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A Planar,Conjugated N4-Macrocyclic Cobalt Complex for Heterogeneous Electrocatalytic CO2 Reduction with High Activity
Authors:Dr Libo Sun  Dr Zhenfeng Huang  Vikas Reddu  Prof Tan Su  Prof Adrian C Fisher  Prof Xin Wang
Institution:1. School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459 Singapore

Cambridge CARES, CREATE Tower, Singapore, 138602 Singapore;2. School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459 Singapore;3. Laboratory of Theoretical and Computational Chemistry, Institute of Theoretical Chemistry, Jilin University, Changchun, 130012 P. R. China;4. Cambridge CARES, CREATE Tower, Singapore, 138602 Singapore

Department of Chemical Engineering and Biotechnology, University of Cambridge, Cambridge, CB2 3RA UK

Abstract:Metal complexes have been widely investigated as promising electrocatalysts for CO2 reduction. Most of the current research efforts focus mainly on ligands based on pyrrole subunits, and the reported activities are still far from satisfactory. A novel planar and conjugated N4-macrocyclic cobalt complex (Co(II)CPY) derived from phenanthroline subunits is prepared herein, and it delivers high activity for heterogeneous CO2 electrocatalysis to CO in aqueous media, and outperforms most of the metal complexes reported so far. At a molar loading of 5.93×10−8 mol cm−2, it exhibits a Faradaic efficiency of 96 % and a turnover frequency of 9.59 s−1 towards CO at −0.70 V vs. RHE. The unraveling of electronic structural features suggests that a synergistic effect between the ligand and cobalt in Co(II)CPY plays a critical role in boosting its activity. As a result, the free energy difference for the formation of *COOH is lower than that with cobalt porphyrin, thus leading to enhanced CO production.
Keywords:CO2 reduction  cobalt  electrocatalysis  heterogeneous catalysis  macrocycles
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