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铁锰二元氧化物改性粉煤灰对地下水中砷的吸附特性OA北大核心CSTPCD

Adsorption properties of fly ash modified with Fe-Mn binary oxide on As(Ⅴ)/As(Ⅲ)in the groundwater

中文摘要英文摘要

在我国内陆盆地和河流三角洲广泛分布着高砷地下水,吸附法作为一种简单而高效的除砷方法得到广泛的应用,但大多数吸附材料对As(Ⅲ)的吸附能力弱于As(Ⅴ),因此开发具有氧化和吸附耦合作用的高效吸附剂具有积极意义.采用共沉淀法制备铁锰二元氧化物改性粉煤灰(FMFA),探究其对As(Ⅲ)/As(Ⅴ)的吸附性能及吸附机理;通过批实验探究FMFA对溶液中As(Ⅲ)/As(Ⅴ)的吸附性能,采用XRD、SEM、BET等表征分析其表面形貌和结构,利用XPS和FT-IR分析吸附前后FMFA表面元素和官能团变化.结果表明:铁、锰氧化物均以不定形相负载于粉煤灰表面,极大地提高了FMFA的比表面积(可达166.77 m2/g),为As(Ⅲ)/As(Ⅴ)的吸附提供了更多的活性位点;FMFA在中性条件下对As(Ⅲ)和As(Ⅴ)的理论最大吸附容量分别为68.19 mg/g和24.42 mg/g,As(Ⅲ)/As(Ⅴ)的吸附等温线模型均符合Freundlich模型,As(Ⅴ)的吸附过程遵循准二级动力学模型,As(Ⅲ)的吸附过程更符合Elovich模型;在溶液初始pH=5~9范围内FMFA的稳定性较好,初始pH>9的碱性环境不利于As(Ⅴ)/As(Ⅲ)的吸附;水中常见共存含氧阴离子对As(Ⅲ)/As(Ⅴ)竞争吸附影响大小的顺序为PO43-->HCO3->SO42-;FMFA可有效去除地下水样品中的砷,且不会造成铁、锰二次污染,同时具有良好的回收再生能力;在FMFA吸附As(Ⅲ)的过程中二氧化锰主要起氧化作用,铁氧化物起吸附作用,砷通过与FMFA表面金属活性羟基配体交换形成内球络合物而被吸附.本文成功制备了可高效去除地下水中As(Ⅲ)/As(Ⅴ)的绿色经济的新型吸附剂,对保障居民饮用水安全具有重要意义.

High arsenic groundwater is widely distributed in inland basins and river deltas in China,and ad-sorption method has been widely used as a simple and efficient method for arsenic removal.However,the adsorption capacity of most adsorbents for As(Ⅲ)is weaker than that of As(Ⅴ),so it is of positive signifi-cance to develop efficient adsorption with the coupling effect of oxidation and adsorption.The fly ash modi-fied with Fe-Mn binary oxide(FMFA)was prepared by co-precipitation,and its adsorption properties and mechanism for As(Ⅲ)/As(Ⅴ)were studied.The adsorption performance of FMFA on As(Ⅲ)/As(Ⅴ)in solution was investigated by batch experiment.The surface morphology and structure of FMFA were ana-lyzed by XRD,SEM and BET,and the changes of elements and functional groups on FMFA surface before and after adsorption were analyzed by XPS and FT-IR.The experimental results show that both the Fe oxide and Mn oxide are loaded on the surface of fly ash in amorphous form,which greatly increases the spe-cific surface area of FMFA(up to 166.77 m2/g),and provides more active sites for As(Ⅲ)/As(Ⅴ)adsorp-tion.In neutral condition,the adsorption capacities of FMFA for As(Ⅲ)and As(Ⅴ)are 68.19 mg/g and 24.42 mg/g,and the adsorption isotherm model of As(Ⅲ)/As(Ⅴ)conforms to Freundlich model.The ad-sorption process of As(Ⅴ)follows the qseudo-second-order kinetic model,and the As(Ⅲ)is more consis-tent with the Elovich model.The alkaline environment with initial pH>9 is not conductive to the adsorp-tion of As(Ⅲ)/As(Ⅴ)by FMFA which is more stable in the range of initial pH=5~9.The effect of the coexisting oxygen-containing anions on competitive adsorption of As(Ⅲ)/As(Ⅴ)in water is PC43->HCO3>SO2-.FMFA can effectively remove arsenic from groundwater samples without causing seconda-ry pollution of iron and manganese,and has good recycling capacity.During the adsorption of As(Ⅲ)by FMFA,manganese dioxides mainly plays the role of oxidation and iron oxide plays the role of adsorption,and arse-nic is adsorbed by exchanging with metal active hydroxyl groups on the FMFA surface to form inner complex.This paper has successfully prepared a new green economic adsorbent which can effectively remove As(Ⅲ)/As(Ⅴ)from groundwater,which is of great significance to ensure the safety of drinking water for residents.

王丽楠;杨保国;谢作明;李树才;张峰

中国地质大学(武汉)环境学院,湖北武汉 430078中国地质大学(武汉)环境学院,湖北武汉 430078||宁夏回族自治区地球物理地球化学调查院(自治区深地探测中心),宁夏银川 750001中国地质大学(武汉)环境学院,湖北武汉 430078||中国地质大学(武汉)生物地质与环境地质国家重点实验室,湖北武汉 430078宁夏回族自治区地球物理地球化学调查院(自治区深地探测中心),宁夏银川 750001

环境科学

高砷地下水改性粉煤灰铁锰二元氧化物吸附

high arsenic groundwatermodified fly ashFe-Mn binary oxideadsorption

《安全与环境工程》 2024 (004)

201-212 / 12

宁夏自然科学基金项目(2020AAC03448);国家自然科学基金面上项目(41572230);国家自然科学基金创新研究群体项目(41521001)

10.13578/j.cnki.issn.1671-1556.20230475

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