Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 51, Pages 61578-61586Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c21663
Keywords
Defect modulator; MOFs; carbon dioxide; photoreduction; absorption energy
Funding
- National Natural Science Foundation of China [22171131, 22033004]
- National Basic Research Program of China [2017YFA0303504, 2019YFC0408303]
- Priority Academic Program Development of Jiangsu Higher Education Institutions
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The study found that shorter dicarboxylate ligands and more amino group-modified defects can decrease the absorption energy of metal-organic frameworks, thereby enhancing the efficiency of photocatalytic CO2 reduction.
The nature of defects and organic ligands can fine-tune the absorption energy (E-abs) of metal-organic frameworks (MOFs), which is crucial for photocatalytic reactions; however, the relevant studies are in their infancy. Herein, a series of typical MOFs of the UiO family (UiO-6x-NH2, x = 8, 7, and 6) with ligands of varied lengths and amino-group-modified defects were synthesized and employed to explore their performance for photocatalytic CO2 reduction. Sample UiO-66-NH2-2ABA (2ABA = 3,S-diamino-benzoate) with the shortest dicarboxylate ligand and two amino-group-modified defects exhibits superior photocatalytic activity due to the lowest E-abs. The CO yield photocatalyzed by UiO-66-NH2-2ABA is 17.5 mu mol g(-1) h(-1), which is 2.4 times that of UiO-68-NH2-BA (BA = benzoate) with the longest ligand and no amino group involved in the defects. Both the experiments and theoretical calculations show that shorter dicarboxylate ligands and more amino groups result in smaller E-abs, which is favorable for photocatalytic reactions. This study provides new insights into boosting the photocatalytic efficiency by modulating the defects and ligands in MOFs.
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