Highly efficient cleavage of CO bonds in diphenyl ether over Ni-S2O82-/ZrO2 solid super acid catalysts

doi:10.1016/j.cjche.2025.08.010

Chinese Journal of Chemical Engineering ›› 2025, Vol. 86 ›› Issue (10): 34-44.DOI: 10.1016/j.cjche.2025.08.010

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Highly efficient cleavage of CO bonds in diphenyl ether over Ni-S₂O₈^2-/ZrO₂ solid super acid catalysts

Xiaoyan Zhao¹, Xin Hu¹, Chuang Zhang¹, Wei Jiang¹, Jingpei Cao^1,2,3, Zuxing Huan¹, Yue Wang¹, Changrui Tan¹

1. Jiangsu Province Engineering Research Center of Fine Utilization of Carbon Resources, China University of Mining & Technology, Xuzhou 221116, China;
2. Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization, China University of Mining and Technology, Xuzhou 221008, China;
3. Carbon Neutrality Institute, China University of Mining and Technology, Xuzhou 221008, China

Received:2025-02-20 Revised:2025-08-25 Accepted:2025-08-26 Online:2025-10-06 Published:2025-10-28
Contact: Xiaoyan Zhao,E-mail:zhaoxiaoyan@cumt.edu.cn;Jingpei Cao,E-mail:caojingpei@cumt.edu.cn
Supported by:
This work was supported by the National Key Research and Development Program of China (2022YFB4101100), the National Natural Science Foundation of China (22178375 and 22478414) and the Priority Academic Program Development of Jiangsu Higher Education Institutions.

Highly efficient cleavage of CO bonds in diphenyl ether over Ni-S₂O₈^2-/ZrO₂ solid super acid catalysts

Xiaoyan Zhao¹, Xin Hu¹, Chuang Zhang¹, Wei Jiang¹, Jingpei Cao^1,2,3, Zuxing Huan¹, Yue Wang¹, Changrui Tan¹

1. Jiangsu Province Engineering Research Center of Fine Utilization of Carbon Resources, China University of Mining & Technology, Xuzhou 221116, China;
2. Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization, China University of Mining and Technology, Xuzhou 221008, China;
3. Carbon Neutrality Institute, China University of Mining and Technology, Xuzhou 221008, China

通讯作者: Xiaoyan Zhao,E-mail:zhaoxiaoyan@cumt.edu.cn;Jingpei Cao,E-mail:caojingpei@cumt.edu.cn
基金资助:
This work was supported by the National Key Research and Development Program of China (2022YFB4101100), the National Natural Science Foundation of China (22178375 and 22478414) and the Priority Academic Program Development of Jiangsu Higher Education Institutions.

Abstract

Abstract: Catalytic aryl ether CO bonds hydrogenolysis was an important route to convert lignite into high value-added chemicals. Solid super acid 10% Ni-S₂O₈^2-/ZrO₂ catalysts were successfully synthesized and evaluated their performance in catalytic hydrolysis of lignite derivatives. The excellent performance of 10% Ni-S₂O₈^2-/ZrO₂ stems from the synergistic interaction between metallic and acidic sites. Specifically, the acidic sites generated by S2O2-8 facilitate the adsorption of O atoms in the substrate, whereas the metal sites optimize the process of hydrogen adsorption and activation and promote the generation of hydrogen radicals, which further enhances the ability to break C—O bonds. Thus, 10% Ni-S₂O₈^2-/ZrO₂ exhibits more significant catalytic activity compared to 10% Ni-ZrO₂ prepared from pure ZrO₂ as a support. Characterization results showed that the 10% Ni-S₂O₈^2-/ZrO₂ catalyst prepared by sodium borohydride reduction method presented a uniform pore structure, which effectively promoted the dispersion of metal Ni on the catalyst surface. Complete conversion of diphenyl ether (DPE) can be achieved under relatively mild conditions, and excellent hydrogenolysis activity is also demonstrated for other lignite derivatives containing C—O bonds. The possible reaction mechanism of DPE hydrogenolysis in the H₂-isopropanol system was investigated. This work represents a significant step forward in the design of highly efficient solid super acid catalysts.

Key words: Hydrogenation, Diphenyl ether, C—O cleavage, Chemical reaction, Ni-S₂O₈^2-/ZrO₂, Catalyst

摘要： Catalytic aryl ether CO bonds hydrogenolysis was an important route to convert lignite into high value-added chemicals. Solid super acid 10% Ni-S₂O₈^2-/ZrO₂ catalysts were successfully synthesized and evaluated their performance in catalytic hydrolysis of lignite derivatives. The excellent performance of 10% Ni-S₂O₈^2-/ZrO₂ stems from the synergistic interaction between metallic and acidic sites. Specifically, the acidic sites generated by S2O2-8 facilitate the adsorption of O atoms in the substrate, whereas the metal sites optimize the process of hydrogen adsorption and activation and promote the generation of hydrogen radicals, which further enhances the ability to break C—O bonds. Thus, 10% Ni-S₂O₈^2-/ZrO₂ exhibits more significant catalytic activity compared to 10% Ni-ZrO₂ prepared from pure ZrO₂ as a support. Characterization results showed that the 10% Ni-S₂O₈^2-/ZrO₂ catalyst prepared by sodium borohydride reduction method presented a uniform pore structure, which effectively promoted the dispersion of metal Ni on the catalyst surface. Complete conversion of diphenyl ether (DPE) can be achieved under relatively mild conditions, and excellent hydrogenolysis activity is also demonstrated for other lignite derivatives containing C—O bonds. The possible reaction mechanism of DPE hydrogenolysis in the H₂-isopropanol system was investigated. This work represents a significant step forward in the design of highly efficient solid super acid catalysts.

关键词: Hydrogenation, Diphenyl ether, C—O cleavage, Chemical reaction, Ni-S₂O₈^2-/ZrO₂, Catalyst

Xiaoyan Zhao, Xin Hu, Chuang Zhang, Wei Jiang, Jingpei Cao, Zuxing Huan, Yue Wang, Changrui Tan. Highly efficient cleavage of CO bonds in diphenyl ether over Ni-S₂O₈^2-/ZrO₂ solid super acid catalysts[J]. Chinese Journal of Chemical Engineering, 2025, 86(10): 34-44.

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Highly efficient cleavage of CO bonds in diphenyl ether over Ni-S₂O₈^2-/ZrO₂ solid super acid catalysts

Highly efficient cleavage of CO bonds in diphenyl ether over Ni-S₂O₈^2-/ZrO₂ solid super acid catalysts

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