期刊
INORGANIC CHEMISTRY FRONTIERS
卷 8, 期 14, 页码 3482-3490出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1qi00319d
关键词
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资金
- National Science Foundation of China [21675127, 31901794]
- National Postdoctoral Program for Innovative Talents [BX20180263]
- China Postdoctoral Science Foundation [2018M641026]
- Shaanxi Provincial Science Fund for Distinguished Young Scholars [2018JC-011]
- Young Talent Fund of University Association for Science and Technology in Shaanxi, China [2019-02-03]
- Key Research and Development Program of Shaanxi Province [2019NY-111]
- Cyrus Tang Foundation
This study demonstrates a ligand with photoresponsive oxidase-like activity for catalyzing oxidation reactions under light control, involving the generation of superoxide radicals through photogenerated electron transfer. Additionally, the inhibitory effect of copper ions on the catalytic system is unveiled.
Metal-organic frameworks (MOFs) are a promising type of candidate for mimicking natural enzymes, where ligands play an important role, but are rarely considered. This work proves that the ligand 2-aminoterephthalic acid (ATA) with photoresponsive oxidase-like activity could catalyze the substrate 3,3 ',5,5 '-tetramethylbenzidine (TMB) to form blue oxTMB under ultraviolet light illumination, and the oxidation reaction could be initiated, suspended, or terminated by light control, ensuring the precision of the spatial and temporal resolution. The presumable mechanism of enzyme-like activity is demonstrated to be relevant to the formation of superoxide radicals (O-2(-)) by photogenerated electron transfer. However, once Cu2+ ions are added to the ATA catalytic chromogenic system, the photooxidase-like activity of ATA could be inhibited due to the electron transfer and the formation of Cu-MOF, establishing a photoresponsive colorimetric sensor of Cu2+. In light of the role of ATA as a ligand in the MOF synthesis and the unique characteristics of MOFs, this paper reports an aluminum-based MOF made of ATA (Al-ATA), which has no oxidase-mimicking activity under dark conditions but shows photooxidase-like activity, confirming the importance of light for enzyme mimicking activity and throwing light on the exploration of the construction of ATA-based MOFs (ATA-MOFs) with photocontrollable oxidase mimicking activity as well as the possible photocatalytic mechanism of the MOFs.
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