Unveiling the Activity and Mechanism Alterations by Pyrene Decoration on a Co(II) Macrocyclic Catalyst for CO2 Reduction
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Títol
Unveiling the Activity and Mechanism Alterations by Pyrene Decoration on a Co(II) Macrocyclic Catalyst for CO2 ReductionAutoria
Data de publicació
2024-01-29Editor
WileyCita bibliogràfica
ZHANG, Weilu, et al. Unveiling the Activity and Mechanism Alterations by Pyrene Decoration on a Co (II) Macrocyclic Catalyst for CO2 Reduction. ChemSusChem, 2024, p. e202301113-e202301113.Tipus de document
info:eu-repo/semantics/articleVersió
info:eu-repo/semantics/submittedVersionParaules clau / Matèries
Resum
Mechanistic studies involving characterization of crucial intermediates are desirable for rational optimization of molecular catalysts toward CO2 reduction, while fundamental challenges are associated with such studies. ... [+]
Mechanistic studies involving characterization of crucial intermediates are desirable for rational optimization of molecular catalysts toward CO2 reduction, while fundamental challenges are associated with such studies. Herein we present the systematic mechanistic investigations on a pyrene-appended CoII macrocyclic catalyst in comparison with its pyrene-free prototype. The comparative results also verify the reasons of the higher catalytic activity of the pyrene-tethered catalyst in noble-metal-free CO2 photoreduction with various photosensitizers, where a remarkable apparent quantum yield of 36±3 % at 425 nm can be obtained for selective CO production. Electrochemical and spectroelectrochemical studies in conjunction with DFT calculations between the two catalysts have characterized the key CO-bound intermediates and revealed their different CO-binding behavior, demonstrating that the pyrene group endows the corresponding CoII catalyst a lower catalytic potential, a higher stability, and a greater ease in CO release, all of which contribute to its better performance. [-]
Entitat finançadora
Guangdong Basic and Applied Basic Research Foundation | Science and Technology Planning Project of Guangzhou
Codi del projecte o subvenció
2022A1515110079 | 202201011113
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