不同碳源的生物质炭-磷化铁/零价铁的制备及对水中3,4,5,6-四氯吡啶-2-羧酸的去除  

Preparation of biochar-iron phosphide/zero-valent iron with different carbon sources and removal of 3,4,5,6-Tetrachloropyridine-2-carboxylic acid from water solution

作　　者：靳惠文 张小乐 牛红云[2] 蔡亚岐[2] JIN Huiwen;ZHANG Xiaole;NIU Hongyun;CAI Yaqi(School of Life Science,North China University of Science and Technology,Tangshan,063210,China;State Key Laboratory of Environmental Chemistry and Ecotoxicology,Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,Beijing,100085,China)

机构地区：[1]华北理工大学生命科学学院,唐山063210 [2]环境化学与生态毒理学国家重点实验室,中国科学院生态环境研究中心,北京100085

出　　处：《环境化学》2024年第9期2998-3008,共11页Environmental Chemistry

基　　金：国家自然科学基金(22036007,22276207);河北省自然科学基金(B2020209005)资助.

摘　　要：改性生物炭材料在环境污染物去除中的应用越来越广泛.本文以鸡粪(CM)、咖啡渣(CG)、活性污泥(SL)等3种废弃生物质为碳源,制备了3种生物质炭-磷化铁/零价铁复合材料(BC-Fe_(x)P/Fe).这些材料主要由生物质炭、磷酸铁、磷化铁、零价铁或碳化铁及氧化铁组成.用于降解水中的3,4,5,6-四氯吡啶-2-羧酸(TCPA)时,以活性污泥为碳源的SL-Fe_(x)P/Fe材料对TCPA的去除效果明显优于以鸡粪为碳源的CM-Fe_(x)P/Fe和以咖啡为碳源的CG-Fe_(x)P/Fe材料,而且SL-Fe_(x)P/Fe对TCPA的降解受pH影响较小.在中性pH反应6 h后,CM-Fe_(x)P/Fe、CG-Fe_(x)P/Fe和SL-Fe_(x)P/Fe对10 mg·L^(-1)的TCPA的降解率分别为90.1%、71.1%和100%,矿化率分别为33.25%、22.61%和64.27%.掩蔽实验和电子自旋共振(ESR)结果表明,SL-Fe_(x)P/Fe体系存在多种活性氧物质.使用前后材料的X射线晶体衍射和X射线光电子能谱分析,材料中的Fe_(x)P、Fe3C、Fe和氮掺杂生物质炭均在有机污染物的降解过程中发挥了作用.Modified biochar materials are more and more widely used in the removal of environmental pollutants.In this study,several biochar-iron phosphide/zero-valent iron composites(BC-Fe_(x)P/Fe)were prepared with chicken manure(CM),coffee grounds(CG)or activated sludge(SL)as carbon source.These materials were mainly composed of biochar,iron phosphate,zero-valent iron or iron carbide and iron oxide.When used for the degradation of 3,4,5,6-tetrachloropyridine-2-carboxylic acid(TCPA)from water,the removal efficiency of TCPA by SL-Fe_(x)P/Fe with activated sludge as carbon source was better than that by CM-Fe_(x)P/Fe with chicken manure as carbon source and CG-Fe_(x)P/Fe with coffee ground as carbon source.Furthermore,the degradation of TCPA by SL-Fe_(x)P/Fe was less affected by pH than those by CM-Fe_(x)P/Fe and CG-Fe_(x)P/Fe.At neutral pH,the degradation percentage of TCPA(10 mg·L^(-1))by CM-Fe_(x)P/Fe,CG-Fe_(x)P/Fe and SL-Fe_(x)P/Fe were 90.1%,71.1%and 100%,and the mineralization efficiency was 33.25%,22.61%and 64.27%,respectively within 6h.The masking experiments and electron spin resonance(ESR)results showed the coexistence of various active oxygen species in SL-Fe_(x)P/Fe system.X-ray diffraction and X-ray photoelectron spectroscopy analysis of the fresh and used materials suggested that Fe_(x)P,Fe3C,Fe and nitrogen-doped biochar in the materials all played roles during the degradation of organic pollutants.

关 键 词：废弃生物质 改性生物炭 复合材料 3 4 5 6-四氯吡啶-2-羧酸 

分 类 号：X-1[环境科学与工程] O6[理学—化学]