Ning An , Min Zhao , Xiangyong Zheng , Qi Wang , Xianfeng Huang , Bo Sun , Yi Shen , Jun Wang , Baoliang Chen , Renlan Liu
{"title":"氮硫共掺杂多孔碳球对土霉素的协同吸附及过氧化二硫酸盐驱动氧化","authors":"Ning An , Min Zhao , Xiangyong Zheng , Qi Wang , Xianfeng Huang , Bo Sun , Yi Shen , Jun Wang , Baoliang Chen , Renlan Liu","doi":"10.1016/j.jhazmat.2021.127444","DOIUrl":null,"url":null,"abstract":"<div><p><span>Metal-free carbonaceous catalysts are receiving increasing attention in wastewater treatment. Here, nitrogen and sulfur co-doped carbon sphere catalysts (N,S-CSs</span><sub>900</sub>-OH) were synthesized using glucose and <span>L</span>-cysteine via a hydrothermal method and high temperature alkali activation. The N,S-CSs<sub>900</sub><span>-10%-OH exhibited excellent catalytic performance for the degradation of oxytetracycline (OTC). The degradation rate was 95.9% in 60 min, and the reaction equilibrium rate constant was 0.0735 min</span><sup>−1</sup> (<em>k</em><sub>0–15 min</sub>). The synergistic effect of adsorption-promoting degradation was demonstrated in the removal process of OTC. The excellent adsorption capacity of N,S-CSs<sub>900</sub><span>-10%-OH ensured the efficient oxidation of OTC. N,S-CSs</span><sub>900</sub>-10%-OH reduced the activation energy of the OTC degradation reaction (<em>E</em><span>a=18.23 kJ/mol). Moreover, the pyrrolic N, thiophene S and carbon skeleton played an important role in the degradation of OTC based on density function theory, and the catalytic mechanism was expounded through radical and nonradical pathways. The active species involved in the reaction were O</span><sub>2</sub><sup>•−</sup>, <sup>1</sup>O<sub>2</sub>, SO<sub>4</sub><sup>•−</sup> and •OH, of which O<sub>2</sub><sup>•−</sup><span> was the primary reactive species. This study provides a new insight into the reaction mechanism for efficient treatment of organic pollutants using metal-free doped porous carbon materials.</span></p></div>","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":12.2000,"publicationDate":"2022-02-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"28","resultStr":"{\"title\":\"Synergistic oxytetracycline adsorption and peroxydisulfate-driven oxidation on nitrogen and sulfur co-doped porous carbon spheres\",\"authors\":\"Ning An , Min Zhao , Xiangyong Zheng , Qi Wang , Xianfeng Huang , Bo Sun , Yi Shen , Jun Wang , Baoliang Chen , Renlan Liu\",\"doi\":\"10.1016/j.jhazmat.2021.127444\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p><span>Metal-free carbonaceous catalysts are receiving increasing attention in wastewater treatment. Here, nitrogen and sulfur co-doped carbon sphere catalysts (N,S-CSs</span><sub>900</sub>-OH) were synthesized using glucose and <span>L</span>-cysteine via a hydrothermal method and high temperature alkali activation. The N,S-CSs<sub>900</sub><span>-10%-OH exhibited excellent catalytic performance for the degradation of oxytetracycline (OTC). The degradation rate was 95.9% in 60 min, and the reaction equilibrium rate constant was 0.0735 min</span><sup>−1</sup> (<em>k</em><sub>0–15 min</sub>). The synergistic effect of adsorption-promoting degradation was demonstrated in the removal process of OTC. The excellent adsorption capacity of N,S-CSs<sub>900</sub><span>-10%-OH ensured the efficient oxidation of OTC. N,S-CSs</span><sub>900</sub>-10%-OH reduced the activation energy of the OTC degradation reaction (<em>E</em><span>a=18.23 kJ/mol). Moreover, the pyrrolic N, thiophene S and carbon skeleton played an important role in the degradation of OTC based on density function theory, and the catalytic mechanism was expounded through radical and nonradical pathways. The active species involved in the reaction were O</span><sub>2</sub><sup>•−</sup>, <sup>1</sup>O<sub>2</sub>, SO<sub>4</sub><sup>•−</sup> and •OH, of which O<sub>2</sub><sup>•−</sup><span> was the primary reactive species. This study provides a new insight into the reaction mechanism for efficient treatment of organic pollutants using metal-free doped porous carbon materials.</span></p></div>\",\"PeriodicalId\":361,\"journal\":{\"name\":\"Journal of Hazardous Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":12.2000,\"publicationDate\":\"2022-02-15\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"28\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Hazardous Materials\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0304389421024122\",\"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":"Journal of Hazardous Materials","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0304389421024122","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}
Synergistic oxytetracycline adsorption and peroxydisulfate-driven oxidation on nitrogen and sulfur co-doped porous carbon spheres
Metal-free carbonaceous catalysts are receiving increasing attention in wastewater treatment. Here, nitrogen and sulfur co-doped carbon sphere catalysts (N,S-CSs900-OH) were synthesized using glucose and L-cysteine via a hydrothermal method and high temperature alkali activation. The N,S-CSs900-10%-OH exhibited excellent catalytic performance for the degradation of oxytetracycline (OTC). The degradation rate was 95.9% in 60 min, and the reaction equilibrium rate constant was 0.0735 min−1 (k0–15 min). The synergistic effect of adsorption-promoting degradation was demonstrated in the removal process of OTC. The excellent adsorption capacity of N,S-CSs900-10%-OH ensured the efficient oxidation of OTC. N,S-CSs900-10%-OH reduced the activation energy of the OTC degradation reaction (Ea=18.23 kJ/mol). Moreover, the pyrrolic N, thiophene S and carbon skeleton played an important role in the degradation of OTC based on density function theory, and the catalytic mechanism was expounded through radical and nonradical pathways. The active species involved in the reaction were O2•−, 1O2, SO4•− and •OH, of which O2•− was the primary reactive species. This study provides a new insight into the reaction mechanism for efficient treatment of organic pollutants using metal-free doped porous carbon materials.
期刊介绍:
The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.