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

Chao Wang, Yuzhuo Chen, Daijian Su, Wai-Lun Man, Kai-Chung Lau, Lianhuan Han*, Liubin Zhao*, Dongping Zhan*, Xunjin Zhu*

*Corresponding author for this work

Research output: Contribution to journalJournal articlepeer-review

7 Citations (Scopus)

Abstract

Electrocatalytic 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.
Original languageEnglish
Article number2303179
Number of pages8
JournalAdvanced Materials
Volume35
Issue number38
Early online date12 Jun 2023
DOIs
Publication statusPublished - 21 Sept 2023

Scopus Subject Areas

  • Mechanics of Materials
  • Mechanical Engineering
  • Materials Science(all)

User-Defined Keywords

  • 3D microporous polymer nanofilms
  • cobalt porphyrin
  • electrocatalytic CO2 reduction
  • electropolymerization

Fingerprint

Dive into the research topics of 'In situ Electropolymerized 3D Microporous Cobalt-Porphyrin Nanofilm for Highly Effective Molecular Electrocatalytic Reduction of Carbon Dioxide'. Together they form a unique fingerprint.

Cite this