{"title":"双金属NH2-MOF(InxFe1−x)同时光催化去除Cr(VI)和As(III)的协同效应","authors":"Xin Zhong, Jing Xu, Sijia Song","doi":"10.1016/j.apsusc.2025.162659","DOIUrl":null,"url":null,"abstract":"<div><div>This work revealed that NH<sub>2</sub>-MIL-68(In) was ineffective for the removal of Cr(VI) by adsorption and photocatalytic reduction, and NH<sub>2</sub>-MIL-88B(Fe) had almost no effect on the photocatalytic oxidation of As(III). With the increase of Fe<sup>3+</sup> doping concentration, the removal of Cr(VI) by adsorption-photoreduction and As(III) by photo-oxidation obviously increased. Amongst, NH<sub>2</sub>-MOF(In<sub>0.2</sub>Fe<sub>0.8</sub>) exhibited the best photocatalytic performance, with total removal rates of 71.75 % for Cr(VI) and 46.64 % for As(III), and the total removal amounts of Cr(VI) and As(III) were 10.62 mg/g and 3.54 mg/g, respectively. Besides, the photoreduction of Cr(VI) by NH<sub>2</sub>-MOF(In<sub>0.2</sub>Fe<sub>0.8</sub>) was about 2.4 times higher than that of NH<sub>2</sub>-MIL-68(In), and the photo-oxidation of As(III) was 1.59 and 1.67 times higher than that of NH<sub>2</sub>-MIL-88B(Fe) and NH<sub>2</sub>-MIL-68(In), respectively. Owing to the modulation between In and Fe ions, the synergistic effect of ligand-to-metal and metal-to-metal charge transfer contributed to the dissociation of <em>e</em><sup>−</sup>-<em>h<sup>+</sup></em> pairs, rapid charge migration, which improved the photocatalytic efficiency. In addition, –NH<sub>2</sub> were the critical reaction sites for metal adsorption-photoreduction, which served as a dual donor of protons and electrons during Cr(VI) adsorption and photoreduction. Eventually, quenching experiments and EPR spectra indicated that <em>e</em><sup>−</sup>, <em>h<sup>+</sup></em>, •OH and •O<sub>2</sub><sup>−</sup> were the main active species.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"690 ","pages":"Article 162659"},"PeriodicalIF":6.3000,"publicationDate":"2025-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic effects in simultaneous photocatalytic removal of Cr(VI) and As(III) by bimetallic NH2-MOF(InxFe1−x)\",\"authors\":\"Xin Zhong, Jing Xu, Sijia Song\",\"doi\":\"10.1016/j.apsusc.2025.162659\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>This work revealed that NH<sub>2</sub>-MIL-68(In) was ineffective for the removal of Cr(VI) by adsorption and photocatalytic reduction, and NH<sub>2</sub>-MIL-88B(Fe) had almost no effect on the photocatalytic oxidation of As(III). With the increase of Fe<sup>3+</sup> doping concentration, the removal of Cr(VI) by adsorption-photoreduction and As(III) by photo-oxidation obviously increased. Amongst, NH<sub>2</sub>-MOF(In<sub>0.2</sub>Fe<sub>0.8</sub>) exhibited the best photocatalytic performance, with total removal rates of 71.75 % for Cr(VI) and 46.64 % for As(III), and the total removal amounts of Cr(VI) and As(III) were 10.62 mg/g and 3.54 mg/g, respectively. Besides, the photoreduction of Cr(VI) by NH<sub>2</sub>-MOF(In<sub>0.2</sub>Fe<sub>0.8</sub>) was about 2.4 times higher than that of NH<sub>2</sub>-MIL-68(In), and the photo-oxidation of As(III) was 1.59 and 1.67 times higher than that of NH<sub>2</sub>-MIL-88B(Fe) and NH<sub>2</sub>-MIL-68(In), respectively. Owing to the modulation between In and Fe ions, the synergistic effect of ligand-to-metal and metal-to-metal charge transfer contributed to the dissociation of <em>e</em><sup>−</sup>-<em>h<sup>+</sup></em> pairs, rapid charge migration, which improved the photocatalytic efficiency. In addition, –NH<sub>2</sub> were the critical reaction sites for metal adsorption-photoreduction, which served as a dual donor of protons and electrons during Cr(VI) adsorption and photoreduction. Eventually, quenching experiments and EPR spectra indicated that <em>e</em><sup>−</sup>, <em>h<sup>+</sup></em>, •OH and •O<sub>2</sub><sup>−</sup> were the main active species.</div></div>\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"690 \",\"pages\":\"Article 162659\"},\"PeriodicalIF\":6.3000,\"publicationDate\":\"2025-02-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0169433225003733\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0169433225003733","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Synergistic effects in simultaneous photocatalytic removal of Cr(VI) and As(III) by bimetallic NH2-MOF(InxFe1−x)
This work revealed that NH2-MIL-68(In) was ineffective for the removal of Cr(VI) by adsorption and photocatalytic reduction, and NH2-MIL-88B(Fe) had almost no effect on the photocatalytic oxidation of As(III). With the increase of Fe3+ doping concentration, the removal of Cr(VI) by adsorption-photoreduction and As(III) by photo-oxidation obviously increased. Amongst, NH2-MOF(In0.2Fe0.8) exhibited the best photocatalytic performance, with total removal rates of 71.75 % for Cr(VI) and 46.64 % for As(III), and the total removal amounts of Cr(VI) and As(III) were 10.62 mg/g and 3.54 mg/g, respectively. Besides, the photoreduction of Cr(VI) by NH2-MOF(In0.2Fe0.8) was about 2.4 times higher than that of NH2-MIL-68(In), and the photo-oxidation of As(III) was 1.59 and 1.67 times higher than that of NH2-MIL-88B(Fe) and NH2-MIL-68(In), respectively. Owing to the modulation between In and Fe ions, the synergistic effect of ligand-to-metal and metal-to-metal charge transfer contributed to the dissociation of e−-h+ pairs, rapid charge migration, which improved the photocatalytic efficiency. In addition, –NH2 were the critical reaction sites for metal adsorption-photoreduction, which served as a dual donor of protons and electrons during Cr(VI) adsorption and photoreduction. Eventually, quenching experiments and EPR spectra indicated that e−, h+, •OH and •O2− were the main active species.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.