Affiliation:
1. State Key Laboratory of Physical Chemistry of Solid Surfaces Fujian Science & Technology Innovation Laboratory for Energy Materials of China Engineering Research Center of Electrochemical Technologies of Ministry of Education Department of Chemistry College of Chemistry and Chemical Engineering Department of Mechanical and Electrical Engineering School of Aerospace Engineering Xiamen University Xiamen 361005 China
2. Department of Chemistry and State Key Laboratory of Environmental and Biological Analysis Hong Kong Baptist University Kowloon Tong Hong Kong China
3. Department of Chemistry School of Chemistry and Chemical Engineering Southwest University Chongqing 400715 China
4. Department of Chemistry City University of Hong Kong Kowloon Hong Kong China
5. Department of Chemistry College of Chemistry and Chemical Engineering Ningxia University Yinchuan 750021 China
Abstract
AbstractElectrocatalytic CO2 reduction reaction (CO2RR) based on molecular catalysts, for example, cobalt porphyrin, is promising to enhance the carbon cycle and mitigate current climate crisis. However, the electrocatalytic performance and accurate evaluations remain problems because of either the low loading amount or the low utilization rate of the electroactive CoN4 sites. Herein a monomer is synthesized, cobalt(II)‐5,10,15,20‐tetrakis(3,5‐di(thiophen‐2‐yl)phenyl)porphyrin (CoP), electropolymerized onto carbon nanotubes (CNTs) networks, affording a molecular electrocatalyst of 3D microporous nanofilm (EP‐CoP, 2–3 nm thickness) with highly dispersed CoN4 sites. The new electrocatalyst shortens the electron transfer pathway, accelerates the redox kinetics of CoN4 sites, and improves the durability of the electrocatalytic CO2RR. From the intrinsic redox behavior of CoN4 sites, the effective utilization rate is obtained as 13.1%, much higher than that of the monomer assembled electrode (5.8%), and the durability is also promoted dramatically (>40 h) in H‐type cells. In commercial flow cells, EP‐CoP can achieve a faradic efficiency for CO (FECO) over 92% at an overpotential of 160 mV. At a higher overpotential of 620 mV, the working current density can reach 310 mA cm−2 with a high FECO of 98.6%, representing the best performance for electrodeposited molecular porphyrin electrocatalysts.
Funder
National Natural Science Foundation of China
Higher Education Discipline Innovation Project
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science
Cited by
4 articles.
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