Effects of different defective linkers on the photocatalytic properties of Cu-BTC for overall water decomposition

This manuscript proposed a synthesis strategy for simultaneously constructing defect structure and mixed valence coordinated unsaturated sites (CUS) in Cu-BTC (BTC=1,3,5-trihydroxybenzene) framework. Different defective linkers with increasing pKa value were used to regulate the defect concentration...

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Published in:Applied catalysis. B, Environmental Environmental, 2022-04, Vol.303, p.120888, Article 120888
Main Authors: Zhang, Li, Guo, Changyan, Chen, Tingxiang, Guo, Yuan, Hassan, Afaq, Kou, Yuli, Guo, Cheng, Wang, Jide
Format: Article
Language:English
Subjects:
Bifunctional catalyst
Catalysts
Catalytic activity
Copper
Current carriers
Defective linker
Defects
Electromagnetic absorption
Hydrogen production
Metal-Organic Frameworks
Photocatalysis
Recombination
Trihydroxybenzene
Water splitting
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Summary:This manuscript proposed a synthesis strategy for simultaneously constructing defect structure and mixed valence coordinated unsaturated sites (CUS) in Cu-BTC (BTC=1,3,5-trihydroxybenzene) framework. Different defective linkers with increasing pKa value were used to regulate the defect concentration and Cu1+/Cu2+ CUS content. The pKa value of defective linkers was proved to be inversely proportional to the defect concentration and Cu1+/Cu2+ CUS content. Compared with pure Cu-BTC, the defective Cu-BTC samples have obviously improved specific surface area, light absorption, bandgap, and charge carrier separation rate. All of these advantages make defective variants become an excellent bifunctional overall water splitting catalyst with O2 and H2 generation rates of 3942 μmol·g-1·h-1 and 15107 μmol·g-1·h-1, respectively. Although the defective linkers with small pKa value can create more defects, excessive defects in framework will lead to the parent structure collapse, and can also serve as recombination centers to reduce the photocatalytic activity of materials. [Display omitted] •Three defective Cu-BTC were synthesized via different defective linkers.•Defective linker with lower pKa would create more defect and Cu1+/Cu2+ CUS.•Too low pKa of defective linker will cause the collapse of parent structure.•Defective Cu-BTC shows improved hydrogen and oxygen evolution performance.•Excessive defect can act as electron hole recombination center.
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2021.120888