浒苔生物炭/氮化碳复合材料对三嗪类除草剂的可见光催化降解性能与机制  

Degradation performance and mechanism of Enteromorpha prolifera biochar/carbon nitride composites on triazine herbicides

作　　者：刘杨 罗万麟 雷晓 张启莉 余佳敏 孙惠青[2] 孔凡玉[2] 刘雪 LIU Yang;LUO Wanlin;LEI Xiao;ZHANG Qili;YU Jiamin;SUN Huiqing;KONG Fanyu;LIU Xue(Sichuan Provincial Tobacco Company of China National Tobacco Corporation,Chengdu,610017,China;Institute of Tobacco Research,Chinese Academy of Agricultural Sciences,Qingdao,266101,China;Liangshan Branch of Sichuan Provincial Tobacco Company,Xichang,615000,China;Luzhou Branch of Sichuan Provincial Tobacco Company,Luzhou,646000,China;Guangyuan Branch of Sichuan Provincial Tobacco Company,Guangyuan,628000,China)

机构地区：[1]中国烟草总公司四川省公司,成都610017 [2]中国农业科学院烟草研究所,青岛266101 [3]四川省烟草公司凉山州公司,西昌615000 [4]四川省烟草公司泸州市公司,泸州646000 [5]四川省烟草公司广元市公司,广元628000

出　　处：《环境化学》2024年第11期3900-3908,共9页Environmental Chemistry

基　　金：中国烟草总公司四川省公司科技项目(SCYC202216);中央级公益性科研院所基本科研业务费专项(1610232024010);国家自然科学基金(31901921)资助.

摘　　要：针对聚合氮化碳(CN)材料比表面积小,光致电子-空穴重组率高的问题,本研究利用废弃浒苔,结合原位煅烧法,制备了浒苔生物炭/氮化碳复合材料(BCE/CN),用于三嗪类除草剂的催化降解.浒苔中富含的铁元素可有效提高CN对可见光的吸收利用性能,BCE/CN对西玛津、莠去津、西草净和莠灭净4种三嗪除草剂的1 h降解率分别提升43.0%、22.5%、31.0%和66.7%.高角环形暗场-扫描透射电子显微镜结果表明,Fe在复合材料中以单原子和团簇形式分布,并与CN中的N以配位键形式结合.活性物种捕获实验证明,光致空穴在除草剂降解过程中发挥决定性作用,单线态氧以及羟基自由基也一定程度参与反应.此外,系统研究了催化剂用量、除草剂初始浓度、反应温度和pH值对降解过程的影响,并在实际环境水样中评价BCE/CN的催化活性.本研究为三嗪类除草剂的高效降解提供了新方法,也为废弃生物质再利用提供了新思路.In order to solve the problems of low specific surface area and high electron-hole recombination rate of polymeric carbon nitride(CN)material,the biochar/carbon nitride composite(BCE/CN)was prepared by in-situ calcination of waste Enteromorpha prolifera and applied for catalytic degradation of triazine herbicides.Iron present in Enteromorpha prolifera effectively enhances CN’s absorption and utilization of visible light.The simultaneous degradation efficiencies of BCE/CN for simazine,atrazine,simetryne and ametryn improved 43.0%,22.5%,31.0%and 66.7%,respectively,within one hour.High angle annular dark field scanning TEM verified the presence of Fe single atom and nanocluster in BCE/CN catalyst,which were coordinated with N of CN substrate.Results of quenching experiments emphasized the prominent role of h+,and the joint contribution from 1O_(2) and·OH during degradation process.In addition,the effects of catalyst dosage,initial concentration of herbicide,reaction temperature and pH value on the degradation process were systematically studied,and the catalytic activity of BCE/CN was evaluated in actual environmental water matrices.This study provides a new method for the efficient degradation of triazine herbicides,and a new perspective for the reuse of waste biomass.

关 键 词：氮化碳 除草剂 光催化降解 机制 浒苔 

分 类 号：X592[环境科学与工程—环境工程] TB333[一般工业技术—材料科学与工程] TQ426[化学工程]