Wenjin Chen , Lele Lei , Ke Zhu , Dongdong He , Hongmei He , Xiulan Li , Yumeng Wang , Jin Huang , Yushi Ai
{"title":"铁-N-S共掺杂银耳样碳催化剂对过氧单硫酸盐降解双酚A的活化作用:吡啶N、铁- nx、噻吩S的协同作用","authors":"Wenjin Chen , Lele Lei , Ke Zhu , Dongdong He , Hongmei He , Xiulan Li , Yumeng Wang , Jin Huang , Yushi Ai","doi":"10.1016/j.jes.2022.09.037","DOIUrl":null,"url":null,"abstract":"<div><p>Bisphenol A (BPA) has received increasing attention due to its long-term industrial application and persistence in environmental pollution. Iron-based carbon catalyst activation of peroxymonosulfate (PMS) shows a good prospect for effective elimination of recalcitrant contaminants in water. Herein, considering the problem about the leaching of iron ions and the optimization of heteroatoms doping, the iron, nitrogen and sulfur co-doped tremella-like carbon catalyst (Fe-NS@C) was rationally designed using very little iron, S-C<sub>3</sub>N<sub>4</sub> and low-cost chitosan (CS) via the impregnation-calcination method. The as-prepared Fe-NS@C exhibited excellent performance for complete removal of BPA (20 mg/L) by activating PMS with the high kinetic constant (1.492 min<sup>−1</sup>) in 15 min. Besides, the Fe-NS@C/PMS system not only possessed wide pH adaptation and high resistance to environmental interference, but also maintained an excellent degradation efficiency on different pollutants. Impressively, increased S-C<sub>3</sub>N<sub>4</sub> doping amount modulated the contents of different N species in Fe-NS@C, and the catalytic activity of Fe-NS@C-1-<em>x</em> was visibly enhanced with increasing S-C<sub>3</sub>N<sub>4</sub> contents, verifying pyridine N and Fe-N<sub><em>x</em></sub> as main active sites in the system. Meanwhile, thiophene sulfur (C-S-C) as active sites played an auxiliary role. Furthermore, quenching experiment, EPR analysis and electrochemical test proved that surface-bound radicals (<sup>·</sup>OH and SO<sub>4</sub><sup>⋅−</sup>) and non-radical pathways worked in the BPA degradation (the former played a dominant role). Finally, possible BPA degradation route were proposed. This work provided a promising way to synthesize the novel Fe, N and S co-doping carbon catalyst for degrading organic pollutants with low metal leaching and high catalytic ability.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"129 ","pages":"Pages 213-228"},"PeriodicalIF":6.9000,"publicationDate":"2023-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"3","resultStr":"{\"title\":\"Peroxymonosulfate activation by Fe-N-S co-doped tremella-like carbocatalyst for degradation of bisphenol A: Synergistic effect of pyridine N, Fe-Nx, thiophene S\",\"authors\":\"Wenjin Chen , Lele Lei , Ke Zhu , Dongdong He , Hongmei He , Xiulan Li , Yumeng Wang , Jin Huang , Yushi Ai\",\"doi\":\"10.1016/j.jes.2022.09.037\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Bisphenol A (BPA) has received increasing attention due to its long-term industrial application and persistence in environmental pollution. Iron-based carbon catalyst activation of peroxymonosulfate (PMS) shows a good prospect for effective elimination of recalcitrant contaminants in water. Herein, considering the problem about the leaching of iron ions and the optimization of heteroatoms doping, the iron, nitrogen and sulfur co-doped tremella-like carbon catalyst (Fe-NS@C) was rationally designed using very little iron, S-C<sub>3</sub>N<sub>4</sub> and low-cost chitosan (CS) via the impregnation-calcination method. The as-prepared Fe-NS@C exhibited excellent performance for complete removal of BPA (20 mg/L) by activating PMS with the high kinetic constant (1.492 min<sup>−1</sup>) in 15 min. Besides, the Fe-NS@C/PMS system not only possessed wide pH adaptation and high resistance to environmental interference, but also maintained an excellent degradation efficiency on different pollutants. Impressively, increased S-C<sub>3</sub>N<sub>4</sub> doping amount modulated the contents of different N species in Fe-NS@C, and the catalytic activity of Fe-NS@C-1-<em>x</em> was visibly enhanced with increasing S-C<sub>3</sub>N<sub>4</sub> contents, verifying