A novel and facile ultraviolet-induced photo-reduction for preparing oxidase-like AuNCs@H2N-ZIF-8 composites in alcohol-water solutions

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-06-30 DOI:10.1016/j.jcat.2024.115631
Xin-Yu Chang , Hong-Wei Li , Yuqing Wu
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Abstract

The composites of H2N-ZIF-8 supported gold nanoclusters (AuNCs@H2N-ZIF-8) were prepared by UV-induced photochemical reduction method in the methanol–water solution. The photochemical reaction was attributed to the generation of free radical as.

CH2·–OH, which reduced Au(III) to Au(0) and produced monodisperse AuNCs (<2.5 nm) in the mesoporous of H2N-ZIF-8. The generated AuNCs@H2N-ZIF-8 show oxidase-like properties to catalyze the oxidation of TMB, ABTS and OPD under mild conditions. Besides, the mechanism study by EPR shows that the composites can promote oxygen to generate singlet oxygen (1O2) and superoxide radicals (·O2-), endowing it excellent catalytic activity of oxidation. Further studies revealed that the large number of exposed small AuNCs in the mesoporous pores of H2N-ZIF-8 and the highly active 211 crystalline facets formed at the edges contribute to the ROS generation intrinsically. Therefore, the present study demonstrates the significance of photochemical reduction method to prepare highly efficient oxidase-like materials, opening up a new avenue to construct noble metal materials as ultra-small nanozyme.

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在醇水溶液中制备氧化酶样 AuNCs@H2N-ZIF-8 复合材料的新颖而简便的紫外线诱导光还原法
在甲醇-水溶液中采用紫外光诱导光化学还原法制备了H2N-ZIF-8支撑的金纳米团簇复合材料(AuNCs@H2N-ZIF-8)。光化学反应是由于产生了自由基 CH2--OH,将 Au(III) 还原成 Au(0),并在 H2N-ZIF-8 的介孔中生成了单分散的 AuNCs(2.5 nm)。生成的 AuNCs@H2N-ZIF-8 具有类似氧化酶的性质,可在温和条件下催化 TMB、ABTS 和 OPD 的氧化。此外,通过 EPR 进行的机理研究表明,该复合材料能促进氧气生成单线态氧(1O2)和超氧自由基(-O2-),从而赋予其优异的氧化催化活性。进一步的研究表明,H2N-ZIF-8 的介孔中大量暴露的小金色氧化萘(AuNC)和边缘形成的高活性 211 晶面从本质上促进了 ROS 的生成。因此,本研究证明了光化学还原法制备高效类氧化酶材料的重要意义,为构建贵金属超小纳米酶材料开辟了一条新途径。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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