Heng Yang, Hao Deng*, Pengliang Liang, XianJin Ma, Jing Yin, Long Jiang, Yanyan Chen, Shuying Shi, Huiqiang Liu, Xue Ma, Yuxiang Li and Ying Xiong*,
{"title":"强酸性水溶液中的铼酸盐和珀尔帖酸盐的光催化还原。","authors":"Heng Yang, Hao Deng*, Pengliang Liang, XianJin Ma, Jing Yin, Long Jiang, Yanyan Chen, Shuying Shi, Huiqiang Liu, Xue Ma, Yuxiang Li and Ying Xiong*, ","doi":"10.1021/acs.est.4c02511","DOIUrl":null,"url":null,"abstract":"<p >Pertechnetate (<sup>99</sup>TcO<sub>4</sub><sup>–</sup>), a physiologically toxic radioactive anion, is of great concern due to its high mobility in environmental contamination remediation. Although the soluble oxyanion can be photoreduced to sparingly soluble TcO<sub>2</sub>·<i>n</i>H<sub>2</sub>O, its effective removal from a strongly acidic aqueous solution remains a challenge. Here, we found that low-crystalline nitrogen-doped titanium oxide (N-TiO<sub>2</sub>, 0.6 g L<sup>–1</sup>) could effectively uptake perrhenate (ReO<sub>4</sub><sup>–</sup>, 10 mg L<sup>–1</sup>, a nonradioactive surrogate for TcO<sub>4</sub><sup>–</sup>) with 50.8% during 360 min under simulated sunlight irradiation at pH 1.0, but P25 and anatase could not. The nitrogen active center formed by trace nitrogen doping in N-TiO<sub>2</sub> can promote the separation and transfer of photogenerated carriers. The positive valence band value of N-TiO<sub>2</sub> is slightly higher than those of P25 and anatase, which means that the photogenerated holes have a stronger oxidizability. These holes are involved in the formation of strong reducing <sup>•</sup>CO<sub>2</sub><sup>–</sup> radicals from formic acid oxidation. The active radicals convert ReO<sub>4</sub><sup>–</sup> to Re(VI), which is subsequently disproportionated to Re(IV) and Re(VII). Effective photocatalytic reduction/removal of Re(VII)/Tc(VII) is performed on the material, which may be considered a potential and convenient strategy for technetium decontamination and extraction in a strongly acidic aqueous solution.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8000,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Photocatalytic Reduction of Perrhenate and Pertechnetate in a Strongly Acidic Aqueous Solution\",\"authors\":\"Heng Yang, Hao Deng*, Pengliang Liang, XianJin Ma, Jing Yin, Long Jiang, Yanyan Chen, Shuying Shi, Huiqiang Liu, Xue Ma, Yuxiang Li and Ying Xiong*, \",\"doi\":\"10.1021/acs.est.4c02511\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Pertechnetate (<sup>99</sup>TcO<sub>4</sub><sup>–</sup>), a physiologically toxic radioactive anion, is of great concern due to its high mobility in environmental contamination remediation. Although the soluble oxyanion can be photoreduced to sparingly soluble TcO<sub>2</sub>·<i>n</i>H<sub>2</sub>O, its effective removal from a strongly acidic aqueous solution remains a challenge. Here, we found that low-crystalline nitrogen-doped titanium oxide (N-TiO<sub>2</sub>, 0.6 g L<sup>–1</sup>) could effectively uptake perrhenate (ReO<sub>4</sub><sup>–</sup>, 10 mg L<sup>–1</sup>, a nonradioactive surrogate for TcO<sub>4</sub><sup>–</sup>) with 50.8% during 360 min under simulated sunlight irradiation at pH 1.0, but P25 and anatase could not. The nitrogen active center formed by trace nitrogen doping in N-TiO<sub>2</sub> can promote the separation and transfer of photogenerated carriers. The positive valence band value of N-TiO<sub>2</sub> is slightly higher than those of P25 and anatase, which means that the photogenerated holes have a stronger oxidizability. These holes are involved in the formation of strong reducing <sup>•</sup>CO<sub>2</sub><sup>–</sup> radicals from formic acid oxidation. The active radicals convert ReO<sub>4</sub><sup>–</sup> to Re(VI), which is subsequently disproportionated to Re(IV) and Re(VII). Effective photocatalytic reduction/removal of Re(VII)/Tc(VII) is performed on the material, which may be considered a potential and convenient strategy for technetium decontamination and extraction in a strongly acidic aqueous solution.</p>\",\"PeriodicalId\":36,\"journal\":{\"name\":\"环境科学与技术\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":10.8000,\"publicationDate\":\"2024-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"环境科学与技术\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.est.4c02511\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.est.4c02511","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
Photocatalytic Reduction of Perrhenate and Pertechnetate in a Strongly Acidic Aqueous Solution
Pertechnetate (99TcO4–), a physiologically toxic radioactive anion, is of great concern due to its high mobility in environmental contamination remediation. Although the soluble oxyanion can be photoreduced to sparingly soluble TcO2·nH2O, its effective removal from a strongly acidic aqueous solution remains a challenge. Here, we found that low-crystalline nitrogen-doped titanium oxide (N-TiO2, 0.6 g L–1) could effectively uptake perrhenate (ReO4–, 10 mg L–1, a nonradioactive surrogate for TcO4–) with 50.8% during 360 min under simulated sunlight irradiation at pH 1.0, but P25 and anatase could not. The nitrogen active center formed by trace nitrogen doping in N-TiO2 can promote the separation and transfer of photogenerated carriers. The positive valence band value of N-TiO2 is slightly higher than those of P25 and anatase, which means that the photogenerated holes have a stronger oxidizability. These holes are involved in the formation of strong reducing •CO2– radicals from formic acid oxidation. The active radicals convert ReO4– to Re(VI), which is subsequently disproportionated to Re(IV) and Re(VII). Effective photocatalytic reduction/removal of Re(VII)/Tc(VII) is performed on the material, which may be considered a potential and convenient strategy for technetium decontamination and extraction in a strongly acidic aqueous solution.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.