The nature of the deactivation of hydrothermally stable Ni/SiO2-Al2O3 catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol

doi:10.1016/j.cjche.2019.03.008

中国化学工程学报 ›› 2019, Vol. 27 ›› Issue (12): 2960-2967.DOI: 10.1016/j.cjche.2019.03.008

The nature of the deactivation of hydrothermally stable Ni/SiO₂-Al₂O₃ catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol

Haitao Li¹, Yin Zhang¹, Hongxi Zhang¹, Xiaoqin Qin¹, Yalin Xu¹, Ruifang Wu¹, Zheng Jiang², Yongxiang Zhao¹

1 Engineering Research Center of Ministry of Education for Fine Chemicals, Shanxi University, Taiyuan 030006, China;
2 Faculty of Engineering and the Environment, University of Southampton, Southampton SO17 1BJ, UK

收稿日期:2018-01-12 修回日期:2019-03-02 出版日期:2019-12-28 发布日期:2020-03-17
通讯作者: Haitao Li, Yongxiang Zhao
基金资助:
Supported by the National Natural Science Foundation of China (21673132).

The nature of the deactivation of hydrothermally stable Ni/SiO₂-Al₂O₃ catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol

Haitao Li¹, Yin Zhang¹, Hongxi Zhang¹, Xiaoqin Qin¹, Yalin Xu¹, Ruifang Wu¹, Zheng Jiang², Yongxiang Zhao¹

1 Engineering Research Center of Ministry of Education for Fine Chemicals, Shanxi University, Taiyuan 030006, China;
2 Faculty of Engineering and the Environment, University of Southampton, Southampton SO17 1BJ, UK

Received:2018-01-12 Revised:2019-03-02 Online:2019-12-28 Published:2020-03-17
Contact: Haitao Li, Yongxiang Zhao
Supported by:
Supported by the National Natural Science Foundation of China (21673132).

摘要/Abstract

摘要： The deactivation of Ni/SiO₂-Al₂O₃ catalyst in hydrogenation of crude 1,4-butanediol was investigated. During the operation time of 2140 h, the catalyst showed slow activity decay. Characterization results, for four spent catalysts used at different time, indicated that the main reason of the catalyst deactivation was the deposition of carbonaceous species that covered the active Ni and blocked mesopores of the catalyst. The TPO and SEM measurements revealed that the carbonaceous species included both oligomeric and polymeric species with high C/H ratio and showed sheet. Such carbonaceous species might be eliminated through either direct H₂ reduction or the combined oxidation-reduction methodologies.

关键词: 1,4-Butanediol, Hydrogenation, Ni/SiO₂-Al₂O₃ catalyst, Deactivation, Regeneration

Abstract: The deactivation of Ni/SiO₂-Al₂O₃ catalyst in hydrogenation of crude 1,4-butanediol was investigated. During the operation time of 2140 h, the catalyst showed slow activity decay. Characterization results, for four spent catalysts used at different time, indicated that the main reason of the catalyst deactivation was the deposition of carbonaceous species that covered the active Ni and blocked mesopores of the catalyst. The TPO and SEM measurements revealed that the carbonaceous species included both oligomeric and polymeric species with high C/H ratio and showed sheet. Such carbonaceous species might be eliminated through either direct H₂ reduction or the combined oxidation-reduction methodologies.

Key words: 1,4-Butanediol, Hydrogenation, Ni/SiO₂-Al₂O₃ catalyst, Deactivation, Regeneration

Haitao Li, Yin Zhang, Hongxi Zhang, Xiaoqin Qin, Yalin Xu, Ruifang Wu, Zheng Jiang, Yongxiang Zhao. The nature of the deactivation of hydrothermally stable Ni/SiO₂-Al₂O₃ catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol[J]. 中国化学工程学报, 2019, 27(12): 2960-2967.

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The nature of the deactivation of hydrothermally stable Ni/SiO₂-Al₂O₃ catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol

The nature of the deactivation of hydrothermally stable Ni/SiO₂-Al₂O₃ catalyst in long-time aqueous phase hydrogenation of crude 1,4-butanediol

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