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Enhancing CO 2 Reduction Efficiency on Cobalt Phthalocyanine via Axial Ligation

Title: Enhancing CO 2 Reduction Efficiency on Cobalt Phthalocyanine via Axial Ligation
Authors: Kang, Hongxing; Staples‐West, Aaliyah; Washington, Audrey; Turchiano, Chris; Cooksy, Andrew; Huang, Jier; Gu, Jing
Contributors: Division of Chemistry
Source: ChemCatChem ; volume 15, issue 14 ; ISSN 1867-3880 1867-3899
Publisher Information: Wiley
Publication Year: 2023
Collection: Wiley Online Library (Open Access Articles via Crossref)
Description: Electrochemical reduction of carbon dioxide (CO 2 RR) to value‐added products is a promising strategy to alleviate the greenhouse gas effect. Molecular catalysts, such as cobalt (II) phthalocyanine (CoPc), are known to be efficient electrocatalysts that are capable of converting CO 2 into carbon monoxide (CO). Herein, we report an axial modification strategy to enhance CoPc's CO 2 RR performance. After coordinating with axial ligands, the electron density of Co was depleted via π‐backbonding. This π‐backbonding weakened the Co‐CO bond, resulting in rapid desorption of CO. Also, the presence axial ligands elevated the Co dz 2 orbital energy, resulting in a significantly enhanced CO selectivity, evidenced by an increased faradaic efficiency (FE) from 82 % (CoPc) to 91 % and 94 % with the presence of pyridine (CoPc‐py) and imidizal ligands (CoPc‐im), respectively, at −0.82 V vs. RHE. Density functional theory calculations reveal that axial ligation of CoPc can reduce the energy barrier for CO 2 activation and facilitate the formation of * COOH.
Document Type: article in journal/newspaper
Language: English
DOI: 10.1002/cctc.202300576
Availability: https://doi.org/10.1002/cctc.202300576; https://chemistry-europe.onlinelibrary.wiley.com/doi/pdf/10.1002/cctc.202300576
Rights: http://creativecommons.org/licenses/by/4.0/ ; http://creativecommons.org/licenses/by/4.0/
Accession Number: edsbas.D344E715
Database: BASE