Kinetics insights into size effects of carbon nanotubes’ growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

doi:10.1016/j.cjche.2024.05.012

中国化学工程学报 ›› 2024, Vol. 72 ›› Issue (8): 133-140.DOI: 10.1016/j.cjche.2024.05.012

Kinetics insights into size effects of carbon nanotubes’ growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

Yan Zhang, Xiangxue Zhang, Keng Sang, Wenyao Chen, Gang Qian, Jing Zhang, Xuezhi Duan, Xinggui Zhou, Weikang Yuan

State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

收稿日期:2024-02-24 修回日期:2024-05-16 出版日期:2024-08-28 发布日期:2024-10-17
通讯作者: Wenyao Chen,E-mail:wenyao.chen@ecust.edu.cn;Xuezhi Duan,E-mail:xzduan@ecust.edu.cn
基金资助:
This work was financially supported by the National Key Research and Development Program of China (2022YFA1503504), the National Natural Science Foundation of China (22038003, 22178100, 22178101, and U22B20141), the Shanghai Pilot Program for Basic Research (22TQ1400100-15), the Innovation Program of Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (21XD1421000), the Shanghai Science and Technology Innovation Action Plan (22JC1403800).

Kinetics insights into size effects of carbon nanotubes’ growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

Yan Zhang, Xiangxue Zhang, Keng Sang, Wenyao Chen, Gang Qian, Jing Zhang, Xuezhi Duan, Xinggui Zhou, Weikang Yuan

State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2024-02-24 Revised:2024-05-16 Online:2024-08-28 Published:2024-10-17
Contact: Wenyao Chen,E-mail:wenyao.chen@ecust.edu.cn;Xuezhi Duan,E-mail:xzduan@ecust.edu.cn
Supported by:
This work was financially supported by the National Key Research and Development Program of China (2022YFA1503504), the National Natural Science Foundation of China (22038003, 22178100, 22178101, and U22B20141), the Shanghai Pilot Program for Basic Research (22TQ1400100-15), the Innovation Program of Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (21XD1421000), the Shanghai Science and Technology Innovation Action Plan (22JC1403800).

摘要/Abstract

摘要： Size effects are a well-documented phenomenon in heterogeneous catalysis, typically attributed to alterations in geometric and electronic properties. In this study, we investigate the influence of catalyst size in the preparation of carbon nanotube (CNT) and the hydrogenation of 4,6-dinitroresorcinol (DNR) using Fe₂O₃ and Pt catalysts, respectively. Various Fe₂O₃/Al₂O₃ catalysts were synthesized for CNT growth through catalytic chemical vapor deposition. Our findings reveal a significant influence of Fe₂O₃ nanoparticle size on the structure and yield of CNT. Specifically, CNT produced with Fe₂O₃/Al₂O₃ containing 28% (mass) Fe loading exhibits abundant surface defects, an increased area for metal-particle immobilization, and a high carbon yield. This makes it a promising candidate for DNR hydrogenation. Utilizing this catalyst support, we further investigate the size effects of Pt nanoparticles on DNR hydrogenation. Larger Pt catalysts demonstrate a preference for 4,6-diaminoresorcinol generation at (1 0 0) sites, whereas smaller Pt catalysts are more susceptible to electronic properties. The kinetics insights obtained from this study have the potential to pave the way for the development of more efficient catalysts for both CNT synthesis and DNR hydrogenation.

关键词: Kinetics, Size effects, Catalytic hydrogenation, Active site

Abstract: Size effects are a well-documented phenomenon in heterogeneous catalysis, typically attributed to alterations in geometric and electronic properties. In this study, we investigate the influence of catalyst size in the preparation of carbon nanotube (CNT) and the hydrogenation of 4,6-dinitroresorcinol (DNR) using Fe₂O₃ and Pt catalysts, respectively. Various Fe₂O₃/Al₂O₃ catalysts were synthesized for CNT growth through catalytic chemical vapor deposition. Our findings reveal a significant influence of Fe₂O₃ nanoparticle size on the structure and yield of CNT. Specifically, CNT produced with Fe₂O₃/Al₂O₃ containing 28% (mass) Fe loading exhibits abundant surface defects, an increased area for metal-particle immobilization, and a high carbon yield. This makes it a promising candidate for DNR hydrogenation. Utilizing this catalyst support, we further investigate the size effects of Pt nanoparticles on DNR hydrogenation. Larger Pt catalysts demonstrate a preference for 4,6-diaminoresorcinol generation at (1 0 0) sites, whereas smaller Pt catalysts are more susceptible to electronic properties. The kinetics insights obtained from this study have the potential to pave the way for the development of more efficient catalysts for both CNT synthesis and DNR hydrogenation.

Key words: Kinetics, Size effects, Catalytic hydrogenation, Active site

Yan Zhang, Xiangxue Zhang, Keng Sang, Wenyao Chen, Gang Qian, Jing Zhang, Xuezhi Duan, Xinggui Zhou, Weikang Yuan. Kinetics insights into size effects of carbon nanotubes’ growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation[J]. 中国化学工程学报, 2024, 72(8): 133-140.

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Kinetics insights into size effects of carbon nanotubes’ growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

Kinetics insights into size effects of carbon nanotubes’ growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

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