High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite

doi:10.1016/j.cjche.2022.08.017

中国化学工程学报 ›› 2023, Vol. 57 ›› Issue (5): 98-108.DOI: 10.1016/j.cjche.2022.08.017

• Full Length Article • 上一篇下一篇

High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite

Chenyang Zhao, Yinhan Cheng, Guangfei Qu, Yongheng Yuan, Fenghui Wu, Ye Liu, Shan Liu, Junyan Li, Ping Ning

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China;National-Regional Engineering Research Center for Recovery of Waste Gases from Metallurgical and Chemical Industries-NCW, Kunming 650500, China

收稿日期:2022-05-15 修回日期:2022-08-13 出版日期:2023-05-28 发布日期:2023-07-08
通讯作者: Guangfei Qu,E-mail:qgflab@sina.com
基金资助:
This work is supported by the National Key Research and Development Plan (2018YFC1900203); The National Science Fund for Distinguished Young Scholars (52000094); The National Natural Science Foundation of China (51968033).

High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite

Chenyang Zhao, Yinhan Cheng, Guangfei Qu, Yongheng Yuan, Fenghui Wu, Ye Liu, Shan Liu, Junyan Li, Ping Ning

Faculty of Environmental Science and Engineering, Kunming University of Science and Technology, Kunming 650500, China;National-Regional Engineering Research Center for Recovery of Waste Gases from Metallurgical and Chemical Industries-NCW, Kunming 650500, China

Received:2022-05-15 Revised:2022-08-13 Online:2023-05-28 Published:2023-07-08
Contact: Guangfei Qu,E-mail:qgflab@sina.com
Supported by:
This work is supported by the National Key Research and Development Plan (2018YFC1900203); The National Science Fund for Distinguished Young Scholars (52000094); The National Natural Science Foundation of China (51968033).

摘要/Abstract

摘要： Pd/Cu liquid-phase composite was utilized as the catalyst in this study to remove PH₃ at low temperatures. The anti-heterotoxicity of catalysts in the PH₃ catalytic oxidation purification process was carefully explored and pioneered. The catalytic performance, thermodynamics, kinetics, and catalytic oxidation mechanism of Pd/Cu liquid-phase catalyst catalytic oxidation of PH₃ were thoroughly investigated. The results showed that Pd/Cu has a superior catalytic effect on the removal of PH₃ in the gas mixture under low temperature. With CO as the carrier gas, the removal efficiency of PH₃ could be maintained at 100% for nearly 450 min, indicating that the Pd/Cu liquid phase catalyst has good resistance to heterotoxicity. According to the thermodynamic, kinetic, and related characterization results of the PH₃ purification process, the kinetic region of the gas–liquid reaction of PH₃ absorption by Pd/Cu solution was an interfacial reaction. Pd was the primary catalyst and Cu was the secondary catalyst, and the adsorption of PH₃ was a primary reaction. PH₃ was spontaneously oxidized to H₃PO₄ in the Pd/Cu catalytic system during the removal process. Pd was regenerated by O₂ and Cu, increasing the activity and stability of the Pd/Cu catalyst in the sustain and efficient purification of PH₃ in tail gas.

关键词: Liquid-phase catalysis, Phosphine, Catalytic oxidation, Kinetic analysis, Transition metals

Abstract: Pd/Cu liquid-phase composite was utilized as the catalyst in this study to remove PH₃ at low temperatures. The anti-heterotoxicity of catalysts in the PH₃ catalytic oxidation purification process was carefully explored and pioneered. The catalytic performance, thermodynamics, kinetics, and catalytic oxidation mechanism of Pd/Cu liquid-phase catalyst catalytic oxidation of PH₃ were thoroughly investigated. The results showed that Pd/Cu has a superior catalytic effect on the removal of PH₃ in the gas mixture under low temperature. With CO as the carrier gas, the removal efficiency of PH₃ could be maintained at 100% for nearly 450 min, indicating that the Pd/Cu liquid phase catalyst has good resistance to heterotoxicity. According to the thermodynamic, kinetic, and related characterization results of the PH₃ purification process, the kinetic region of the gas–liquid reaction of PH₃ absorption by Pd/Cu solution was an interfacial reaction. Pd was the primary catalyst and Cu was the secondary catalyst, and the adsorption of PH₃ was a primary reaction. PH₃ was spontaneously oxidized to H₃PO₄ in the Pd/Cu catalytic system during the removal process. Pd was regenerated by O₂ and Cu, increasing the activity and stability of the Pd/Cu catalyst in the sustain and efficient purification of PH₃ in tail gas.

Key words: Liquid-phase catalysis, Phosphine, Catalytic oxidation, Kinetic analysis, Transition metals

Chenyang Zhao, Yinhan Cheng, Guangfei Qu, Yongheng Yuan, Fenghui Wu, Ye Liu, Shan Liu, Junyan Li, Ping Ning. High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite[J]. 中国化学工程学报, 2023, 57(5): 98-108.

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High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite

High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite

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