One-step hydrothermal synthesis of CQDs/TiO2/NH2-MIL-125 for efficient photocatalytic production of H2O2 under visible light

光催化 热液循环 异质结 水热合成 制氢 可见光谱 分解水 材料科学 光化学 电子转移 氧气 化学工程 纳米技术 光电子学 氢 化学 催化作用 工程类 有机化学
作者
Jianhui Shi,Kaikai Pu,Ting Kai Zhao,Jiating Shi,Na Zheng,Lijun Nie,Kunkun Xue,Yuhang Gao
出处
期刊:Journal of Environmental Sciences-china [Elsevier BV]
卷期号:152: 637-653 被引量:26
标识
DOI:10.1016/j.jes.2024.05.034
摘要

NH2-MIL-125 and its derivatives are receiving more attention in various aspects of photocatalytic reactions, especially in the photocatalytic hydrogen peroxide (H2O2) production from water (H2O) and oxygen (O2), which is a promising and sustainable strategy. However, the generation of H2O2 from NH2-MIL-125 is far from satisfactory due to rapid photo-generated carriers recombination and poor surface electron transfer. In the work, the composite photocatalyst CQDs/TiO2/NH2-MIL-125 (C/T/NM) was designed for the first time by one-step hydrothermal method. TiO2 was in situ converted from partial NH2-MIL-125 (NM) during the successful loaded of Carbon quantum dots (CQDs) by hydrothermal process. The results indicated the type Ⅱ heterojunction was successfully constructed between the NM and TiO2 interface, which could promote the transmission of photo-generated electrons. In addition, the successful loaded of CQDs could effectively transfer and stored the photo-generated electrons to the photocatalyst surface to participate in the reaction, and further avoiding the recombination of photo-generated carriers. The C/T/NM composite photocatalyst achieved a H2O2 generation of 455 µmol/L for 5 hours under visible light without oxygen bubbling, which was 7.1 times superior to that of NM. The H2O2 generation rate reached 645.4 µM/(g·h), which was in priority in the reported literature under the same conditions. Finally, based on the active species capture experiments, energy band structure analysis and the photoelectrochemical measurements, a possible mechanism for the efficient H2O2 generation through C/T/NM had been proposed. This work provided new ideas for designing NH2-MIL-125 based composite photocatalysts for the production of H2O2.
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