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• W4386347436 startingPage "19856" @default.
• W4386347436 abstract "Introducing an external visible-light field would be a promising strategy to improve the activity of the electrocatalytic CO2 reduction reaction (CO2RR), but it still remains a challenge due to the short excited-state lifetime of active sites. Herein, Ru(bpy)3Cl2 struts as powerful photosensitive donors were immobilized into the backbones of Co-porphyrin-based covalent organic frameworks (named Co-Bpy-COF-Rux, x is the molar ratio of Ru and Co species, x = 1/2 and 2/3) via coordination bonds, for the photo-coupled CO2RR to produce CO. The optimal Co-Bpy-COF-Ru1/2 displays a high CO Faradaic efficiency of 96.7% at −0.7 V vs reversible hydrogen electrode (RHE) and a CO partial current density of 16.27 mA cm–2 at −1.1 V vs RHE under the assistance of light, both of which were far surpassing the values observed in the dark. The significantly enhanced activity is mainly attributed to the incorporation of a Ru(bpy)3Cl2 donor with long excited-state lifetime and concomitantly giant built-in electric field in Co-Bpy-COF-Ru1/2, which efficiently accelerate the photo-induced electron transfer from Ru(bpy)3Cl2 to the cobalt-porphyrin under the external light. Thus, the cobalt-porphyrin active sites have a longer excited-state lifetime to lower the rate-determining steps’ energy occurring during the actual photo-coupled electrocatalytic CO2RR process. This is the first work of porphyrin-based COFs for photo-coupled CO2RR, opening a new frontier for the construction of efficient photo-coupled electrocatalysts." @default.
• W4386347436 created "2023-09-02" @default.
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• W4386347436 date "2023-08-31" @default.
• W4386347436 modified "2023-10-18" @default.
• W4386347436 title "Photocoupled Electroreduction of CO₂ over Photosensitizer-Decorated Covalent Organic Frameworks" @default.
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• W4386347436 doi "https://doi.org/10.1021/jacs.3c06113" @default.
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• W4386347436 hasPublicationYear "2023" @default.
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