pyridine N and Fe-N<sub><em>x</em></sub> as main active sites in the system. Meanwhile, thiophene sulfur (C-S-C) as active sites played an auxiliary role. Furthermore, quenching experiment, EPR analysis and electrochemical test proved that surface-bound radicals (<sup>·</sup>OH and SO<sub>4</sub><sup>⋅−</sup>) and non-radical pathways worked in the BPA degradation (the former played a dominant role). Finally, possible BPA degradation route were proposed. This work provided a promising way to synthesize the novel Fe, N and S co-doping carbon catalyst for degrading organic pollutants with low metal leaching and high catalytic ability.</p></div>\",\"PeriodicalId\":15774,\"journal\":{\"name\":\"Journal of environmental sciences\",\"volume\":\"129 \",\"pages\":\"Pages 213-228\"},\"PeriodicalIF\":6.9000,\"publicationDate\":\"2023-07-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"3\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of environmental sciences\",\"FirstCategoryId\":\"1089\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1001074222004843\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"Environmental Science\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of environmental sciences","FirstCategoryId":"1089","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1001074222004843","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"Environmental Science","Score":null,"Total":0}
Peroxymonosulfate activation by Fe-N-S co-doped tremella-like carbocatalyst for degradation of bisphenol A: Synergistic effect of pyridine N, Fe-Nx, thiophene S
Bisphenol A (BPA) has received increasing attention due to its long-term industrial application and persistence in environmental pollution. Iron-based carbon catalyst activation of peroxymonosulfate (PMS) shows a good prospect for effective elimination of recalcitrant contaminants in water. Herein, considering the problem about the leaching of iron ions and the optimization of heteroatoms doping, the iron, nitrogen and sulfur co-doped tremella-like carbon catalyst (Fe-NS@C) was rationally designed using very little iron, S-C3N4 and low-cost chitosan (CS) via the impregnation-calcination method. The as-prepared Fe-NS@C exhibited excellent performance for complete removal of BPA (20 mg/L) by activating PMS with the high kinetic constant (1.492 min−1) in 15 min. Besides, the Fe-NS@C/PMS system not only possessed wide pH adaptation and high resistance to environmental interference, but also maintained an excellent degradation efficiency on different pollutants. Impressively, increased S-C3N4 doping amount modulated the contents of different N species in Fe-NS@C, and the catalytic activity of Fe-NS@C-1-x was visibly enhanced with increasing S-C3N4 contents, verifying pyridine N and Fe-Nx as main active sites in the system. Meanwhile, thiophene sulfur (C-S-C) as active sites played an auxiliary role. Furthermore, quenching experiment, EPR analysis and electrochemical test proved that surface-bound radicals (·OH and SO4⋅−) and non-radical pathways worked in the BPA degradation (the former played a dominant role). Finally, possible BPA degradation route were proposed. This work provided a promising way to synthesize the novel Fe, N and S co-doping carbon catalyst for degrading organic pollutants with low metal leaching and high catalytic ability.
期刊介绍:
Journal of Environmental Sciences is an international peer-reviewed journal established in 1989. It is sponsored by the Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, and it is jointly published by Elsevier and Science Press. It aims to foster interdisciplinary communication and promote understanding of significant environmental issues. The journal seeks to publish significant and novel research on the fate and behaviour of emerging contaminants, human impact on the environment, human exposure to environmental contaminants and their health effects, and environmental remediation and management. Original research articles, critical reviews, highlights, and perspectives of high quality are published both in print and online.