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

doi:10.1016/j.cjche.2022.02.015

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 240-247.DOI: 10.1016/j.cjche.2022.02.015

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 Liu^1,2,3

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

收稿日期:2021-08-31 修回日期:2022-02-23 出版日期:2022-03-28 发布日期:2022-04-28
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.

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 Liu^1,2,3

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:2022-03-28 Published:2022-04-28
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.

摘要/Abstract

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

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

Bofeng Zhang, Mingxia Song, Hongwang Liu, Guozhu Li, Sibao Liu, Li Wang, Xiangwen Zhang, Guozhu Liu. Role of Ni species in ZnO supported on Silicalite-1 for efficient propane dehydrogenation[J]. 中国化学工程学报, 2022, 43(3): 240-247.

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

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

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