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Abstract:
Charge transfer efficiency between discrete photosensitizers and catalytic sites is a key limiting factor in artificial photosynthesis. It is highly desirable but challenging to efficiently combine the two sections into an integration system and get insight into the kinetics and mechanisms. Here in, the photosensitizer [Ru(bpy)3]2+ (bpy = 2,2 ' bipyridine) and active cobalt porphyrin (Co-Por) sites were integrated into a covalent organic framework (COF), named COF-RuBpy-Co, for efficient charge transfer and photocatalytic CO2 reduction. The catalyst COF-RuBpyCo exhibited excellent CO2 photoreduction activity towards CO production with a rate of 547 mu mol g(-1)h(-1), which is 1.4-fold enhancement over the physical mixture of Ru(bpy)(3)Cl-2 and COF-Bpy-Co. In situ X-ray photoelectron spectroscopy combined with theoretical calculation results revealed that COF-RuBpy-Co achieved efficient photoelectron transfer from [Ru(bpy)(3)](2+) to cobalt porphyrin. More importantly, transient absorption spectroscopy indicated that the covalent linking [Ru(bpy)(3)](2+) and Co-Por units realized a faster charge transfer (44.2 ps) over the large it-conjugated system. This work provides vital insights into the charge carrier transfer process and demonstrates the potential of COFs as a platform in artificial photosynthesis.
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Source :
CHEMICAL ENGINEERING JOURNAL
ISSN: 1385-8947
Year: 2023
Volume: 458
1 3 . 4
JCR@2023
1 3 . 4 0 0
JCR@2023
ESI Discipline: ENGINEERING;
ESI HC Threshold:35
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 36
SCOPUS Cited Count: 38
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 4
Affiliated Colleges: