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基于 MOF 的氮掺杂 ZnO 碳骨架@分级 BiMoO S 型异质结用于 SMX 的光降解:机制、途径和 DFT 计算。

MOF-derived N-doped ZnO carbon skeleton@hierarchical BiMoO S-scheme heterojunction for photodegradation of SMX: Mechanism, pathways and DFT calculation.

机构信息

State Key Laboratory of Urban Water Resource and Environment (SKLUWRE), School of Environment, Harbin Institute of Technology, Harbin 150090, PR China.

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, PR China.

出版信息

J Hazard Mater. 2022 Mar 15;426:128106. doi: 10.1016/j.jhazmat.2021.128106. Epub 2021 Dec 21.

DOI:10.1016/j.jhazmat.2021.128106
PMID:34953261
Abstract

Semiconductor photocatalytic degradation of pollutants is considered to be one of the promising sustainable energy routes. Nevertheless, it is challenging for photocatalysts to have excellent visible light absorption and suppress photo-generated electron-hole recombination at the same time. Here, we prepared nitrogen-doped ZnO carbon skeleton by directly calcining the metal-organic framework. Then hierarchical BiMoO nanosheets are grown in situ on its surface to synthesize S-scheme heterojunction. This special 3D layered and oxygen vacancies work together to make photo-generated electrons and holes easier to separate and migrate. Therefore, the pseudo-first-order kinetic constant of N-doped ZnO carbon skeleton@BiMoO degradation of sulfamethoxazole reaches 0.022 min, which is almost 10 times that of ZIF-8 derived ZnO and 27.5 times BiMoO under visible light irradiation. Meanwhile, the mechanism of driving charge transfer of S-scheme heterojunction, and the photocatalytic degradation pathway of sulfamethoxazole are also analyzed. This work will provide a new way to construct S-scheme heterojunction photocatalyst to degrade antibiotic pollutants.

摘要

半导体光催化降解污染物被认为是有前途的可持续能源途径之一。然而,光催化剂同时具有优异的可见光吸收和抑制光生载流子复合的能力是具有挑战性的。在这里,我们通过直接煅烧金属有机骨架制备了氮掺杂 ZnO 碳骨架。然后在其表面原位生长分级 BiMoO 纳米片以合成 S 型异质结。这种特殊的 3D 层状结构和氧空位共同作用,使光生电子和空穴更容易分离和迁移。因此,氮掺杂 ZnO 碳骨架@BiMoO 降解磺胺甲恶唑的伪一级动力学常数达到 0.022 min,在可见光照射下几乎是 ZIF-8 衍生 ZnO 的 10 倍,是 BiMoO 的 27.5 倍。同时,还分析了 S 型异质结的电荷转移驱动机制以及磺胺甲恶唑的光催化降解途径。这项工作将为构建 S 型异质结光催化剂降解抗生素污染物提供新途径。

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