Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO2

doi:10.1016/j.cjche.2022.05.030

Chinese Journal of Chemical Engineering ›› 2023, Vol. 55 ›› Issue (3): 212-221.DOI: 10.1016/j.cjche.2022.05.030

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Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO₂

Mingdong Sun¹, Dongxin Pan¹, Tingting Ye¹, Jing Gu², Yu Zhou¹, Jun Wang¹

1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;
2. School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, China

Received:2022-01-08 Revised:2022-05-28 Online:2023-06-03 Published:2023-03-28
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 ( 22072065, 22178162, U1662107, and 21476109), Six talent peaks project in Jiangsu Province (JNHB-035), State Key Laboratory of Materials-Oriented Chemical Engineering (KL18-09), and the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). The computational resources generously provided by the High-Performance Computing Center of Nanjing Tech University are greatly appreciated.

Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO₂

Mingdong Sun¹, Dongxin Pan¹, Tingting Ye¹, Jing Gu², Yu Zhou¹, Jun Wang¹

1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 210009, China;
2. School of Chemistry and Chemical Engineering, Anhui University of Technology, Maanshan 243002, China

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 ( 22072065, 22178162, U1662107, and 21476109), Six talent peaks project in Jiangsu Province (JNHB-035), State Key Laboratory of Materials-Oriented Chemical Engineering (KL18-09), and the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD). The computational resources generously provided by the High-Performance Computing Center of Nanjing Tech University are greatly appreciated.

Abstract

Abstract: Electrochemical CO₂ reduction reaction (CO₂RR) has attracted growing attention in energy storage and sustainable production of fuels and chemicals. N-doped carbon materials are preferred metal-free electrocatalysts, but it remains one challenge to finely engineer the active sites and porosity. Herein, we demonstrated that ionic porous polyamides were a kind of versatile precursors to prepare functional carbon materials in a one-step pyrolysis process. The polyamide precursors allowed the maintenance of abundant N species at high temperatures. The existence of ionic moieties and large specific surface area of the precursors promoted the formation of larger porosity carbon with a large specific surface area and sufficient active graphitic-N species by controlling the pyrolysis temperature. The catalyst was highly selective in the CO₂RR to produce CO with a maximum Faraday efficiency above 99%, attributable to the improved mass transfer in a large porosity system. This work shows that ionic polyamides are promising carbon precursors for the fabrication of metal-free electrocatalysts for CO₂RR.

Key words: Carbon dioxide, Electrochemistry, Reduction, Ionic mesoporous polyamide, N-doped carbon material

摘要： Electrochemical CO₂ reduction reaction (CO₂RR) has attracted growing attention in energy storage and sustainable production of fuels and chemicals. N-doped carbon materials are preferred metal-free electrocatalysts, but it remains one challenge to finely engineer the active sites and porosity. Herein, we demonstrated that ionic porous polyamides were a kind of versatile precursors to prepare functional carbon materials in a one-step pyrolysis process. The polyamide precursors allowed the maintenance of abundant N species at high temperatures. The existence of ionic moieties and large specific surface area of the precursors promoted the formation of larger porosity carbon with a large specific surface area and sufficient active graphitic-N species by controlling the pyrolysis temperature. The catalyst was highly selective in the CO₂RR to produce CO with a maximum Faraday efficiency above 99%, attributable to the improved mass transfer in a large porosity system. This work shows that ionic polyamides are promising carbon precursors for the fabrication of metal-free electrocatalysts for CO₂RR.

关键词: Carbon dioxide, Electrochemistry, Reduction, Ionic mesoporous polyamide, N-doped carbon material

Mingdong Sun, Dongxin Pan, Tingting Ye, Jing Gu, Yu Zhou, Jun Wang. Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO₂[J]. Chinese Journal of Chemical Engineering, 2023, 55(3): 212-221.

Mingdong Sun, Dongxin Pan, Tingting Ye, Jing Gu, Yu Zhou, Jun Wang. Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO₂[J]. 中国化学工程学报, 2023, 55(3): 212-221.

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Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO₂

Ionic porous polyamide derived N-doped carbon towards highly selective electroreduction of CO₂

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