In situ Electropolymerized 3D Microporous Cobalt-Porphyrin Nanofilm for Highly Effective Molecular Electrocatalytic Reduction of Carbon Dioxide.

Autor:	Wang C; 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., Chen Y; Department of Chemistry and State Key Laboratory of Environmental and Biological Analysis, Hong Kong Baptist University, Kowloon Tong, Hong Kong, China., Su D; Department of Chemistry, School of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, China., Man WL; Department of Chemistry and State Key Laboratory of Environmental and Biological Analysis, Hong Kong Baptist University, Kowloon Tong, Hong Kong, China., Lau KC; Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong, China., Han L; 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., Zhao L; Department of Chemistry, School of Chemistry and Chemical Engineering, Southwest University, Chongqing, 400715, China., Zhan D; 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.; Department of Chemistry, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, 750021, China., Zhu X; Department of Chemistry and State Key Laboratory of Environmental and Biological Analysis, Hong Kong Baptist University, Kowloon Tong, Hong Kong, China.
Jazyk:	angličtina
Zdroj:	Advanced materials (Deerfield Beach, Fla.) [Adv Mater] 2023 Sep; Vol. 35 (38), pp. e2303179. Date of Electronic Publication: 2023 Jul 26.
DOI:	10.1002/adma.202303179
Abstrakt:	Electrocatalytic CO 2 reduction reaction (CO 2 RR) 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 CoN 4 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 CoN 4 sites. The new electrocatalyst shortens the electron transfer pathway, accelerates the redox kinetics of CoN 4 sites, and improves the durability of the electrocatalytic CO 2 RR. From the intrinsic redox behavior of CoN 4 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 (FE CO ) 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 FE CO of 98.6%, representing the best performance for electrodeposited molecular porphyrin electrocatalysts. (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)
Databáze:	MEDLINE
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