Process monitoring of the Au-S bond conversion in acetylene hydrochlorination

doi:10.1016/j.cjche.2021.04.026

Chinese Journal of Chemical Engineering ›› 2022, Vol. 45 ›› Issue (5): 32-40.DOI: 10.1016/j.cjche.2021.04.026

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Process monitoring of the Au-S bond conversion in acetylene hydrochlorination

Lutai Song¹, Li Liu¹, Mingyuan Zhu^1,2, Bin Dai^1,2

1 School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832000, China;
2 Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi 832000, China

Received:2021-01-30 Revised:2021-03-30 Online:2022-06-22 Published:2022-05-28
Contact: Mingyuan Zhu,E-mail:zhuminyuan@shzu.edu.cn;Bin Dai,E-mail:db_tea@shzu.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (21666033), the State Key Research and Development Project of China (2016YFB0301603), the International Corporation of S&T Project in Xinjiang Bingtuan (2018BC003), and the International Corporation of S&T Project in Shihezi University (GJHZ201701).

Process monitoring of the Au-S bond conversion in acetylene hydrochlorination

Lutai Song¹, Li Liu¹, Mingyuan Zhu^1,2, Bin Dai^1,2

1 School of Chemistry and Chemical Engineering, Shihezi University, Shihezi 832000, China;
2 Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan, Shihezi 832000, China

通讯作者: Mingyuan Zhu,E-mail:zhuminyuan@shzu.edu.cn;Bin Dai,E-mail:db_tea@shzu.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (21666033), the State Key Research and Development Project of China (2016YFB0301603), the International Corporation of S&T Project in Xinjiang Bingtuan (2018BC003), and the International Corporation of S&T Project in Shihezi University (GJHZ201701).

Abstract

Abstract: The continuous expansion of vinyl chloride production increases environmental pollution caused by mercury catalysts, which is an issue that urgently needs to be solved. Green and stable catalysts should be researched to alleviate this issue. In this research, Thiolactic acid acts as a ligand where sulfhydryl groups form a stable complex with Au on the surface of a spherical activated carbon (SAC). An Au-thiolactic acid/SAC catalyst was designed with a Au theoretical loading of 0.5% (mass) to overcome the disadvantages of traditional Au-based catalysts, such as a low conversion rate and poor life cycle. The ratio of Au to ligand was screened, and the activity was best when Au/S = 1:8. The formation of the Au-S bond was proven by FT-IR and UV–vis. The longevity test of the Au1S8 /SAC catalyst was carried out at 1200 h^-1 for 50 h. Samples with reaction times of 0 h, 5 h, 10 h, 20 h, and 50 h were taken to monitor the catalyst status. The XPS and TPR tests proved that the Au-S bond broke as the acetylene hydrochlorination reaction proceeded. The DFT calculation proved that the Au-S bond is the active site, and the sulfur atom promotes the adsorption of C₂H₂ by the catalyst.

Key words: Acetylene hydrochlorination, Au-S bond, Process monitoring, Valence shift

摘要： The continuous expansion of vinyl chloride production increases environmental pollution caused by mercury catalysts, which is an issue that urgently needs to be solved. Green and stable catalysts should be researched to alleviate this issue. In this research, Thiolactic acid acts as a ligand where sulfhydryl groups form a stable complex with Au on the surface of a spherical activated carbon (SAC). An Au-thiolactic acid/SAC catalyst was designed with a Au theoretical loading of 0.5% (mass) to overcome the disadvantages of traditional Au-based catalysts, such as a low conversion rate and poor life cycle. The ratio of Au to ligand was screened, and the activity was best when Au/S = 1:8. The formation of the Au-S bond was proven by FT-IR and UV–vis. The longevity test of the Au1S8 /SAC catalyst was carried out at 1200 h^-1 for 50 h. Samples with reaction times of 0 h, 5 h, 10 h, 20 h, and 50 h were taken to monitor the catalyst status. The XPS and TPR tests proved that the Au-S bond broke as the acetylene hydrochlorination reaction proceeded. The DFT calculation proved that the Au-S bond is the active site, and the sulfur atom promotes the adsorption of C₂H₂ by the catalyst.

关键词: Acetylene hydrochlorination, Au-S bond, Process monitoring, Valence shift

Lutai Song, Li Liu, Mingyuan Zhu, Bin Dai. Process monitoring of the Au-S bond conversion in acetylene hydrochlorination[J]. Chinese Journal of Chemical Engineering, 2022, 45(5): 32-40.

Lutai Song, Li Liu, Mingyuan Zhu, Bin Dai. Process monitoring of the Au-S bond conversion in acetylene hydrochlorination[J]. 中国化学工程学报, 2022, 45(5): 32-40.

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Process monitoring of the Au-S bond conversion in acetylene hydrochlorination

Process monitoring of the Au-S bond conversion in acetylene hydrochlorination

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