Phosphorus and nitrogen co-doped graphene for catalytic dehydrochlorination of 1,2-dichloroethane

doi:10.1016/j.cjche.2023.05.012

中国化学工程学报 ›› 2023, Vol. 64 ›› Issue (12): 149-155.DOI: 10.1016/j.cjche.2023.05.012

• Full Length Article • 上一篇下一篇

Phosphorus and nitrogen co-doped graphene for catalytic dehydrochlorination of 1,2-dichloroethane

Haonan Yu^1,2, Xiaofeng Yang¹, Hongbin Yang¹, Jinming Xu¹, Yanqiang Huang¹

1. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
2. University of Chinese Academy of Sciences, Beijing 100049, China

收稿日期:2023-03-25 修回日期:2023-05-24 出版日期:2023-12-28 发布日期:2024-02-05
通讯作者: Jinming Xu,E-mail:xujm@dicp.ac.cn;Yanqiang Huang,E-mail:yqhuang@dicp.ac.cn
基金资助:
This work is financially supported by the Chinese Academy of Sciences Project for Young Scientists in Basic Research, China (YSBR-022), the National Natural Science Foundation of China, China (21925803), and the Youth Innovation Promotion Association CAS, China.

Phosphorus and nitrogen co-doped graphene for catalytic dehydrochlorination of 1,2-dichloroethane

Haonan Yu^1,2, Xiaofeng Yang¹, Hongbin Yang¹, Jinming Xu¹, Yanqiang Huang¹

1. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
2. University of Chinese Academy of Sciences, Beijing 100049, China

Received:2023-03-25 Revised:2023-05-24 Online:2023-12-28 Published:2024-02-05
Contact: Jinming Xu,E-mail:xujm@dicp.ac.cn;Yanqiang Huang,E-mail:yqhuang@dicp.ac.cn
Supported by:
This work is financially supported by the Chinese Academy of Sciences Project for Young Scientists in Basic Research, China (YSBR-022), the National Natural Science Foundation of China, China (21925803), and the Youth Innovation Promotion Association CAS, China.

摘要/Abstract

摘要： A phosphorus and nitrogen co-doped graphene (PNG) was developed via a two-step pyrolysis approach through the intermedium of g-C₃N₄ template and glyphosate as the phosphorus source, and was used for the catalytic dehydrochlorination of 1,2-dichloroethane (EDC) to vinyl chloride monomer (VCM) production. The characterization results indicate that a volcano relationship of surface area and surface properties with the usage of phosphorus precursor was observed, and the sample of PNG-900-6 possesses not only the thin film structure with enhanced surface area but also the smaller grain size of PNG attachments. Accordingly, such PNGs show a great improvement of catalytic performance in the dehydrochlorination of EDC, and the PNG-900-6 catalyst behaves the best with a 4-times higher activity than that on the nitrogen doped graphene (NG). It was also proved that the synergetic effect of the unique P-C coordination on the graphene to generate more quaternary nitrogen species was crucial in determining the catalytic performance of EDC conversion. Our results demonstrate that the phosphorus and nitrogen co-doped graphene offers many advantages in physical structure and chemical property, and are also great potential on the catalytic application in the dehydrochlorination of 1,2-dichloroethane.

关键词: Catalysis, Nanomaterials, Fixed-bed, Dehydrochlorination, Doped graphene

Abstract: A phosphorus and nitrogen co-doped graphene (PNG) was developed via a two-step pyrolysis approach through the intermedium of g-C₃N₄ template and glyphosate as the phosphorus source, and was used for the catalytic dehydrochlorination of 1,2-dichloroethane (EDC) to vinyl chloride monomer (VCM) production. The characterization results indicate that a volcano relationship of surface area and surface properties with the usage of phosphorus precursor was observed, and the sample of PNG-900-6 possesses not only the thin film structure with enhanced surface area but also the smaller grain size of PNG attachments. Accordingly, such PNGs show a great improvement of catalytic performance in the dehydrochlorination of EDC, and the PNG-900-6 catalyst behaves the best with a 4-times higher activity than that on the nitrogen doped graphene (NG). It was also proved that the synergetic effect of the unique P-C coordination on the graphene to generate more quaternary nitrogen species was crucial in determining the catalytic performance of EDC conversion. Our results demonstrate that the phosphorus and nitrogen co-doped graphene offers many advantages in physical structure and chemical property, and are also great potential on the catalytic application in the dehydrochlorination of 1,2-dichloroethane.

Key words: Catalysis, Nanomaterials, Fixed-bed, Dehydrochlorination, Doped graphene

Haonan Yu, Xiaofeng Yang, Hongbin Yang, Jinming Xu, Yanqiang Huang. Phosphorus and nitrogen co-doped graphene for catalytic dehydrochlorination of 1,2-dichloroethane[J]. 中国化学工程学报, 2023, 64(12): 149-155.

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Phosphorus and nitrogen co-doped graphene for catalytic dehydrochlorination of 1,2-dichloroethane

Phosphorus and nitrogen co-doped graphene for catalytic dehydrochlorination of 1,2-dichloroethane

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