{"title":"构建用于高效光降解四环素的非经典 I 型异质结","authors":"Huan Yan, Xinhui Lu, Guoqiang Shen, Yangrui Xu, Xinping Zhang, Qinlan Luo*, Guosheng Zhou, Ziyang Lu*, Yangqiang Huang, Xiao Luo and Hao Chen*, ","doi":"10.1021/acs.iecr.4c0322910.1021/acs.iecr.4c03229","DOIUrl":null,"url":null,"abstract":"<p >Traditional Type-I heterojunctions, the combination of large- and narrow-bandgap semiconductors, possess a long electron transmission path and an electron–hole confinement region, making them not conducive to improving catalytic performance. Hence, few studies about the heterostructure combined with large and narrow bandgap in chemocatalysis were invested, especially in terms of reaction mechanism. Herein, a narrow bandgap (CdS) and a large bandgap (hexagonal boron nitride, h-BN) were selected as the research objects to fabricate h-BN/CdS heterojunction by Joule heating by an ultrafast heating procedure. Density functional theory (DFT) calculations were performed and showed that in the h-BN/CdS heterojunctions photogenerated electrons (e<sup>–</sup>) transferred from h-BN to CdS, while the photogenerated holes (h<sup>+</sup>) moved conversely, which is completely different from that of classical Type-I heterojunctions. Thus, a nonclassical Type-I h-BN/CdS heterojunction was successfully constructed, as proved by DFT calculations and experimental verification, which revealed excellent visible light response and photocatalytic degradation ability of tetracycline (TC). The optimized h-BN/CdS heterojunction exhibited a high degradation rate of 84.78% under visible light irradiation. Additionally, the applicability of h-BN/CdS heterojunction was expanded to photodegradation of different water environments. A nonclassical Type-I heterojunction that combined large- and narrow-bandgap materials was proposed, which opened up a new path for efficient photocatalysis in antibiotic wastewater degradation.</p>","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"63 45","pages":"19589–19599 19589–19599"},"PeriodicalIF":3.8000,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Construction of Nonclassical Type-I Heterojunction for Efficient Photodegrading Tetracycline\",\"authors\":\"Huan Yan, Xinhui Lu, Guoqiang Shen, Yangrui Xu, Xinping Zhang, Qinlan Luo*, Guosheng Zhou, Ziyang Lu*, Yangqiang Huang, Xiao Luo and Hao Chen*, \",\"doi\":\"10.1021/acs.iecr.4c0322910.1021/acs.iecr.4c03229\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Traditional Type-I heterojunctions, the combination of large- and narrow-bandgap semiconductors, possess a long electron transmission path and an electron–hole confinement region, making them not conducive to improving catalytic performance. Hence, few studies about the heterostructure combined with large and narrow bandgap in chemocatalysis were invested, especially in terms of reaction mechanism. Herein, a narrow bandgap (CdS) and a large bandgap (hexagonal boron nitride, h-BN) were selected as the research objects to fabricate h-BN/CdS heterojunction by Joule heating by an ultrafast heating procedure. Density functional theory (DFT) calculations were performed and showed that in the h-BN/CdS heterojunctions photogenerated electrons (e<sup>–</sup>) transferred from h-BN to CdS, while the photogenerated holes (h<sup>+</sup>) moved conversely, which is completely different from that of classical Type-I heterojunctions. Thus, a nonclassical Type-I h-BN/CdS heterojunction was successfully constructed, as proved by DFT calculations and experimental verification, which revealed excellent visible light response and photocatalytic degradation ability of tetracycline (TC). The optimized h-BN/CdS heterojunction exhibited a high degradation rate of 84.78% under visible light irradiation. Additionally, the applicability of h-BN/CdS heterojunction was expanded to photodegradation of different water environments. A nonclassical Type-I heterojunction that combined large- and narrow-bandgap materials was proposed, which opened up a new path for efficient photocatalysis in antibiotic wastewater degradation.</p>\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"63 45\",\"pages\":\"19589–19599 19589–19599\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2024-11-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.iecr.4c03229\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.iecr.4c03229","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
传统的 I 型异质结是大带隙和窄带隙半导体的结合,具有较长的电子传输路径和电子-空穴禁锢区,不利于提高催化性能。因此,有关大带隙和窄带隙异质结构在化学催化中的应用,尤其是反应机理方面的研究较少。本文选择了窄带隙(CdS)和大带隙(六方氮化硼,h-BN)作为研究对象,通过焦耳加热超快加热程序制备 h-BN/CdS 异质结。密度泛函理论(DFT)计算表明,在 h-BN/CdS 异质结中,光生电子(e-)从 h-BN 转移到 CdS,而光生空穴(h+)则反向移动,这与经典的 I 型异质结完全不同。因此,通过 DFT 计算和实验验证,成功地构建了非经典的 I 型 h-BN/CdS 异质结,并显示出优异的可见光响应和对四环素(TC)的光催化降解能力。优化后的 h-BN/CdS 异质结在可见光照射下的降解率高达 84.78%。此外,h-BN/CdS 异质结的适用性还扩展到了不同水环境的光降解。该研究提出了一种结合了大带隙和窄带隙材料的非典型 I 型异质结,为抗生素废水的高效光催化降解开辟了一条新途径。
Construction of Nonclassical Type-I Heterojunction for Efficient Photodegrading Tetracycline
Traditional Type-I heterojunctions, the combination of large- and narrow-bandgap semiconductors, possess a long electron transmission path and an electron–hole confinement region, making them not conducive to improving catalytic performance. Hence, few studies about the heterostructure combined with large and narrow bandgap in chemocatalysis were invested, especially in terms of reaction mechanism. Herein, a narrow bandgap (CdS) and a large bandgap (hexagonal boron nitride, h-BN) were selected as the research objects to fabricate h-BN/CdS heterojunction by Joule heating by an ultrafast heating procedure. Density functional theory (DFT) calculations were performed and showed that in the h-BN/CdS heterojunctions photogenerated electrons (e–) transferred from h-BN to CdS, while the photogenerated holes (h+) moved conversely, which is completely different from that of classical Type-I heterojunctions. Thus, a nonclassical Type-I h-BN/CdS heterojunction was successfully constructed, as proved by DFT calculations and experimental verification, which revealed excellent visible light response and photocatalytic degradation ability of tetracycline (TC). The optimized h-BN/CdS heterojunction exhibited a high degradation rate of 84.78% under visible light irradiation. Additionally, the applicability of h-BN/CdS heterojunction was expanded to photodegradation of different water environments. A nonclassical Type-I heterojunction that combined large- and narrow-bandgap materials was proposed, which opened up a new path for efficient photocatalysis in antibiotic wastewater degradation.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.