SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2021, Vol. 39 ›› Issue (11): 144-153.DOI: 10.1016/j.cjche.2021.05.032

• Catalysis, Kinetics and Reaction Engineering • Previous Articles     Next Articles

Catalytic hydrogenation performance of ZIF-8 carbide for electrochemical reduction of carbon dioxide

Shuai Fan, Huiyuan Cheng, Manman Feng, Xuemei Wu, Zihao Fan, Dongwei Pan, Gaohong He   

  1. State Key Laboratory of Fine Chemicals, Research and Development Center of Membrane Science and Technology, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
  • Received:2020-11-18 Revised:2021-05-17 Online:2021-12-27 Published:2021-11-28
  • Contact: Xuemei Wu, Gaohong He
  • Supported by:
    This work was financially supported by the National Natural Science Foundation of China (Joint Fund U1663223 and 21776034), Science Fund for Creative Research Groups of the National Natural Science Foundation of China (22021005), the National Key Research and Development Program of China (2016YFB0101203), Educational Department of Liaoning Province of China (LT2015007), Fundamental Research Funds for the Central Universities (DUT16TD19) and the Changjiang Scholar Program (T2012049).

Catalytic hydrogenation performance of ZIF-8 carbide for electrochemical reduction of carbon dioxide

Shuai Fan, Huiyuan Cheng, Manman Feng, Xuemei Wu, Zihao Fan, Dongwei Pan, Gaohong He   

  1. State Key Laboratory of Fine Chemicals, Research and Development Center of Membrane Science and Technology, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
  • 通讯作者: Xuemei Wu, Gaohong He
  • 基金资助:
    This work was financially supported by the National Natural Science Foundation of China (Joint Fund U1663223 and 21776034), Science Fund for Creative Research Groups of the National Natural Science Foundation of China (22021005), the National Key Research and Development Program of China (2016YFB0101203), Educational Department of Liaoning Province of China (LT2015007), Fundamental Research Funds for the Central Universities (DUT16TD19) and the Changjiang Scholar Program (T2012049).

Abstract: The conversion of CO2 electrocatalytic hydrogenation into energy-rich fuel is considered to be the most effective way to carbon recycle. Nitrogen-doping carbonized ZIF-8 is proposed as carrier of the earth-rich Sn catalyst to overcome the limit of electron transfer and CO2 adsorption capacity of Sn. Hierarchically porous structure of Sn doped carbonized ZIF-8 is controlled by hydrothermal and carbonization conditions, which induces much higher specific surface area than that of the commercial Sn nanoparticle (1003.174 vs. 7.410 m2·g-1). The shift of nitrogen peaks in X-ray Photoelectron Spectroscopy spectra indicates interaction between ZIF-8 and Sn, which induces the shift of electron cloud from Sn to the chemical nitrogen to enhance conductivity and regulate electron transfer from catalyst to CO2. Lower mass transfer resistance and Warburg resistance are investigated through EIS, which significantly improves the catalytic activity for CO2 reduction reaction (CO2RR). Onset potential of the reaction is reduced from -0.74 V to less than -0.54 V vs. RHE. The total Faraday efficiency of HCOOH and CO reaches 68.9% at -1.14 V vs. RHE, which is much higher than that of the commercial Sn (45.0%) and some other Sn-based catalyst reported in the literature.

Key words: Carbon dioxide, Electrochemistry, Selective catalytic reduction, Electrochemical hydrogen pump, Nitrogen-doping carbonized ZIF-8

摘要: The conversion of CO2 electrocatalytic hydrogenation into energy-rich fuel is considered to be the most effective way to carbon recycle. Nitrogen-doping carbonized ZIF-8 is proposed as carrier of the earth-rich Sn catalyst to overcome the limit of electron transfer and CO2 adsorption capacity of Sn. Hierarchically porous structure of Sn doped carbonized ZIF-8 is controlled by hydrothermal and carbonization conditions, which induces much higher specific surface area than that of the commercial Sn nanoparticle (1003.174 vs. 7.410 m2·g-1). The shift of nitrogen peaks in X-ray Photoelectron Spectroscopy spectra indicates interaction between ZIF-8 and Sn, which induces the shift of electron cloud from Sn to the chemical nitrogen to enhance conductivity and regulate electron transfer from catalyst to CO2. Lower mass transfer resistance and Warburg resistance are investigated through EIS, which significantly improves the catalytic activity for CO2 reduction reaction (CO2RR). Onset potential of the reaction is reduced from -0.74 V to less than -0.54 V vs. RHE. The total Faraday efficiency of HCOOH and CO reaches 68.9% at -1.14 V vs. RHE, which is much higher than that of the commercial Sn (45.0%) and some other Sn-based catalyst reported in the literature.

关键词: Carbon dioxide, Electrochemistry, Selective catalytic reduction, Electrochemical hydrogen pump, Nitrogen-doping carbonized ZIF-8