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 化学 催化作用 工程类 有机化学
作者
Jianhui Shi,Jianhui Shi,Kaikai Pu,Ting Zhao,Jiating Shi,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:16
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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