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构建用于甲基橙光降解的C-O桥连CeO/g-CN S型异质结:实验与理论计算

Constructing C-O bridged CeO/g-CN S-scheme heterojunction for methyl orange photodegradation:Experimental and theoretical calculation.

作者信息

Yang Chen, Yang Jian, Liu Shuangshuang, Zhao Mingxue, Duan Xu, Wu Hongli, Liu Lang, Liu Weizao, Li Jiangling, Ren Shan, Liu Qingcai

机构信息

College of Materials Science and Engineering, Chongqing University, Chongqing, 400044, China.

College of Materials Science and Engineering, Chongqing University, Chongqing, 400044, China.

出版信息

J Environ Manage. 2023 Jun 1;335:117608. doi: 10.1016/j.jenvman.2023.117608. Epub 2023 Mar 1.

Abstract

Owing to its feasibility, efficiency in light-harvesting and effectiveness in the interfacial charge transfer between two n-type semiconductors, constructing heterojunction photocatalysts have been identified as an effective way for enhancing the photocatalytic properties. In this research, a C-O bridged CeO/g-CN (cCN) Step-scheme (S-scheme) heterojunction photocatalyst was constructed successfully. Under visible light irradiation, the cCN heterojunction exhibited the photocatalytic degradation efficiency of methyl orange, which was about 4.5 and 1.5 times higher than that of pristine CeO and CN, respectively. The DFT calculations, XPS and FTIR analyses demonstrated the formation of C-O linkages. And the calculations of work functions revealed the electrons would flow from g-CN to CeO due to the difference in Fermi levels, resulting in the production of internal electric fields. Benefiting from the C-O bond and internal electric field, the photo-induced holes in the valence band of g-CN and the photo-induced electrons from conduction band of CeO would be recombined when exposed to visible light irradiation, while leaving the electrons with higher redox potential in the conduction band of g-CN. This collaboration accelerated the separation and transfer rate of photo-generated electron-hole pairs, which promoted the generation of superoxide radical (•O) and improved the photocatalytic activity.

摘要

由于其可行性、光捕获效率以及在两种n型半导体之间界面电荷转移的有效性,构建异质结光催化剂已被认为是增强光催化性能的有效途径。在本研究中,成功构建了一种C-O桥连的CeO/g-CN(cCN)型阶梯式(S型)异质结光催化剂。在可见光照射下,cCN异质结表现出对甲基橙的光催化降解效率,分别比原始CeO和CN高约4.5倍和1.5倍。DFT计算、XPS和FTIR分析证明了C-O键的形成。功函数的计算表明,由于费米能级的差异,电子将从g-CN流向CeO,从而产生内电场。受益于C-O键和内电场,g-CN价带中的光生空穴和CeO导带中的光生电子在可见光照射下会复合,而在g-CN导带中留下具有更高氧化还原电位的电子。这种协同作用加速了光生电子-空穴对的分离和转移速率,促进了超氧自由基(•O)的产生并提高了光催化活性。

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