首页|期刊导航|环境工程学报|废弃芦苇衍生生物炭中碱性氮位点的限域调控对过二硫酸盐非自由基路径的影响

废弃芦苇衍生生物炭中碱性氮位点的限域调控对过二硫酸盐非自由基路径的影响OA

Effect of confined regulation of alkaline nitrogen sites in waste reed-derived biochar on the non-radical pathway of peroxydisulfate

中文摘要英文摘要

腐殖酸(humic acid,HA)作为污水深度处理中的典型难降解有机物,对其进行有效去除一直是研究难点.过硫酸盐高级氧化技术中,非自由基主导的氧化路径比传统的自由基氧化路径更能有效地利用氧化剂,通过优化活化途径,可实现对非自由基路径的定向精准调控.然而,碱性氮位点设计对非自由基氧化路径的调控机制尚未完全被阐明.本研究以废弃芦苇为前驱体构建氮掺杂生物炭(nitrogen-doped biochar,N@BAC),通过活化过二硫酸盐(peroxydisulfate,PDS)实现HA的高效降解,重点揭示了氮物种对非自由基氧化路径的调控规律.结果表明,氮掺杂使生物炭形成层状褶皱结构,比表面积提升至 409.60 m2∙g-1,其中吡啶N和吡咯N相对含量增加了近 8倍.在N@BAC/PDS体系中HA可实现完全去除.N@BAC中的碳骨架在该体系中起到了对比表面积、孔隙度和活性位点的支撑作用.密度泛函理论计算结果表明,吡啶N和吡啶N的引入改变了局部电荷分布,将电子转移路径贡献率由 4%提升至21%,从而大幅提升了系统的反应动力学性能.以上研究结果可为PDS 活化反应性能提升提供新策略,同时也可为水生植物资源化利用开辟新路径.

Humic acid(HA),as a typical refractory organic compound in advanced wastewater treatment,poses a persistent challenge for effective removal.In persulfate-based advanced oxidation processes,the non-radical oxidation pathway demonstrates higher efficiency in oxidant utilization compared to conventional radical oxidation pathways.By optimizing activation strategies,targeted and precise regulation of the non-radical pathway can be achieved.However,the regulatory mechanism of alkaline nitrogen sites on the non-radical oxidation pathway has not yet been fully elucidated.In this study,waste reed was used as a precursor to synthesize nitrogen-doped biochar(N@BAC),which effectively activated peroxydisulfate(PDS)to achieve efficient degradation of HA.The research focused on elucidating the regulatory role of nitrogen species in the non-radical oxidation pathway.Results showed that nitrogen doping induced a layered wrinkled structure in the biochar,increasing the specific surface area to 409.60 m2∙g-1,while the relative content of pyridinic N and pyrrolic N increased nearly eightfold.In the N@BAC/PDS system,complete removal of HA was achieved.The carbon framework in N@BAC provided essential support for specific surface area,porosity,and active sites.Density functional theory calculations revealed that the introduction of pyridinic N and pyrrolic N altered the local charge distribution,increasing the electron transfer pathway contribution from 4%to 21%,thereby significantly enhancing the reaction kinetics of the system.These findings offer a novel strategy for improving PDS activation performance and open up new avenues for the resource utilization of aquatic plants.

张晨;武浩浩;张伟;李剑锋

山西财经大学资源环境学院,太原 030006山西大学资源与环境学院,太原 030006山西大学资源与环境学院,太原 030006山西大学资源与环境学院,太原 030006

资源环境

氮位点过二硫酸盐非自由基活化电子转移过程腐殖酸生物炭

nitrogen sitesperoxydisulfatenon-radical activationelectron transfer processhumic acidbiochar

《环境工程学报》 2026 (2)

376-388,13

国家自然科学基金资助项目(22106096)山西省基础研究计划面上资助项目(202403021221215)

10.12030/j.cjee.202505051

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