SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2022, Vol. 43 ›› Issue (3): 240-247.DOI: 10.1016/j.cjche.2022.02.015

Previous Articles     Next Articles

Role of Ni species in ZnO supported on Silicalite-1 for efficient propane dehydrogenation

Bofeng Zhang1, Mingxia Song1, Hongwang Liu1, Guozhu Li1, Sibao Liu1, Li Wang1, Xiangwen Zhang1, Guozhu Liu1,2,3   

  1. 1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
    2. Zhejiang Institute of Tianjin University, Ningbo 315201, China;
    3. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China
  • Received:2021-08-31 Revised:2022-02-23 Online:2022-04-28 Published:2022-03-28
  • Contact: Guozhu Liu,E-mail:gliu@tju.edu.cn
  • Supported by:
    Financial supports by the National Natural Science Foundation of China (22025802) and the Haihe Laboratory of Sustainable Chemical Transformations (CYZC202101) is gratefully acknowledged.

Role of Ni species in ZnO supported on Silicalite-1 for efficient propane dehydrogenation

Bofeng Zhang1, Mingxia Song1, Hongwang Liu1, Guozhu Li1, Sibao Liu1, Li Wang1, Xiangwen Zhang1, Guozhu Liu1,2,3   

  1. 1. Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
    2. Zhejiang Institute of Tianjin University, Ningbo 315201, China;
    3. Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China
  • 通讯作者: Guozhu Liu,E-mail:gliu@tju.edu.cn
  • 基金资助:
    Financial supports by the National Natural Science Foundation of China (22025802) and the Haihe Laboratory of Sustainable Chemical Transformations (CYZC202101) is gratefully acknowledged.

Abstract: Propane dehydrogenation (PDH) is one of the most effective technologies to produce propene. Non-noble zinc-based catalysts have paid increasing attention because of low cost and nontoxic, compared with industrial Pt and Cr-based catalysts. However, they often suffer from limited catalytic activity and poor stability. Here, we introduced moderate Ni into ZnO supported Silicalite-1 zeolite to increase catalytic activity and stability simultaneously. Zn2+ was the definite active site and NiZn alloy facilitated the sluggish H recombination into H2 via reverse spillover. Furthermore, the introduction of Ni increased Lewis acid strength caused by electron transfer from ZnO to NiZn alloy, contributing to improved stability. For resulted 0.5NiZn/S-1, propene formation rate was 0.18 mol C3H6·(g Zn)-1·h-1 at 550 ℃, which was above 1.5 times higher than that over Zn/S-1 without Ni. Under stability test, the deactivation of 0.5NiZn/S-1 was 0.019 h-1, which was only 1/10 of that over Zn/S-1.

Key words: Propane dehydrogenation, NiZn alloy, Reverse hydrogen spillover, Lewis acid, Zeolite

摘要: Propane dehydrogenation (PDH) is one of the most effective technologies to produce propene. Non-noble zinc-based catalysts have paid increasing attention because of low cost and nontoxic, compared with industrial Pt and Cr-based catalysts. However, they often suffer from limited catalytic activity and poor stability. Here, we introduced moderate Ni into ZnO supported Silicalite-1 zeolite to increase catalytic activity and stability simultaneously. Zn2+ was the definite active site and NiZn alloy facilitated the sluggish H recombination into H2 via reverse spillover. Furthermore, the introduction of Ni increased Lewis acid strength caused by electron transfer from ZnO to NiZn alloy, contributing to improved stability. For resulted 0.5NiZn/S-1, propene formation rate was 0.18 mol C3H6·(g Zn)-1·h-1 at 550 ℃, which was above 1.5 times higher than that over Zn/S-1 without Ni. Under stability test, the deactivation of 0.5NiZn/S-1 was 0.019 h-1, which was only 1/10 of that over Zn/S-1.

关键词: Propane dehydrogenation, NiZn alloy, Reverse hydrogen spillover, Lewis acid, Zeolite