Synergistic Catalysis over Iron‐Nitrogen Sites Anchored with Cobalt Phthalocyanine for Efficient CO2 Electroreduction. Issue 41 (22nd August 2019)

• Record Type: Journal Article
• Authors: Lin, Long; Li, Haobo; Yan, Chengcheng; Li, Hefei; Si, Rui; Li, Mingrun; Xiao, Jianping; Wang, Guoxiong; Bao, Xinhe
• Is Part Of: Advanced materials. Volume 31:Issue 41(2019)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2019-08-22
• Subjects: carbon dioxide electroreduction -- cobalt phthalocyanine -- iron‐nitrogen site -- synergistic catalysis; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adma.201903470
• Languages: English
• ISSNs: 0935-9648

Abstract

Abstract: Simultaneously achieving high Faradaic efficiency, current density, and stability at low overpotentials is essential for industrial applications of electrochemical CO2 reduction reaction (CO2 RR). However, great challenges still remain in this catalytic process. Herein, a synergistic catalysis strategy is presented to improve CO2 RR performance by anchoring Fe‐N sites with cobalt phthalocyanine (denoted as CoPc©Fe‐N‐C). The potential window of CO Faradaic efficiency above 90% is significantly broadened from 0.18 V over Fe‐N‐C alone to 0.71 V over CoPc©Fe‐N‐C while the onset potential of CO2 RR over both catalysts is as low as −0.13 V versus reversible hydrogen electrode. What is more, the maximum CO current density is increased ten times with significantly enhanced stability. Density functional theory calculations suggest that anchored cobalt phthalocyanine promotes the CO desorption and suppresses the competitive hydrogen evolution reaction over Fe‐N sites, while the *COOH formation remains almost unchanged, thus demonstrating unprecedented synergistic effect toward CO2 RR. Abstract : Compared with Fe–N–C and CoPc©Zn–N–C, CoPc©Fe–N–C shows a 10‐ and 2.5‐fold increase in the maximum CO current density with a low onset potential, a wide potential window of CO Faradaic efficiency above 90% and significantly enhanced stability. The anchored CoPc promotes CO desorption and suppresses the competitive hydrogen evolution reaction over Fe–N sites, demonstrating an unprecedented synergistic effect toward CO2 electroreduction.