{"title":"缺陷驱动双功能Cu/N共掺杂生物炭同步吸附和瞬间催化降解有机污染物","authors":"Rui Yu, Fang He, Jingjing Wang, Zaiwen Jia, Chao Liu, Haihong Zhou","doi":"10.1016/j.jenvman.2025.127703","DOIUrl":null,"url":null,"abstract":"<div><div>As a commonly used antibiotic in healthcare and livestock production, tetracycline (TC) remains in water bodies and poses ecological and health risks, making its efficient removal from wastewater essential. A copper (Cu) and nitrogen (N) co-doped biochar (BC) catalyst (denoted as Cu-N@KBC) was synthesized, exhibiting low energy consumption, excellent adsorption capacity, and superior catalytic performance. Cu-N@KBC achieved 35.2 % TC removal within 20 min, with the solid-liquid distribution coefficient (K<sub>d</sub>) of 4.541 L g<sup>−1</sup>, owing to its well-developed pore structure and abundant defect sites. N doping into the sp<sup>2</sup>-hybridized carbon network, synergistically coupled with uniform Cu loading, induced the formation of oxygen vacancies and surface defects, thereby creating additional active sites for TC adsorption. A maximum TC degradation of 96.5 % was achieved within 60 min under the optimized conditions. The combined incorporation of Cu and N elevated the graphitization degree (I<sub>D</sub>/I<sub>G</sub> = 0.93), optimizing electron transfer and facilitating ≡ Cu<sup>2+</sup>-O-O-SO<sub>3</sub> configuration. This further accelerated the Cu<sup>+</sup>/Cu<sup>2+</sup> redox cycle and the generation of reactive oxygen species (ROS) (•OH, SO<sub>4</sub><sup>•−</sup>, O<sub>2</sub><sup>•−</sup>, <sup>1</sup>O<sub>2</sub>, and Cu<sup>III</sup>=O). Additionally, the Cu-N@KBC/peroxymonosulfate (PMS) system demonstrated excellent stability, universality, and resistance to interference. Notably, its integration with membrane technology demonstrated the potential of the Cu-N@KBC-cellulose acetate membrane for practical wastewater treatment applications. This study offered a fresh perspective on the adsorption mechanism and the <sup>1</sup>O<sub>2</sub>-dominant non-radical degradation pathway of Cu-N@KBC/PMS/TC system.</div></div>","PeriodicalId":356,"journal":{"name":"Journal of Environmental Management","volume":"395 ","pages":"Article 127703"},"PeriodicalIF":8.4000,"publicationDate":"2025-10-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Defect-driven bifunctional Cu/N co-doped biochar for synchronized adsorption and instant catalysis in organic pollutant degradation\",\"authors\":\"Rui Yu, Fang He, Jingjing Wang, Zaiwen Jia, Chao Liu, Haihong Zhou\",\"doi\":\"10.1016/j.jenvman.2025.127703\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>As a commonly used antibiotic in healthcare and livestock production, tetracycline (TC) remains in water bodies and poses ecological and health risks, making its efficient removal from wastewater essential. A copper (Cu) and nitrogen (N) co-doped biochar (BC) catalyst (denoted as Cu-N@KBC) was synthesized, exhibiting low energy consumption, excellent adsorption capacity, and superior catalytic performance. Cu-N@KBC achieved 35.2 % TC removal within 20 min, with the solid-liquid distribution coefficient (K<sub>d</sub>) of 4.541 L g<sup>−1</sup>, owing to its well-developed pore structure and abundant defect sites. N doping into the sp<sup>2</sup>-hybridized carbon network, synergistically coupled with uniform Cu loading, induced the formation of oxygen vacancies and surface defects, thereby creating additional active sites for TC adsorption. A maximum TC degradation of 96.5 % was achieved within 60 min under the optimized conditions. The combined incorporation of Cu and N elevated the graphitization degree (I<sub>D</sub>/I<sub>G</sub> = 0.93), optimizing electron transfer and facilitating ≡ Cu<sup>2+</sup>-O-O-SO<sub>3</sub> configuration. This further accelerated the Cu<sup>+</sup>/Cu<sup>2+</sup> redox cycle and the generation of