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Free radicals induced ultra-rapid synthesis of N-doped carbon sphere catalyst with boosted pyrrolic N active sites for efficient acetylene hydrochlorination

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Abstract

Activated carbon-supported HgCl2 catalysts have seriously impeded the development of the polyvinyl chloride (PVC) industry due to the sublimation of Hg species and environmental pollution problems. Herein, the template-free and organic solvent-free strategy was devised to synthesize non-metallic based nitrogen-doped carbon (U-NC) sphere catalyst for acetylene hydrochlorination. This green strategy via ultrasonic chemistry initiates resin crosslinking reactions between aminophenol and formaldehyde resin by free radicals, leading to the ultra-rapid formation of U-NC with remarkably high pyrrolic N content in only 5 min. This U-NC catalyst exhibited an outstanding space-time-yield (1.6 gVCM·gcat−1·h−1), even comparable to the reported metallic catalyst. By combining kinetic analysis, advanced characterizations, and density functional theory, it is found that the amount of pyrrolic N is in linear with C2H2 conversion, and pyrrolic N in U-NC can effectively improve acetylene hydrochlorination performance by mediating HCl adsorption. This work sheds new light on rationally constructing metal-free catalyst for acetylene hydrochlorination.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 21978325), Innovation Research Projects (Nos. 20CX06072A, 20CX06095A, and 20CX06096A), the Natural Science Foundation of Shandong Province (Nos. ZR2020KB006 and ZR2020YQ17), and the Science and Technology Project of Xinjiang Bingtuan Supported by Central Government (No. 2022BC001).

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  1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China), Qingdao, 266580, China

    Yuxiang Bao, Xiuhui Zheng, Jianlin Cao, Yongxiao Tuo, Xiang Feng, Chaohe Yang & De Chen

  2. Department of Chemical Engineering, Norwegian University of Science and Technology, Trondheim, 7491, Norway

    De Chen

  3. School of Chemistry and Chemical Engineering of Shihezi University, Shihezi, 832000, China

    Bin Dai

  4. College of Chemistry & Chemical Engineering of Yantai University, Yantai, 264005, China

    Shuo Li & Mingyuan Zhu

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  1. Yuxiang Bao
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Free radicals induced ultra-rapid synthesis of N-doped carbon sphere catalyst with boosted pyrrolic N active sites for efficient acetylene hydrochlorination

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Bao, Y., Zheng, X., Cao, J. et al. Free radicals induced ultra-rapid synthesis of N-doped carbon sphere catalyst with boosted pyrrolic N active sites for efficient acetylene hydrochlorination. Nano Res. 16, 6178–6186 (2023). https://doi.org/10.1007/s12274-022-5237-y

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