V-O Mixed Oxides for Chemical Looping Oxidative Dehydrogenation

被引:175
作者
Chen, Sai [1 ]
Zeng, Liang [1 ]
Mu, Rentao [1 ]
Xiong, Chuanye [1 ]
Zhao, Zhi-Jian [1 ]
Zhao, Chengjie [1 ]
Pei, Chunlei [1 ]
Peng, Luming [2 ]
Luo, Jun [3 ]
Fan, Liang-Shih [4 ]
Gong, Jinlong [1 ]
机构
[1] Tianjin Univ, Collaborat Innovat Ctr Chem Sci & Engn, Sch Chem Engn & Technol, Key Lab Green Chem Technol,Minist Educ, Tianjin 300072, Peoples R China
[2] Nanjing Univ, Sch Chem & Chem Engn, Minist Educ, Key Lab Mesoscop Chem, Nanjing 210093, Jiangsu, Peoples R China
[3] Tianjin Univ Technol, Sch Mat, Inst New Energy Mat & Low Carbon Technol, Ctr Electron Microscopy, Tianjin 300384, Peoples R China
[4] Ohio State Univ, William G Lowrie Dept Chem & Biomol Engn, Columbus, OH 43210 USA
基金
中国国家自然科学基金;
关键词
PROPANE DEHYDROGENATION; METAL-OXIDES; RAMAN-SPECTROSCOPY; REDOX CATALYSTS; SELECTIVITY; REACTIVITY; CHEMISTRY; OPERATION; PROPENE; ALKANES;
D O I
10.1021/jacs.9b09235
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Oxygen chemistry plays a pivotal role in numerous chemical reactions. In particular, selective cleavage of C-H bonds by metal oxo species is highly desirable in dehydrogenation of light alkanes. However, high selectivity of alkene is usually hampered through consecutive oxygenation reactions in a conventional oxidative dehydrogenation (ODH) scheme. Herein, we show that dual-functional Mo-V-O mixed oxides selectively convert propane to propylene via an alternative chemical looping oxidative dehydrogenation (CL-ODH) approach. At 500 degrees C, we obtain 89% propylene selectivity at 36% propane conversion over 100 dehydrogenation-regeneration cycles. We attribute such high propylene yield-which exceeds that of previously reported ODH catalysts-to the involvement and precise modulation of bulk lattice oxygen via atomic-scale doping of Mo and show that increasing the binding energy of V-O bonds is critical to enhance the selectivity of propylene. This work provides the fundamental understanding of metal-oxygen chemistry and a promising strategy for alkane dehydrogenation.
引用
收藏
页码:18653 / 18657
页数:5
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