reactive oxygen species (ROS) (•OH, SO<sub>4</sub><sup>•−</sup>, O<sub>2</sub><sup>•−</sup>, <sup>1</sup>O<sub>2</sub>, and Cu<sup>III</sup>=O). Additionally, the Cu-N@KBC/peroxymonosulfate (PMS) system demonstrated excellent stability, universality, and resistance to interference. Notably, its integration with membrane technology demonstrated the potential of the Cu-N@KBC-cellulose acetate membrane for practical wastewater treatment applications. This study offered a fresh perspective on the adsorption mechanism and the <sup>1</sup>O<sub>2</sub>-dominant non-radical degradation pathway of Cu-N@KBC/PMS/TC system.</div></div>\",\"PeriodicalId\":356,\"journal\":{\"name\":\"Journal of Environmental Management\",\"volume\":\"395 \",\"pages\":\"Article 127703\"},\"PeriodicalIF\":8.4000,\"publicationDate\":\"2025-10-22\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Environmental Management\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0301479725036795\",\"RegionNum\":2,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Environmental Management","FirstCategoryId":"93","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0301479725036795","RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
作为医疗保健和畜牧业生产中常用的抗生素,四环素(TC)残留在水体中,对生态和健康构成威胁,因此从废水中有效去除四环素至关重要。合成了一种铜(Cu)和氮(N)共掺生物炭(BC)催化剂(表示为Cu-N@KBC),该催化剂具有低能耗、优异的吸附能力和优异的催化性能。Cu-N@KBC在20 min内脱除了35.2%的TC,固液分布系数(Kd)为4.541 L g−1,这是由于其孔隙结构发育良好,缺陷位点丰富。N掺杂到sp2杂化碳网络中,与均匀的Cu负载协同耦合,诱导氧空位和表面缺陷的形成,从而为TC吸附创造了额外的活性位点。在优化后的条件下,60 min内最大降解率为96.5%。Cu和N的结合提高了石墨化程度(ID/IG = 0.93),优化了电子转移并促进了≡Cu2+-O-O-SO3的构型。这进一步加速了Cu+/Cu2+氧化还原循环和活性氧(ROS)(•OH、SO4•−、O2•−、1O2和CuIII=O)的生成。此外,Cu-N@KBC/过氧单硫酸酯(PMS)体系表现出优异的稳定性、通用性和抗干扰性。值得注意的是,它与膜技术的结合显示了Cu-N@KBC-cellulose醋酸膜在实际废水处理应用中的潜力。该研究为Cu-N@KBC/PMS/TC体系的吸附机理和o2主导的非自由基降解途径提供了新的视角。
Defect-driven bifunctional Cu/N co-doped biochar for synchronized adsorption and instant catalysis in organic pollutant degradation
As a commonly used antibiotic in healthcare and livestock production, tetracycline (TC) remains in water bodies and poses ecological and health risks, making its efficient removal from wastewater essential. A copper (Cu) and nitrogen (N) co-doped biochar (BC) catalyst (denoted as Cu-N@KBC) was synthesized, exhibiting low energy consumption, excellent adsorption capacity, and superior catalytic performance. Cu-N@KBC achieved 35.2 % TC removal within 20 min, with the solid-liquid distribution coefficient (Kd) of 4.541 L g−1, owing to its well-developed pore structure and abundant defect sites. N doping into the sp2-hybridized carbon network, synergistically coupled with uniform Cu loading, induced the formation of oxygen vacancies and surface defects, thereby creating additional active sites for TC adsorption. A maximum TC degradation of 96.5 % was achieved within 60 min under the optimized conditions. The combined incorporation of Cu and N elevated the graphitization degree (ID/IG = 0.93), optimizing electron transfer and facilitating ≡ Cu2+-O-O-SO3 configuration. This further accelerated the Cu+/Cu2+ redox cycle and the generation of reactive oxygen species (ROS) (•OH, SO4•−, O2•−, 1O2, and CuIII=O). Additionally, the Cu-N@KBC/peroxymonosulfate (PMS) system demonstrated excellent stability, universality, and resistance to interference. Notably, its integration with membrane technology demonstrated the potential of the Cu-N@KBC-cellulose acetate membrane for practical wastewater treatment applications. This study offered a fresh perspective on the adsorption mechanism and the 1O2-dominant non-radical degradation pathway of Cu-N@KBC/PMS/TC system.
期刊介绍:
The Journal of Environmental Management is a journal for the publication of peer reviewed, original research for all aspects of management and the managed use of the environment, both natural and man-made.Critical review articles are also welcome; submission of these is strongly encouraged.