物理化学学报 >> 2023, Vol. 39 >> Issue (6): 2209016.doi: 10.3866/PKU.WHXB202209016

所属专题: S型光催化剂

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0D/2D碳氮量子点(CNQDs)/BiOBr复合的S型异质结高效光催化降解和产H2O2

昝忠奇1, 李喜宝1,*(), 高晓明2, 黄军同1,*(), 罗一丹1, 韩露3,*()   

  1. 1 南昌航空大学材料科学与工程学院, 南昌 330063
    2 延安大学化学化工系, 陕西省化学反应工程重点实验室, 陕西 延安 716000
    3 辽宁科技大学材料与冶金学院, 辽宁 鞍山 114051
  • 收稿日期:2022-09-12 录用日期:2022-11-24 发布日期:2022-11-29
  • 通讯作者: 李喜宝,黄军同,韩露 E-mail:lixibao@nchu.edu.cn;huangjt@nchu.edu.cn;hanlu@ustl.edu.cn

0D/2D Carbon Nitride Quantum Dots (CNQDs)/BiOBr S-Scheme Heterojunction for Robust Photocatalytic Degradation and H2O2 Production

Zhongqi Zan1, Xibao Li1,*(), Xiaoming Gao2, Juntong Huang1,*(), Yidan Luo1, Lu Han3,*()   

  1. 1 School of Materials Science and Engineering, Nanchang Hangkong University, Nanchang 330063, China
    2 Department of Chemistry and Chemical Engineering, Shaanxi Key Laboratory of Chemical Reaction Engineering, Yan'an University, Yan'an 716000, Shaanxi Province, China
    3 School of Materials and Metallurgy, University of Science and Technology Liaoning, Anshan 114051, Liaoning Province, China
  • Received:2022-09-12 Accepted:2022-11-24 Published:2022-11-29
  • Contact: Xibao Li, Juntong Huang, Lu Han E-mail:lixibao@nchu.edu.cn;huangjt@nchu.edu.cn;hanlu@ustl.edu.cn

摘要:

光生载流子的快速复合制约着BiOBr的光催化性能,通过构建界面紧密结合的异质结可以有效地解决这个问题。在本研究中,通过采用简单的高温高压水热法,首次在二维(2D)BiOBr表面上成功复合了零维(0D)的g-C3N4量子点(CNQDs),并形成了具有紧密接触界面的0D/2D CNQDs/BiOBr S型异质结,主要原因是CNQDs杂环中的π电子与BiOBr产生了相互作用。CNQDs/BiOBr-1.50%复合材料在光照下降解四环素(TC)、环丙沙星(CIP)和产H2O2的表观反应速率常数k值分别是BiOBr的2.02、2.91和1.54倍。在循环测试中,CNQDs/BiOBr-1.50%显示出相对较高的光催化活性和结构稳定性。通过X射线光电子能谱(XPS)分析,明确CNQDs中的π电子与BiOBr具有相互作用,确认了异质结中光生电子的转移方向。CNQDs/BiOBr S型异质结的成功构建使其具有非凡的光催化稳定性和活性。更多活性物质的产生和稳定的催化活性归因于电子和空穴的独特转移机制。CNQDs/BiOBr S型异质结的特殊的电子-空穴转移机理实现了载流子在空间的有效分离和转移,且在光照条件下,催化剂上产生了更多的活性自由基,CNQDs/BiOBr复合材料的光催化活性和产H2O2的能力显著增强。这项工作将为构建用于降解有机污染物和原位产H2O2的0D/2D S型异质结提供借鉴与参考。

关键词: 光催化, 量子点, S型异质结, 催化活性, H2O2

Abstract:

The construction of heterojunctions is a method employed to inhibit the rapid recombination of photogenerated carriers. In this work, zero-dimensional (0D) g-C3N4 quantum dots (CNQDs) were composited with two-dimensional (2D) BiOBr for the first time using the typical hydrothermal method under the conditions of a high temperature and high pressure, and a 0D/2D CNQD/BiOBr S-scheme heterojunction with an intimate-contact interface was formed. The π-electrons in the heterocycle of the CNQDs were bound to BiOBr by interaction. The apparent reaction rate constants generated by CNQDs/BiOB-1.50% for tetracycline (TC) and ciprofloxacin (CIP) degradation and H2O2 production were 2.02, 2.91, and 1.54 times that of the original BiOBr, respectively. In the cycle test, CNQDs/BiOBr-1.50% displayed a relatively high photocatalytic activity and structural stability. X-ray photoelectron spectroscopy (XPS) analysis showed that the π electrons in the CNQDs interacted with BiOBr, and also confirmed the flow of photogenerated electrons in this heterojunction. This successfully constructed S-scheme exhibited extraordinary photocatalytic activity and stability. The more active species and stable catalytic activity were attributed to the distinctive transfer mechanism of the carriers. This work will provide reference for constructing 0D/2D S-scheme heterojunctions for the degradation of organic pollutants and in situ production of H2O2.

Key words: Photocatalysis, Quantum dots, S-scheme, Catalytic activity, H2O2