Phthalocyanine-derived catalysts decorated by metallic nanoclusters for enhanced CO2 electroreduction

Electrochemical CO2 reduction (CO2RR) over molecular catalysts is a paramount approach for CO2 conversion to CO. Herein, we report a novel phthalocyanine-derived catalyst synthesized by a two-step method with a much improved electroconductivity. Furthermore, the catalyst contains both Ni–N4 sites an...

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Bibliographic Details
Published in:Green energy & environment 2023-04, Vol.8 (2), p.444-451
Main Authors: Chen, Jiacheng, Li, Jiayu, Xu, Jing, Zhu, Minghui, Han, Yi-Fan
Format: Article
Language:English
Subjects:
Carbon dioxide
Electroreduction
Hybrid catalyst
Mechanism
Nickel-based catalysts
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Summary:Electrochemical CO2 reduction (CO2RR) over molecular catalysts is a paramount approach for CO2 conversion to CO. Herein, we report a novel phthalocyanine-derived catalyst synthesized by a two-step method with a much improved electroconductivity. Furthermore, the catalyst contains both Ni–N4 sites and highly dispersed metallic Ni nanoclusters, leading to an increased CO2RR currents by two folds. Isotope labelling study and in situ spectroscopic analysis demonstrate that the existence of metallic Ni nanoclusters is the key factor for the activity enhancement and can shift the CO2RR mechanism from being electron transfer (ET)-limited (forming ∗COO−) to concerted proton-electron transfer (CPET)-limited (forming CO). •We report a novel catalyst containing Ni–N4 and highly dispersed metallic Ni nanoclusters.•The coexistence of Ni–N4 and metallic Ni nanoclusters increases the TOFCO by ca. 50%.•High-temperature pyrolysis shifts the RDS of CO2RR on NiPc-based catalysts.
ISSN:2468-0257
2468-0257
DOI:10.1016/j.gee.2021.05.006