Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

doi:10.1016/j.cjche.2023.08.001

中国化学工程学报 ›› 2024, Vol. 65 ›› Issue (1): 19-28.DOI: 10.1016/j.cjche.2023.08.001

• Full Length Article • 上一篇下一篇

Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

Xiaojing Liu¹, Ruohan Zhao¹, Hao Zhao¹, Zhimiao Wang^1,2, Fang Li^1,2, Wei Xue^1,2, Yanji Wang^1,2,3

1 Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China;
2 Tianjin Key Laboratory of Chemical Process Safety, Tianjin 300130, China;
3 Hebei Industrial Technology Research Institute of Green Chemical Industry, Huanghua 061100, China

收稿日期:2023-05-10 修回日期:2023-07-27 出版日期:2024-01-28 发布日期:2024-04-17
通讯作者: Zhimiao Wang,Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China. E-mail:wangzhimiao@hebut.edu.cn;Fang Li,Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China. E-mail:lifang@hebut.edu.cn;Wei Xue,Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China. E-mail:weixue@hebut.edu.cn
基金资助:
Thanks for the support by the National Natural Science Foundation of China (U21A20306, U20A20152), and Natural Science Foundation of Hebei Province (B2022202077).

Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

Xiaojing Liu¹, Ruohan Zhao¹, Hao Zhao¹, Zhimiao Wang^1,2, Fang Li^1,2, Wei Xue^1,2, Yanji Wang^1,2,3

1 Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China;
2 Tianjin Key Laboratory of Chemical Process Safety, Tianjin 300130, China;
3 Hebei Industrial Technology Research Institute of Green Chemical Industry, Huanghua 061100, China

Received:2023-05-10 Revised:2023-07-27 Online:2024-01-28 Published:2024-04-17
Contact: Zhimiao Wang,Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China. E-mail:wangzhimiao@hebut.edu.cn;Fang Li,Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China. E-mail:lifang@hebut.edu.cn;Wei Xue,Hebei Provincial Key Laboratory of Green Chemical Technology and High Efficient Energy Saving, School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China. E-mail:weixue@hebut.edu.cn
Supported by:
Thanks for the support by the National Natural Science Foundation of China (U21A20306, U20A20152), and Natural Science Foundation of Hebei Province (B2022202077).

摘要/Abstract

摘要： Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry. Herein, a heterogeneous Pd catalyst (Pd/NCF) was prepared by supporting Pd ultrafine metal nanoparticles (NPs) on nitrogen-doped carbon;synthesized by using F127 as a stabilizer, as well as chitosan as a carbon and nitrogen source. The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate, exhibiting higher stability than Pd/NC prepared without F127 addition. The hydrogen bond between chitosan (CTS) and F127 was enhanced by F127, which anchored the N in the free amino group, increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs. This process helped to improve metal dispersion. The increased metal-support interaction, which limits the leaching and coarsening of Pd NPs, improves the stability of the Pd/NCF catalyst. Furthermore, density functional theory calculations indicated that pyridine N stabilized the Pd²⁺ species, significantly inhibiting the loss of Pd²⁺ in Pd/NCF during the reaction process. This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

关键词: Supported Pd catalyst, N-doped carbon, Amphiphilic triblock copolymer, Pyridinic nitrogen, Stability

Abstract: Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry. Herein, a heterogeneous Pd catalyst (Pd/NCF) was prepared by supporting Pd ultrafine metal nanoparticles (NPs) on nitrogen-doped carbon;synthesized by using F127 as a stabilizer, as well as chitosan as a carbon and nitrogen source. The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate, exhibiting higher stability than Pd/NC prepared without F127 addition. The hydrogen bond between chitosan (CTS) and F127 was enhanced by F127, which anchored the N in the free amino group, increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs. This process helped to improve metal dispersion. The increased metal-support interaction, which limits the leaching and coarsening of Pd NPs, improves the stability of the Pd/NCF catalyst. Furthermore, density functional theory calculations indicated that pyridine N stabilized the Pd²⁺ species, significantly inhibiting the loss of Pd²⁺ in Pd/NCF during the reaction process. This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

Key words: Supported Pd catalyst, N-doped carbon, Amphiphilic triblock copolymer, Pyridinic nitrogen, Stability

Xiaojing Liu, Ruohan Zhao, Hao Zhao, Zhimiao Wang, Fang Li, Wei Xue, Yanji Wang. Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol[J]. 中国化学工程学报, 2024, 65(1): 19-28.

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Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

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