Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide

doi:10.1016/j.cjche.2021.07.020

中国化学工程学报 ›› 2022, Vol. 43 ›› Issue (3): 192-201.DOI: 10.1016/j.cjche.2021.07.020

Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide

Mingdong Sun¹, Zhengyun Bian¹, Weiwei Cui¹, Xiaolong Zhao¹, Shu Dong¹, Xuebin Ke², Yu Zhou¹, Jun Wang¹

1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;
2. Department of Chemical Engineering, University of Hull, Hull HU6 7RX, United Kingdom

收稿日期:2021-03-11 修回日期:2021-06-13 出版日期:2022-03-28 发布日期:2022-04-28
通讯作者: Yu Zhou,E-mail:njutzhouyu@njtech.edu.cn;Jun Wang,E-mail:junwang@njtech.edu.cn
基金资助:
We gratefully acknowledge support from the National Natural Science Foundation of China (Nos. 22072065, U1662107, and 21476109), Six talent peaks project in Jiangsu Province (JNHB-035), State Key Laboratory of Materials-Oriented Chemical Engineering (KL17-04), Jiangsu Provincial Science Foundation for Youths (SBK2020044703), the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), High-Performance Computing Center of Nanjing Tech University for supporting the computational resources and the public service platform for the industrialization of innovative achievements in the field of industrial catalysis.

Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide

Mingdong Sun¹, Zhengyun Bian¹, Weiwei Cui¹, Xiaolong Zhao¹, Shu Dong¹, Xuebin Ke², Yu Zhou¹, Jun Wang¹

1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;
2. Department of Chemical Engineering, University of Hull, Hull HU6 7RX, United Kingdom

Received:2021-03-11 Revised:2021-06-13 Online:2022-03-28 Published:2022-04-28
Contact: Yu Zhou,E-mail:njutzhouyu@njtech.edu.cn;Jun Wang,E-mail:junwang@njtech.edu.cn
Supported by:
We gratefully acknowledge support from the National Natural Science Foundation of China (Nos. 22072065, U1662107, and 21476109), Six talent peaks project in Jiangsu Province (JNHB-035), State Key Laboratory of Materials-Oriented Chemical Engineering (KL17-04), Jiangsu Provincial Science Foundation for Youths (SBK2020044703), the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), High-Performance Computing Center of Nanjing Tech University for supporting the computational resources and the public service platform for the industrialization of innovative achievements in the field of industrial catalysis.

摘要/Abstract

摘要： Heteroatom-doped carbon materials have demonstrated great potential in the electrochemical reduction reaction of CO₂ (CO₂RR) due to their versatile structure and function. However, rational structure control remains one challenge. In this work, we reported a unique carbon precursor of soft template-containing porous poly(ionic liquid) (PIL) that was directly synthesized via free-radical self-polymerization of ionic liquid monomer in a soft template route. Variation of the carbonization temperature in a direct pyrolysis process without any additive yielded a series of carbon materials with facile adjustable textural properties and N species. Significantly, the integration of soft-template in the PIL precursor led to the formation of hierarchical porous carbon material with a higher surface area and larger pore size than that from the template-free precursor. In CO₂RR to CO, the champion catalyst gave a Faraday efficiency of 83.0% and a current density of 1.79 mA·cm^-2 at -0.9 V vs. reversible hydrogen electrode (vs. RHE). The abundant graphite N species and hierarchical pore structure, especially the unique hierarchical small-/ultra-micropores were revealed to enable better CO₂RR performance.

关键词: CO₂RR, Poly(ionic liquid), N-doped carbon materials, Pore diameter, Hierarchical pore

Abstract: Heteroatom-doped carbon materials have demonstrated great potential in the electrochemical reduction reaction of CO₂ (CO₂RR) due to their versatile structure and function. However, rational structure control remains one challenge. In this work, we reported a unique carbon precursor of soft template-containing porous poly(ionic liquid) (PIL) that was directly synthesized via free-radical self-polymerization of ionic liquid monomer in a soft template route. Variation of the carbonization temperature in a direct pyrolysis process without any additive yielded a series of carbon materials with facile adjustable textural properties and N species. Significantly, the integration of soft-template in the PIL precursor led to the formation of hierarchical porous carbon material with a higher surface area and larger pore size than that from the template-free precursor. In CO₂RR to CO, the champion catalyst gave a Faraday efficiency of 83.0% and a current density of 1.79 mA·cm^-2 at -0.9 V vs. reversible hydrogen electrode (vs. RHE). The abundant graphite N species and hierarchical pore structure, especially the unique hierarchical small-/ultra-micropores were revealed to enable better CO₂RR performance.

Key words: CO₂RR, Poly(ionic liquid), N-doped carbon materials, Pore diameter, Hierarchical pore

Mingdong Sun, Zhengyun Bian, Weiwei Cui, Xiaolong Zhao, Shu Dong, Xuebin Ke, Yu Zhou, Jun Wang. Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide[J]. 中国化学工程学报, 2022, 43(3): 192-201.

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Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide

Pyrolyzing soft template-containing poly(ionic liquid) into hierarchical N-doped porous carbon for electroreduction of carbon dioxide

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