Chenghua Fan , Dongbo Wang , Yuyan Feng , Qingge Feng , Dachao Ma , Qiming Wang , Ying Lu , Wenqiang Yang
{"title":"通过氮化碳中的碳空位调节单原子锰区的电荷密度,高效激活高碘酸盐降解磺胺甲噁唑","authors":"Chenghua Fan , Dongbo Wang , Yuyan Feng , Qingge Feng , Dachao Ma , Qiming Wang , Ying Lu , Wenqiang Yang","doi":"10.1016/j.seppur.2024.130515","DOIUrl":null,"url":null,"abstract":"<div><div>The advanced oxidation system involving periodate (PI) has demonstrated effective degradation capabilities for certain organic pollutants in water. A critical aspect of this process is the efficient activation of periodate. In this experiment, carbon vacancy-containing graphitic carbon nitride (C<sub>v</sub>-CN) was prepared through a simple high-temperature calcination method, and Mn atoms were uniformly dispersed on its surface, forming Mn-C<sub>v</sub>-CN. The presence of carbon vacancies modulated the electron density around the single-atom Mn, significantly enhancing the activation efficiency of PI. Surface-anchored Mn atoms with carbon vacancies in carbon nitride/periodate (Mn-C<sub>v</sub>-CN/PI) system degraded 99% of sulfamethoxazole (SMX) within 25 min. Various degradation factors for SMX, including <img>O<sub>2</sub><sup>−</sup>, <sup>1</sup>O<sub>2</sub>, <img>IO<sub>3</sub>, <img>OH, and electron transfer processes, were detected, with <img>O<sub>2</sub><sup>−</sup> identified as the primary reactive oxygen species (ROS). PI was activated by acquiring electrons from active sites, generating a substantial amount of <img>O<sub>2</sub><sup>−</sup> to catalytically transform the pollutants. Liquid chromatography-mass spectrometry was used to analyze the possible degradation pathways and intermediates of SMX. Multiple experiments demonstrated that the Mn-C<sub>v</sub>-CN/PI system showed promising potential in treating water containing recalcitrant antibiotics. The findings provided a novel strategy for efficiently activating PI with single-atom catalysts to remove refractory pollutants from water.</div></div>","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"359 ","pages":"Article 130515"},"PeriodicalIF":8.1000,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient activation of periodate for sulfamethoxazole degradation by modulating charge density in single-atom Mn regions via carbon vacancies in carbon nitride\",\"authors\":\"Chenghua Fan , Dongbo Wang , Yuyan Feng , Qingge Feng , Dachao Ma , Qiming Wang , Ying Lu , Wenqiang Yang\",\"doi\":\"10.1016/j.seppur.2024.130515\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The advanced oxidation system involving periodate (PI) has demonstrated effective degradation capabilities for certain organic pollutants in water. A critical aspect of this process is the efficient activation of periodate. In this experiment, carbon vacancy-containing graphitic carbon nitride (C<sub>v</sub>-CN) was prepared through a simple high-temperature calcination method, and Mn atoms were uniformly dispersed on its surface, forming Mn-C<sub>v</sub>-CN. The presence of carbon vacancies modulated the electron density around the single-atom Mn, significantly enhancing the activation efficiency of PI. Surface-anchored Mn atoms with carbon vacancies in carbon nitride/periodate (Mn-C<sub>v</sub>-CN/PI) system degraded 99% of sulfamethoxazole (SMX) within 25 min. Various degradation factors for SMX, including <img>O<sub>2</sub><sup>−</sup>, <sup>1</sup>O<sub>2</sub>, <img>IO<sub>3</sub>, <img>OH, and electron transfer processes, were detected, with <img>O<sub>2</sub><sup>−</sup> identified as the primary reactive oxygen species (ROS). PI was activated by acquiring electrons from active sites, generating a substantial amount of <img>O<sub>2</sub><sup>−</sup> to catalytically transform the pollutants. Liquid chromatography-mass spectrometry was used to analyze the possible degradation pathways and intermediates of SMX. Multiple experiments demonstrated that the Mn-C<sub>v</sub>-CN/PI system showed promising potential in treating water containing recalcitrant antibiotics. The findings provided a novel strategy for efficiently activating PI with single-atom catalysts to remove refractory pollutants from water.</div></div>\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"359 \",\"pages\":\"Article 130515\"},\"PeriodicalIF\":8.1000,\"publicationDate\":\"2024-11-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Separation and Purification Technology\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1383586624042540\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Separation and Purification Technology","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1383586624042540","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Efficient activation of periodate for sulfamethoxazole degradation by modulating charge density in single-atom Mn regions via carbon vacancies in carbon nitride
The advanced oxidation system involving periodate (PI) has demonstrated effective degradation capabilities for certain organic pollutants in water. A critical aspect of this process is the efficient activation of periodate. In this experiment, carbon vacancy-containing graphitic carbon nitride (Cv-CN) was prepared through a simple high-temperature calcination method, and Mn atoms were uniformly dispersed on its surface, forming Mn-Cv-CN. The presence of carbon vacancies modulated the electron density around the single-atom Mn, significantly enhancing the activation efficiency of PI. Surface-anchored Mn atoms with carbon vacancies in carbon nitride/periodate (Mn-Cv-CN/PI) system degraded 99% of sulfamethoxazole (SMX) within 25 min. Various degradation factors for SMX, including O2−, 1O2, IO3, OH, and electron transfer processes, were detected, with O2− identified as the primary reactive oxygen species (ROS). PI was activated by acquiring electrons from active sites, generating a substantial amount of O2− to catalytically transform the pollutants. Liquid chromatography-mass spectrometry was used to analyze the possible degradation pathways and intermediates of SMX. Multiple experiments demonstrated that the Mn-Cv-CN/PI system showed promising potential in treating water containing recalcitrant antibiotics. The findings provided a novel strategy for efficiently activating PI with single-atom catalysts to remove refractory pollutants from water.
期刊介绍:
Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.