Isolated boron in zeolite for oxidative dehydrogenation of propane

Hang Zhou; Xianfeng Yi; Yu Hui; Liang Wang; Wei Chen; Yucai Qin; Ming Wang; Jiabi Ma; Xuefeng Chu; Yeqing Wang; Xin Hong; Zifeng Chen; Xiangju Meng; Hai Wang; Qiuyan Zhu; Lijuan Song; Anmin Zheng; Feng-Shou Xiao

doi:10.1126/science.abe7935

Isolated boron in zeolite for oxidative dehydrogenation of propane

Science. 2021 Apr 2;372(6537):76-80. doi: 10.1126/science.abe7935.

Authors

Hang Zhou^{1

2}, Xianfeng Yi^{3

2}, Yu Hui^{4

2}, Liang Wang^{5

6}, Wei Chen³, Yucai Qin⁴, Ming Wang⁷, Jiabi Ma⁷, Xuefeng Chu⁸, Yeqing Wang⁹, Xin Hong⁹, Zifeng Chen⁹, Xiangju Meng¹⁰, Hai Wang¹, Qiuyan Zhu⁹, Lijuan Song⁴, Anmin Zheng¹¹, Feng-Shou Xiao^{5

6

9}

Affiliations

¹ Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
² These authors contributed equally to this work.
³ National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China.
⁴ Key Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Shihua University, Fushun 113001, China.
⁵ Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China. liangwang@zju.edu.cn zhenganm@wipm.ac.cn mengxj@zju.edu.cn fsxiao@zju.edu.cn.
⁶ Ningbo Research Institute, Zhejiang University, Ningbo 315100, China.
⁷ Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing 100081, China.
⁸ Key Laboratory of Architectural Cold Climate Energy Management, Jilin Jianzhu University, Changchun 130118, China.
⁹ Department of Chemistry, Zhejiang University, Hangzhou 310028, China.
¹⁰ Department of Chemistry, Zhejiang University, Hangzhou 310028, China. liangwang@zju.edu.cn zhenganm@wipm.ac.cn mengxj@zju.edu.cn fsxiao@zju.edu.cn.
¹¹ National Center for Magnetic Resonance in Wuhan, State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, China. liangwang@zju.edu.cn zhenganm@wipm.ac.cn mengxj@zju.edu.cn fsxiao@zju.edu.cn.

PMID: 33795454
DOI: 10.1126/science.abe7935

Abstract

Oxidative dehydrogenation of propane (ODHP) is a key technology for producing propene from shale gas, but conventional metal oxide catalysts are prone to overoxidation to form valueless CO _x Boron-based catalysts were recently found to be selective for this reaction, and B-O-B oligomers are generally regarded as active centers. We show here that the isolated boron in a zeolite framework without such oligomers exhibits high activity and selectivity for ODHP, which also hinders full hydrolysis for boron leaching in a humid atmosphere because of the B-O-SiO _x linkage, achieving superior durability in a long-period test. Furthermore, we demonstrate an isolated boron with a -B[OH…O(H)-Si]₂ structure in borosilicate zeolite as the active center, which enables the activation of oxygen and a carbon-hydrogen bond to catalyze the ODHP.

Publication types

Research Support, Non-U.S. Gov't