Rational design of nitrogen-doped carbon for palladium catalysts in hydrogenation of hydrazo compounds

doi:10.1016/j.cjche.2024.09.023

中国化学工程学报 ›› 2025, Vol. 77 ›› Issue (1): 156-166.DOI: 10.1016/j.cjche.2024.09.023

Rational design of nitrogen-doped carbon for palladium catalysts in hydrogenation of hydrazo compounds

Junzhe Xu¹, Shuang Liu¹, Lin Li², Xian Qin¹, Ruixin Qu¹, Jinguo Wang¹, Di Liu³, Gaixia Wei⁴

1. School of Chemistry and Chemical Engineering, Shanghai University of Engineering Science, Shanghai 201620, China;
2. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
3. Samsung (China) Semiconductor CO., LTD, Xi'an 710075, China;
4. Qingyang Chemical Industry Corporation, Liaoyang 111001, China

收稿日期:2024-05-02 修回日期:2024-08-31 接受日期:2024-09-01 出版日期:2025-01-28 发布日期:2024-11-05
通讯作者: Shuang Liu,E-mail:liushuang-cc@126.com;Lin Li,E-mail:llin@dicp.ac.cn
基金资助:
This work is financially supported by the National Natural Science Foundation of China (21503264, 22179081 and 22076117), and Natural Science Foundation of Shanghai (20ZR1422500).

Rational design of nitrogen-doped carbon for palladium catalysts in hydrogenation of hydrazo compounds

Junzhe Xu¹, Shuang Liu¹, Lin Li², Xian Qin¹, Ruixin Qu¹, Jinguo Wang¹, Di Liu³, Gaixia Wei⁴

1. School of Chemistry and Chemical Engineering, Shanghai University of Engineering Science, Shanghai 201620, China;
2. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China;
3. Samsung (China) Semiconductor CO., LTD, Xi'an 710075, China;
4. Qingyang Chemical Industry Corporation, Liaoyang 111001, China

Received:2024-05-02 Revised:2024-08-31 Accepted:2024-09-01 Online:2025-01-28 Published:2024-11-05
Contact: Shuang Liu,E-mail:liushuang-cc@126.com;Lin Li,E-mail:llin@dicp.ac.cn
Supported by:
This work is financially supported by the National Natural Science Foundation of China (21503264, 22179081 and 22076117), and Natural Science Foundation of Shanghai (20ZR1422500).

摘要/Abstract

摘要： We synthesized CN11, a carbon nitride material rich in sp³ hybrid graphitic nitrogen (sp³-N), employing a facile oxalic acid-assisted melamine molecular assembly strategy. CN11 promoted the formation of Pd nanoparticles (NPs) predominantly exposing {2 0 0} facets, termed Pd/CN11-2. This facet-specific configuration significantly boosted hydrogen adsorption, leading to notable improvements in catalytic activity. Compared to Pd/XC-72-2 and Pd/g-C₃N₄-2, Pd/CN11-2 exhibited a remarkable two-fold and nineteen-fold increase in catalytic yield for hydrazo compound hydrogenation, respectively. Pd/CN11-2 also demonstrated robust performance across a range of reaction conditions, maintaining excellent yield. This study emphasizes the critical role of tailored support structures in controlling Pd NPs facets, thereby enhancing hydrogenation efficiency. It provides valuable insights for advancing the industrial application of Pd-based catalysts, underscoring the importance of strategic support modulation for optimizing catalytic performance.

关键词: Pd nanocatalyst, Nitrogen-doped carbon, Hydrogenation, Deprotection of CBz, Bimethylation of amino

Abstract: We synthesized CN11, a carbon nitride material rich in sp³ hybrid graphitic nitrogen (sp³-N), employing a facile oxalic acid-assisted melamine molecular assembly strategy. CN11 promoted the formation of Pd nanoparticles (NPs) predominantly exposing {2 0 0} facets, termed Pd/CN11-2. This facet-specific configuration significantly boosted hydrogen adsorption, leading to notable improvements in catalytic activity. Compared to Pd/XC-72-2 and Pd/g-C₃N₄-2, Pd/CN11-2 exhibited a remarkable two-fold and nineteen-fold increase in catalytic yield for hydrazo compound hydrogenation, respectively. Pd/CN11-2 also demonstrated robust performance across a range of reaction conditions, maintaining excellent yield. This study emphasizes the critical role of tailored support structures in controlling Pd NPs facets, thereby enhancing hydrogenation efficiency. It provides valuable insights for advancing the industrial application of Pd-based catalysts, underscoring the importance of strategic support modulation for optimizing catalytic performance.

Key words: Pd nanocatalyst, Nitrogen-doped carbon, Hydrogenation, Deprotection of CBz, Bimethylation of amino

Junzhe Xu, Shuang Liu, Lin Li, Xian Qin, Ruixin Qu, Jinguo Wang, Di Liu, Gaixia Wei. Rational design of nitrogen-doped carbon for palladium catalysts in hydrogenation of hydrazo compounds[J]. 中国化学工程学报, 2025, 77(1): 156-166.

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Rational design of nitrogen-doped carbon for palladium catalysts in hydrogenation of hydrazo compounds

Rational design of nitrogen-doped carbon for palladium catalysts in hydrogenation of hydrazo compounds

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