Yue Ma, Yi Chen, Minghui Sun, Xinhe Zhang, Bo Liu, Shi Zhou, Wei Jiang, Chunbo Liu
{"title":"碳纳米管催化剂中Co-Co/Co-N活性位点的工程设计用于高效类芬顿去除磺胺甲恶唑","authors":"Yue Ma, Yi Chen, Minghui Sun, Xinhe Zhang, Bo Liu, Shi Zhou, Wei Jiang, Chunbo Liu","doi":"10.1016/j.seppur.2025.135474","DOIUrl":null,"url":null,"abstract":"Development highly efficient and stable carbon-loaded cobalt-based catalysts holds great significance for Fenton-like wastewater purification. The incorporation of N atoms into the carbon substrate can effectively modulate the charge distribution of the catalyst and generate multiple active sites. Herein, using ZIF-9 and melamine as precursors, Co nanoparticles encapsulated N-doped carbon nanotubes (Co@NCNT) were constructed. In Fenton-like catalysis, Co@NCNT could efficiently activate peroxymonosulfate (PMS) to produce reactive oxygen species (ROS), and completely degrade sulfamethoxazole (SMX) within 5 min. Meanwhile, the Co@NCNT/PMS system shows good resistance to inorganic anions and natural organic matter and is highly adaptable to various organic pollutants. Continuous 10 h operation of SMX degradation indicates Co@NCNT has good cycling stability and practical application potential. Mechanism analysis reveals the synergistic effect between radicals (SO<sub>4</sub><sup>•-</sup>) and non-radicals (<sup>1</sup>O<sub>2</sub>, Co(IV) = O). In addition, there are two active sites (Co-Co/Co-N) to propel PMS activation, Co<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>Co bonds primarily contribute to the formation of <sup>1</sup>O<sub>2</sub>, Co(IV) = O, and SO<sub>4</sub><sup>•-</sup>, whereas Co<img alt=\"single bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\" style=\"vertical-align:middle\"/>N bonds generate a minor amount of <sup>1</sup>O<sub>2</sub>, minimize Co leakage, and enhance electron transfer efficiency. In summary, this work provides a strategy for the simple fabrication of catalysts with dual active sites for efficient Fenton-like catalysis.","PeriodicalId":427,"journal":{"name":"Separation and Purification Technology","volume":"123 1","pages":""},"PeriodicalIF":9.0000,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Engineering active Co-Co/Co-N sites in carbon nanotube catalyst for efficient Fenton-like removal of sulfamethoxazole\",\"authors\":\"Yue Ma, Yi Chen, Minghui Sun, Xinhe Zhang, Bo Liu, Shi Zhou, Wei Jiang, Chunbo Liu\",\"doi\":\"10.1016/j.seppur.2025.135474\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Development highly efficient and stable carbon-loaded cobalt-based catalysts holds great significance for Fenton-like wastewater purification. The incorporation of N atoms into the carbon substrate can effectively modulate the charge distribution of the catalyst and generate multiple active sites. Herein, using ZIF-9 and melamine as precursors, Co nanoparticles encapsulated N-doped carbon nanotubes (Co@NCNT) were constructed. In Fenton-like catalysis, Co@NCNT could efficiently activate peroxymonosulfate (PMS) to produce reactive oxygen species (ROS), and completely degrade sulfamethoxazole (SMX) within 5 min. Meanwhile, the Co@NCNT/PMS system shows good resistance to inorganic anions and natural organic matter and is highly adaptable to various organic pollutants. Continuous 10 h operation of SMX degradation indicates Co@NCNT has good cycling stability and practical application potential. Mechanism analysis reveals the synergistic effect between radicals (SO<sub>4</sub><sup>•-</sup>) and non-radicals (<sup>1</sup>O<sub>2</sub>, Co(IV) = O). In addition, there are two active sites (Co-Co/Co-N) to propel PMS activation, Co<img alt=\\\"single bond\\\" src=\\\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\\\" style=\\\"vertical-align:middle\\\"/>Co bonds primarily contribute to the formation of <sup>1</sup>O<sub>2</sub>, Co(IV) = O, and SO<sub>4</sub><sup>•-</sup>, whereas Co<img alt=\\\"single bond\\\" src=\\\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/sbnd.gif\\\" style=\\\"vertical-align:middle\\\"/>N bonds generate a minor amount of <sup>1</sup>O<sub>2</sub>, minimize Co leakage, and enhance electron transfer efficiency. In summary, this work provides a strategy for the simple fabrication of catalysts with dual active sites for efficient Fenton-like catalysis.\",\"PeriodicalId\":427,\"journal\":{\"name\":\"Separation and Purification Technology\",\"volume\":\"123 1\",\"pages\":\"\"},\"PeriodicalIF\":9.0000,\"publicationDate\":\"2025-10-06\",\"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://doi.org/10.1016/j.seppur.2025.135474\",\"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://doi.org/10.1016/j.seppur.2025.135474","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}
Engineering active Co-Co/Co-N sites in carbon nanotube catalyst for efficient Fenton-like removal of sulfamethoxazole
Development highly efficient and stable carbon-loaded cobalt-based catalysts holds great significance for Fenton-like wastewater purification. The incorporation of N atoms into the carbon substrate can effectively modulate the charge distribution of the catalyst and generate multiple active sites. Herein, using ZIF-9 and melamine as precursors, Co nanoparticles encapsulated N-doped carbon nanotubes (Co@NCNT) were constructed. In Fenton-like catalysis, Co@NCNT could efficiently activate peroxymonosulfate (PMS) to produce reactive oxygen species (ROS), and completely degrade sulfamethoxazole (SMX) within 5 min. Meanwhile, the Co@NCNT/PMS system shows good resistance to inorganic anions and natural organic matter and is highly adaptable to various organic pollutants. Continuous 10 h operation of SMX degradation indicates Co@NCNT has good cycling stability and practical application potential. Mechanism analysis reveals the synergistic effect between radicals (SO4•-) and non-radicals (1O2, Co(IV) = O). In addition, there are two active sites (Co-Co/Co-N) to propel PMS activation, CoCo bonds primarily contribute to the formation of 1O2, Co(IV) = O, and SO4•-, whereas CoN bonds generate a minor amount of 1O2, minimize Co leakage, and enhance electron transfer efficiency. In summary, this work provides a strategy for the simple fabrication of catalysts with dual active sites for efficient Fenton-like catalysis.
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.