Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols

doi:10.1016/j.cjche.2023.09.011

中国化学工程学报 ›› 2024, Vol. 66 ›› Issue (2): 157-166.DOI: 10.1016/j.cjche.2023.09.011

• Full Length Article • 上一篇下一篇

Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols

Zhihao Guo, Jiuxuan Zhang, Lanlan Chen, Chaoqun Fan, Hong Jiang, Rizhi Chen

State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China

收稿日期:2023-07-19 修回日期:2023-09-21 出版日期:2024-02-28 发布日期:2024-04-20
通讯作者: Hong Jiang,E-mail:hjiang@njtech.edu.cn
基金资助:
The financial support from the National Key Research and Development Program (2021YFC3001103), the National Natural Science Foundation (22278209, 22178165, 21921006, and 22208149), the Natural Science Foundation of Jiangsu Province (BK20211262 and BK20220354), and a project funded by the priority academic program development of Jiangsu higher education institutions (PAPD) of China.

Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols

Zhihao Guo, Jiuxuan Zhang, Lanlan Chen, Chaoqun Fan, Hong Jiang, Rizhi Chen

State Key Laboratory of Materials-Oriented Chemical Engineering, Nanjing Tech University, Nanjing 211816, China

Received:2023-07-19 Revised:2023-09-21 Online:2024-02-28 Published:2024-04-20
Contact: Hong Jiang,E-mail:hjiang@njtech.edu.cn
Supported by:
The financial support from the National Key Research and Development Program (2021YFC3001103), the National Natural Science Foundation (22278209, 22178165, 21921006, and 22208149), the Natural Science Foundation of Jiangsu Province (BK20211262 and BK20220354), and a project funded by the priority academic program development of Jiangsu higher education institutions (PAPD) of China.

摘要/Abstract

摘要： The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability, environmental friendliness, and non-toxicity is of great importance. Herein, a series of Co-based catalysts, named Co@NCNTs, were designed and constructed by direct pyrolysis of hollow ZIF-67 (HZIF-67) under H₂/Ar atmosphere. The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes (NCNTs) with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature. Due to the synergistic effects of in situ-formed hollow NCNTs, well-dispersed Co nanoparticles, and intact carbon matrix, the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols. The turnover frequencyvalue of Co@NCNTs-0.10-450 is 3.52h^-1, 5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550, exceeding most previously reported non-noble metal catalysts. Our findings provide new insights into the development of non-precious metal, efficient, and cost-effective metal–organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.

关键词: Phenolic compounds, Hollow ZIF-67 pyrolysis, Nitrogen-doped carbon nanotubes, Reduction, Multiphase reaction, Catalysis

Abstract: The selective hydrogenation of highly toxic phenolic compounds to generate alcohols with thermal stability, environmental friendliness, and non-toxicity is of great importance. Herein, a series of Co-based catalysts, named Co@NCNTs, were designed and constructed by direct pyrolysis of hollow ZIF-67 (HZIF-67) under H₂/Ar atmosphere. The evolution of the catalyst surface from the shell layer assembled by ZIF-67-derived particles to the in situ-grown hollow nitrogen-doped carbon nanotubes (NCNTs) with certain length and density is achieved by adjusting the pyrolysis atmosphere and temperature. Due to the synergistic effects of in situ-formed hollow NCNTs, well-dispersed Co nanoparticles, and intact carbon matrix, the as-prepared Co@NCNTs-0.10-450 catalyst exhibits superior catalytic performance in the hydrogenation of phenolic compounds to alcohols. The turnover frequencyvalue of Co@NCNTs-0.10-450 is 3.52h^-1, 5.9 times higher than that of Co@NCNTs-0.40-450 and 4.5 times higher than that of Co@NCNTs-0.10-550, exceeding most previously reported non-noble metal catalysts. Our findings provide new insights into the development of non-precious metal, efficient, and cost-effective metal–organic framework-derived catalysts for the hydrogenation of phenolic compounds to alcohols.

Key words: Phenolic compounds, Hollow ZIF-67 pyrolysis, Nitrogen-doped carbon nanotubes, Reduction, Multiphase reaction, Catalysis

Zhihao Guo, Jiuxuan Zhang, Lanlan Chen, Chaoqun Fan, Hong Jiang, Rizhi Chen. Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols[J]. 中国化学工程学报, 2024, 66(2): 157-166.

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Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols

Hollow ZIF-67-derived Co@N-doped carbon nanotubes boosting the hydrogenation of phenolic compounds to alcohols

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