Defective TiO x overlayers catalyze propane dehydrogenation promoted by base metals

Author:

Chen Sai123ORCID,Xu Yiyi123ORCID,Chang Xin234ORCID,Pan Yue5,Sun Guodong1234,Wang Xianhui123ORCID,Fu Donglong123ORCID,Pei Chunlei123ORCID,Zhao Zhi-Jian123ORCID,Su Dong5ORCID,Gong Jinlong12346ORCID

Affiliation:

1. School of Chemical Engineering and Technology, Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin University, Tianjin 300072, China.

2. Collaborative Innovation Center for Chemical Science and Engineering (Tianjin), Tianjin 300072, China.

3. International Joint Laboratory of Low-carbon Chemical Engineering of Ministry of Education, Tianjin 300350, China.

4. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China.

5. Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.

6. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China.

Abstract

The industrial catalysts utilized for propane dehydrogenation (PDH) to propylene, an important alternative to petroleum-based cracking processes, either use expensive metals or metal oxides that are environmentally unbenign. We report that a typically less-active oxide, titanium oxide (TiO 2 ), can be combined with earth-abundant metallic nickel (Ni) to form an unconventional Ni@TiO x catalyst for efficient PDH. The catalyst demonstrates a 94% propylene selectivity at 40% propane conversion and superior stability under industrially relevant conditions. Complete encapsulation of Ni nanoparticles was allowed at elevated temperatures (>550°C). A mechanistic study suggested that the defective TiO x overlayer consisting of tetracoordinated Ti sites with oxygen vacancies is catalytically active. Subsurface metallic Ni acts as an electronic promoter to accelerate carbon-hydrogen bond activation and hydrogen (H 2 ) desorption on the TiO x overlayer.

Publisher

American Association for the Advancement of Science (AAAS)

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