纳米零价铁在水相反应中的表面化学和晶相转化

doi:10.6023/A18100412

化学学报 ›› 2019, Vol. 77 ›› Issue (2): 121-129.DOI: 10.6023/A18100412 上一篇下一篇

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纳米零价铁在水相反应中的表面化学和晶相转化

刘静^a,b, 顾天航^a,b, 王伟^a,c, 刘爱荣^a,b, 张伟贤^a,b

a 污染控制与资源化研究国家重点实验室上海 200092;
b 同济大学环境科学与工程学院上海 200092;
c 同济大学化学科学与工程学院上海 200092

投稿日期:2018-10-02 发布日期:2018-11-13
通讯作者: 刘爱荣,E-mail:liuairong@tongji.edu.cn E-mail:liuairong@tongji.edu.cn
作者简介:刘静,同济大学环境科学与工程学院2014级博士生,研究方向为纳米零价铁在水相中性质演变.读博期间获得多次奖学金;顾天航,同济大学环境科学与工程学院2018级博士生,研究方向为纳米零价铁富集水中稀有元素;王伟,博士,同济大学化学专业博士后,主要从事铁基纳米材料用于重金属污染控制及资源化方面的研究及实践工作,作为主要完成人之一将铁基纳米技术成功应用于复杂多金属废水处理工程,已发表SCI论文10余篇;刘爱荣,博士,硕士生导师,研究方向主要有铁基纳米材料的地球化学循环、水污染控制环境纳米材料、水环境化学理论与技术.主持国家自然科学基金项目两项,发表SCI论文10余篇.
基金资助:
项目受国家自然科学基金（Nos.41673096，41772243，51578398）和“博新计划”（BX201700172）资助.

Surface Chemistry and Phase Transformation of Nanoscale Zero-Valent Iron (nZVI) in Aquatic Media

Liu Jing^a,b, Gu Tianhang^a,b, Wang Wei^a,c, Liu Ai-rong^a,b, Zhang Wei-xian^a,b

a State Key Laboratory of Pollution Control and Resource Reuse, Shanghai 200092;
b College of Environmental Science and Engineering, Tongji University, Shanghai 200092;
c School of Chemical Science and Engineering, Tongji University, Shanghai 200092

Received:2018-10-02 Published:2018-11-13
Contact: 10.6023/A18100412 E-mail:liuairong@tongji.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 41673096, 41772243, 51578398) and National Postdoctoral Program for Innovative Talents (BX201700172).

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摘要/Abstract

纳米零价铁在水相中的表面化学特性和晶相等性质变化，将影响其反应活性及环境归趋等.总结近期课题组关于纳米零价铁在水相中表面化学和晶相转化的研究进展，为纳米零价铁污染控制化学提供基础理论.重点探讨水中有无溶解氧、不同水力学条件复氧（静态和扰动）、重金属共存、无机阴离子共存对纳米零价铁颗粒表面化学特性和晶相转变的影响.同时也研究高分子电解质表面修饰后，颗粒在水相中表面及晶相的演变及对重金属去除性能的影响.研究表明，纳米零价铁与水相中的水分子、溶解氧、重金属离子及无机阴离子反应，零价铁失去电子演变为氧化铁、羟基氧化铁等；环境条件对颗粒结构性能产生影响，从而影响污染物去除效率及其在环境中的归趋.未来研究将重点探讨结构性能动态变化与不同污染物之间反应性能的影响，建立纳米颗粒的结构与性能之间关系模型，为纳米零价铁材料的环境应用提供理论依据.

关键词: 纳米零价铁, 水相, 纳米零价铁, 水相, 表面化学, 晶相, 表面化学, 晶相, 性质转化, 性质转化

The unique "core-shell" structure endows nanoscale zero-valent iron (nZVI) rich aquatic surface chemistry properties. Transformation of surface chemistry and crystal phase of nZVI affect its reactivity and environmental transport and fate. Recent advances on the surface chemistry and phase transformation of nZVI in aqueous media are highlighted in this paper focusing on a basic theory of nZVI for pollution control and environmental application. Surface chemistry and phase of both fresh and reacted nZVI are presented. The structure, composition and properties of nanoparticles are determined not only by reaction time but also by environmental conditions. Specifically, the influences of dissolved oxygen, hydraulic conditions (static and stirring), types and concentrations of heavy metals (U(VI), Cr(VI), Se(IV)) and anions (NO₃^-, SO₄^2-, HPO₄^2- and HCO₃^-) are investigated. In addition, the effect of surface modification with polyelectrolytes, including anionic polyacrylamide (APAM) and carboxymethylcellulose sodium (CMC), on microstructure, morphology and composition of nanoparticles in aqueous phase was discussed. Results demonstrate that environmental conditions have significant impacts on particles structure, composition and properties, consequently on nZVI performance for pollutant removal. After corrosion under different aqueous conditions, the core-shell structured nZVI are distorted and the metallic iron core is transformed into different iron oxides/hydroxides, such as γ-Fe₂O₃, Fe₃O₄ and γ-FeOOH. These iron (hydr)oxides exhibit different surface complexation and affinity proprieties, thus eventually affecting the pollutant removal performance and the environmental fate of reaction products. More research on the effect of dynamic structure transformation by different types of pollutants, and a reaction model between the surface chemistry/phase transformation and removal performance are needed to deepen our understanding on nZVI surface chemistry, and develop more effective technologies of environmental applications.

Key words: nanoscale zero-valent iron, aquatic media, nanoscale zero-valent iron, aquatic media, surface chemistry, crystal phase, surface chemistry, crystal phase, transformation, transformation

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刘静, 顾天航, 王伟, 刘爱荣, 张伟贤. 纳米零价铁在水相反应中的表面化学和晶相转化[J]. 化学学报, 2019, 77(2): 121-129.

Liu Jing, Gu Tianhang, Wang Wei, Liu Ai-rong, Zhang Wei-xian. Surface Chemistry and Phase Transformation of Nanoscale Zero-Valent Iron (nZVI) in Aquatic Media[J]. Acta Chim. Sinica, 2019, 77(2): 121-129.

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纳米零价铁在水相反应中的表面化学和晶相转化

Surface Chemistry and Phase Transformation of Nanoscale Zero-Valent Iron (nZVI) in Aquatic Media

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