Unravelling the role of reactive oxygen species in ultrathin Z-scheme heterojunction with surface zinc vacancies for photocatalytic H2O2 generation and CTC degradation

被引:70
作者
Liu, Hui-Yun [1 ]
Niu, Cheng-Gang [1 ]
Huang, Da-Wei [2 ]
Liang, Chao [3 ]
Guo, Hai [4 ]
Yang, Ya-Ya [1 ]
Li, Lu [1 ]
机构
[1] Hunan Univ, Coll Environm Sci & Engn, Key Lab Environm Biol & Pollut Control, Minist Educ, Changsha 410082, Peoples R China
[2] Minist Ecol & Environm PRC, South China Inst Environm Sci, Guangzhou 510655, Peoples R China
[3] Yantai Univ, Sch Environm & Mat Engn, Yantai 264005, Shandong, Peoples R China
[4] Hunan Univ Technol & Business, Sch Resources & Environm, Changsha 410205, Peoples R China
基金
中国国家自然科学基金;
关键词
Built-in electronic field; Ultrathin; 2D; 2D contact; ROS; Zn vacancies; GRAPHITIC CARBON NITRIDE; CHARGE-TRANSFER; SYSTEM; NANOSHEETS;
D O I
10.1016/j.cej.2023.143007
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Photo-induced reactive oxygen species (ROS) produced by molecular oxygen activation and oxidization of H2O/ OH- during photocatalytic reaction are extremely important in environmental remediation. Herein, a dual pathway to improve ROS formation was designed through establishing ultrathin 2D/2D Z-scheme heterojunction and defect engineering in O-doped g-C3N4/ZnIn2S4-Zn (ZIS-Z/OCN) composite. The results of experiment and density functional theory (DFT) calculation indicate that the charge-carriers are spatially separated in composite driven by different work functions and ultrathin 2D/2D interface, boosting charge-transfer efficiency from 42.05 % (ZnIn2S4-Zn) to 59.93 % (40ZIS-Z/OCN). Benefiting by this fact, improving molecular oxygen activation capacity can induce more ROS generation. In consequence, 40ZIS-Z/OCN reveals optimal chlortetracycline hydrochloride (CTC) removal efficiency (88.43 %) and hydrogen peroxide (H2O2) yield (168.67 mu mol/L) under visible light irradiation. The results of control experiments show that H2O2 is generated via two-step electron reduction route and singlet oxygen (1O2) conversion. This study provides new views on the construction of costeffective and reusable photocatalysts for environmental remediation and energy conversion.
引用
收藏
页数:19
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