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通过剥离的石墨相氮化碳催化剂在紫外-A光和可见光照射下对有机微污染物进行光催化降解。

Photocatalytic degradation of organic micropollutants under UV-A and visible light irradiation by exfoliated g-CN catalysts.

作者信息

Antonopoulou Maria, Bika Panagiota, Papailias Ilias, Zervou Sevasti-Kiriaki, Vrettou Androniki, Efthimiou Ioanna, Mitrikas George, Ioannidis Nikolaos, Trapalis Christos, Dallas Panagiotis, Vlastos Dimitris, Hiskia Anastasia

机构信息

Department of Sustainable Agriculture, University of Patras, 30100, Agrinio, Greece.

Institute of Nanoscience & Nanotechnology, NCSR "Demokritos", Patr. Gregoriou E' & 27 Neapoleos Str, 15341 Agia Paraskevi, Athens, Greece.

出版信息

Sci Total Environ. 2023 Sep 20;892:164218. doi: 10.1016/j.scitotenv.2023.164218. Epub 2023 May 19.

Abstract

In the present study, the photocatalytic performance of exfoliated graphitic carbon nitride (g-CN) catalysts, with enhanced properties and response in UV and visible light irradiation, was evaluated for the removal of selected contaminants i.e., diuron, bisphenol A and ethyl paraben. Commercial TiO Degussa P25 was also used as a reference photocatalyst. The g-CN catalysts demonstrated good photocatalytic activity which in some cases is comparable to TiO Degussa P25 leading to high removal percentages of the studied micropollutants under UV-A light irradiation. In contrast to TiO Degussa P25, g-CN catalysts were also able to degrade the studied micropollutants under visible light irradiation. For all the studied g-CN catalysts under both UV-A and visible light irradiation, the overall degradation rate decreases in the order of bisphenol A > diuron > ethyl paraben. Among the studied g-CN, the chemically exfoliated catalyst (g-CN-CHEM) showed superior photocatalytic activity under UV-A light irradiation due to its enhanced characteristics, such as pore volume and specific surface area and ~ 82.0 % in 6 min, ~75.7 % in 15 min and ~ 96.3 % in 40 min removals were achieved for BPA, DIU and EP, respectively. Under visible light irradiation, the thermally exfoliated catalyst (g-CN-THERM) demonstrated the best photocatalytic performance and the degradation ranged from ~29.5 to 59.4 % after 120 min. EPR data revealed that the three g-CN semiconductors generate mainly O, whereas TiO Degussa P25 generates both HO and O, the latter only under UV-A light irradiation. Nevertheless, the indirect formation of HO in the case of g-CN should also be considered. Hydroxylation, oxidation, dealkylation, dechlorination and ring opening were the main degradation pathways. The process proceeded without significant alterations in toxicity levels. Based on the results, heterogeneous photocatalysis using g-CN catalysts is a promising method for the removal of organic micropollutants without the formation of harmful transformation products.

摘要

在本研究中,对剥离的石墨相氮化碳(g-CN)催化剂的光催化性能进行了评估,该催化剂具有增强的性能以及在紫外光和可见光照射下的响应能力,用于去除选定的污染物,即敌草隆、双酚A和对羟基苯甲酸乙酯。市售的TiO₂ Degussa P25也用作参考光催化剂。g-CN催化剂表现出良好的光催化活性,在某些情况下可与TiO₂ Degussa P25相媲美,在UV-A光照射下对所研究的微污染物具有较高的去除率。与TiO₂ Degussa P25不同,g-CN催化剂在可见光照射下也能够降解所研究的微污染物。对于在UV-A和可见光照射下所有研究的g-CN催化剂,总体降解速率按双酚A>敌草隆>对羟基苯甲酸乙酯的顺序降低。在所研究的g-CN中,化学剥离的催化剂(g-CN-CHEM)在UV-A光照射下表现出优异的光催化活性,这归因于其增强的特性,如孔体积和比表面积,对于双酚A(BPA)、敌草隆(DIU)和对羟基苯甲酸乙酯(EP),分别在6分钟内实现了约82.0%的去除率,15分钟内约75.7%的去除率,40分钟内约96.3%的去除率。在可见光照射下,热剥离的催化剂(g-CN-THERM)表现出最佳的光催化性能,120分钟后的降解率在约29.5%至59.4%之间。电子顺磁共振(EPR)数据表明,三种g-CN半导体主要产生O₂⁻,而TiO₂ Degussa P25既产生·OH又产生O₂⁻,后者仅在UV-A光照射下产生。然而,在g-CN的情况下,也应考虑·OH的间接形成。羟基化、氧化、脱烷基化、脱氯和开环是主要的降解途径。该过程在毒性水平没有显著变化的情况下进行。基于这些结果,使用g-CN催化剂的多相光催化是一种有前途的去除有机微污染物的方法,且不会形成有害的转化产物。

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