In:
Nanoscale, Royal Society of Chemistry (RSC), Vol. 15, No. 10 ( 2023), p. 5036-5043
Abstract:
A combination of a semiconductor-based photosensitizer with molecular catalysts via covalent bonds is an effective way to utilize solar energy to reduce CO 2 into value-added chemicals with high efficiency and selectivity. In this study, 2,2′-bpy-5,5′-dialdehyde functioned as organic ligands and were embedded into the skeleton of g-CN through imine bonds via thermal copolymerization. The introduction of 2,2′-bpy can not only chelate with earth-abundant Co as single-site catalytic centers but also can optimize the properties of original g-CN such as the enlarged specific surface area and extended visible light absorption range. The CO evolution rate of g-CN-bpy-Co can reach up to 106.3 μmol g −1 h −1 with a selectivity of 97% over proton reduction, which was 82-fold than that of g-CN-Co. The different coordination environments and valence states of cobalt were also studied simultaneously and the results showed that Co( ii ) exhibited superior catalytic activity towards Co( iii ). Control experiments demonstrated that the covalent linkage between g-CN and Co-2,2′-bpy plays a vital role in photocatalytic activity and selectivity. Besides, the CO generation rate demonstrated linear growth upon visible light irradiation up to 72 h and preferable recyclability. This research provides a new facile way to fabricate low-priced photocatalysts with high activity and selectivity and bridge homogeneous and heterogeneous catalysis.
Type of Medium:
Online Resource
ISSN:
2040-3364
,
2040-3372
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2023
detail.hit.zdb_id:
2515664-0
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