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自稳定间接 Z 型 g-CN/I-BiOI 上光催化 CHSH 氧化的高效性能和转化途径。

Highly Efficient Performance and Conversion Pathway of Photocatalytic CHSH Oxidation on Self-Stabilized Indirect Z-Scheme g-CN/I-BiOI.

机构信息

School of Environmental Science and Engineering , Sun Yat-sen University , Guangzhou 510275 , China.

Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology , Guangzhou 510275 , China.

出版信息

ACS Appl Mater Interfaces. 2018 Jun 6;10(22):18693-18708. doi: 10.1021/acsami.8b03250. Epub 2018 May 25.

Abstract

A self-stabilized Z-scheme porous g-CN/I-containing BiOI ultrathin nanosheets (g-CN/I-BiOI) heterojunction photocatalyst with I/I redox mediator was successfully synthesized by a facile solvothermal method coupling with light illumination. The structure and optical properties of g-CN/I-BiOI composites were systematically characterized by means of X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared, X-ray photoelectron spectroscopy, N adsorption/desorption, UV-vis diffuse reflectance spectrum, and photoluminescence. The g-CN/I-BiOI composites, with a heterojunction between porous g-CN and BiOI ultrathin nanosheets, were first applied for the photocatalytic elimination of ppm-leveled CHSH under light-emitting diode visible light illumination. The g-CN/I-BiOI heterojunction with 10% g-CN showed a dramatically enhanced photocatalytic activity in the removal of CHSH compared with pure BiOI and g-CN due to its effective interfacial charge transfer and separation. The adsorption and photocatalytic oxidation of CHSH over g-CN/I-BiOI were deeply explored by in situ diffuse reflectance infrared Fourier transform spectroscopy, and the intermediates and conversion pathways were elucidated and compared. Furthermore, on the basis of reactive species trapping, electron spin resonance and Mott-Schottky experiments, it was revealed that the responsible reactive species for catalytic CHSH composition were h, O, and O; thus, the g-CN/I-BiOI heterojunction followed an indirect all-solid state Z-scheme charge-transfer mode with self-stabilized I/I pairs as redox mediator, which could accelerate the separation of photogenerated charge and enhance the redox reaction power of charged carriers simultaneously.

摘要

一种自稳定 Z 型多孔 g-CN/I 掺杂 BiOI 超薄纳米片(g-CN/I-BiOI)异质结光催化剂,具有 I/I 氧化还原介体,通过简便的溶剂热法与光照相结合成功合成。采用 X 射线衍射、扫描电子显微镜、透射电子显微镜、傅里叶变换红外光谱、X 射线光电子能谱、N 吸附/脱附、紫外-可见漫反射光谱和光致发光等手段系统地表征了 g-CN/I-BiOI 复合材料的结构和光学性质。首先,将具有多孔 g-CN 和 BiOI 超薄纳米片之间异质结的 g-CN/I-BiOI 复合材料应用于发光二极管可见光照射下 ppm 级 CHSH 的光催化消除。与纯 BiOI 和 g-CN 相比,具有 10% g-CN 的 g-CN/I-BiOI 异质结在去除 CHSH 方面表现出显著增强的光催化活性,这是由于其有效的界面电荷转移和分离。通过原位漫反射红外傅里叶变换光谱深入探讨了 g-CN/I-BiOI 上 CHSH 的吸附和光催化氧化,阐明并比较了中间产物和转化途径。此外,基于活性物种捕获、电子自旋共振和 Mott-Schottky 实验,揭示了催化 CHSH 组成的活性物种是 h、O 和 O;因此,g-CN/I-BiOI 异质结遵循自稳定 I/I 对作为氧化还原介体的间接全固态 Z 型电荷转移模式,可同时加速光生电荷的分离并增强载流子的氧化还原反应能力。

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