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化学进展 2022, Vol. 34 Issue (9): 2081-2093 DOI: 10.7536/PC211102 前一篇   后一篇

• 综述 •

铁基材料改性零价铝的作用机制及应用

杨世迎1,2,3,*(), 李乾凤3, 吴随3, 张维银3   

  1. 1 海洋环境与生态教育部重点实验室 青岛 266100
    2 山东省海洋环境地质工程重点实验室 青岛 266100
    3 中国海洋大学环境科学与工程学院 青岛 266100
  • 收稿日期:2021-11-03 修回日期:2022-01-24 出版日期:2022-09-20 发布日期:2022-04-01
  • 基金资助:
    山东省自然科学基金项目(ZR2020MB093)
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Mechanisms and Applications of Zero-Valent Aluminum Modified by Iron-Based Materials

Shiying Yang1,2,3(), Qianfeng Li3, Sui Wu3, Weiyin Zhang3   

  1. 1 The Key Laboratory of Marine Environment & Ecology, Ministry of Education,Qingdao 266100, China
    2 Shandong Provincial Key Laboratory of Marine Environment and Geological Engineering (MEGE),Qingdao 266100, China
    3 College of Environmental Science and Engineering, Ocean University of China,Qingdao 266100, China
  • Received:2021-11-03 Revised:2022-01-24 Online:2022-09-20 Published:2022-04-01
  • Contact: *e-mail: ysy@ouc.edu.cn
  • Supported by:
    Natural Science Foundation of Shandong Province(ZR2020MB093)

近年来,零价铝(Zero-Valent Aluminum,ZVAl)因其具有极低的氧化还原电位、是优良的电子供体等化学特性,已被广泛地用于水中污染物的去除;但因其表面致密的氧化膜会阻碍其活性释放,并且在反应中表面易形成(氢)氧化物而造成二次钝化,从而导致其反应寿命短。研究表明,零价铁、铁矿石、含铁黏土矿物等铁基材料与ZVAl复合后可克服ZVAl自身的弊端,除了可以改变ZVAl的硬度、磁性等物理性能外,更有意义的是,可以通过:1)加快反应速率、2)拓宽pH范围、3)延长反应持久性、4)增强反应选择性等化学作用机制实现提高其去除水中污染物效能的目的。因此,本文在系统总结不同方法下铁基材料对ZVAl的改性机制(即发生氧化还原反应、金属间的反应或是自蔓延反应)的基础上,重点对该改性作用在去除水中污染物时的增强机制,以及进一步的优化策略(引入第三金属、外加非金属单质、添加聚合物、投加配体和构建负载物等)进行了详细综述;并对铁基材料改性ZVAl后构筑的复合材料值得深入研究的方向进行了展望,以期推动ZVAl水处理新技术在环境领域更深入的研究和更广泛的应用。

关键词： 零价铝, 铁基材料, 表面修饰, 水处理, 污染物去除, 增强机制

In recent years, zero-valent Aluminum (ZVAl) has been widely used for contaminants removal in water due to its extremely low redox potential and being an excellent electron donor. However, the dense oxide film on its surface restrains the activity of ZVAl, and it is easy to form Al-(hydr)oxide on its surface during the reaction, resulting in a secondary passivation and a short reacting life for ZVAl. The research shows that ZVAl could overcome its own disadvantages after compounded with iron-based materials such as zero-valent iron, iron ore and iron-containing clay minerals. Besides changing the physical properties such as hardness and magnetism of ZVAl, it is more meaningful that its efficiency for pollutants removal from water through chemical mechanisms is improved, such as 1) speeding up the reaction rate, 2) broadening pH ranges, 3) promoting durability, and 4) enhancing reaction selectivity. Therefore, on the basis of systematically summarizing the combining mechanisms between iron-based materials and ZVAl (i.e., redox reaction, intermetallic reaction or self-propagating reaction) under different synthetic methods, this review mainly focuses on the enhancing mechanisms of ZVAl composites modified by iron-based materials for pollutants removal in water, and further on the optimization strategies such as introducing a third metal, adding non-metallic elements, polymer or ligand, and constructing a load in detail. Finally, the research direction of ZVAl composites modified by iron-based materials is prospected in order to promote further research and wider application in environmental field for the novel ZVAl based water or wastewater technology.

Contents

1 Introduction

2 Combining mechanism between iron-based materials and ZVAl

2.1 Redox reaction

2.2 Intermetallic reaction

2.3 Self-propagating reaction

3 Strengthening mechanism of ZVAl composites modified by iron-based materials in water treatment application

3.1 Speeding up the reaction rate

3.2 Widening pH ranges

3.3 Promoting durability

3.4 Enhancing reaction selectivity

4 Optimization strategies of ZVAl composites modified by iron-based materials for removing contaminants from water

4.1 Introducing a third metal

4.2 Adding non-metallic elements

4.3 Adding polymer

4.4 Adding ligand

4.5 Constructing a load

5 Conclusions and outlook

Key words: zero-valent aluminum, iron-based materials, surface modification, water treatment, contaminant removal, enhancing mechanisms
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表1 基于不同反应机制合成铁改性ZVAl-复合材料的优缺点汇总
Table 1 Typical cases study on different synthesis reaction mechanisms of ZVAl composites modified by iron-based materials.
Reaction mechanism Methods Advantage Disadvantage ref
Redox reaction Chemical deposition/Co-reduction The nucleation and growth process of composites can be controlled by adjusting the reaction parameters
Controllable structure (core/shell, heterostructure, intermetallic compound or alloy), composition, size and morphology		 Wasted chemical reagent
Secondary pollution
Non-uniform distribution of the second metal on the surface of the core metal
Weak combination of the two metals		 29,38,43,44
Electroless plating
method		 Uniform dispersion, good coating effect Poor density of the coating layer 41
Mechanical ball
milling		 Mild reaction conditions
Simple process
Easily realized in projects		 Uncontrollable structure and composition 45,46
Intermetallic reaction Mechanical ball
milling		 Mild reaction conditions
Simple process
Easily realized in projects		 Expensive and enormous energy consumption to maintain extreme reaction conditions
Lower production rate		 30,47
Gas atomization To generate powders of circular form and good flowing properties Complicated apparatus and yields products in a small amount 48,49
Plasma technique Shortened catalyst preparation time
Low energy requirements
Highly distributed active species are produced
Production of uniform metal particle size		 Complex methods cannot be applied on industrial scale
Catalyst deactivation problem		 50,51
Melt method Iron oxide film is not easily formed on the surface of the material, and the alloy material remains active High-temperature heating and annealing for long periods of time
Difficult to obtain composites with high surface areas		 52⇓~54
Self-propagating reaction Mechanical ball
milling/Friction stir
processing		 The generated frictional heat and severe plastic deformation to increase the extent and rate of in situ reactions Expensive and enormous energy consumption 55
图1 (a) ZVAl和 (b) Fe/Al双金属材料的SEM图以及EDS光谱[39]
Fig. 1 SEM images and EDS spectra of (a) ZVAl and (b) Fe/Al bimetallic particles[39]
图2 Fe2O3在Al颗粒上的涂层方案[42]
Fig. 2 Scheme of Fe2O3 coating on Al particles.[42]
图3 Al包Fe、Fe包Al双金属的示意图[23]
Fig. 3 Diagram of the Al/Fe and Fe/Al[23]
图4 mZVAl(a-a')及Fe-mZVAlbm(b-b')的SEM图及相应EDS分析[46]
Fig. 4 SEM images and respective EDS analyses of mZVAl (a-a″) and Fe-mZVAlbm (b-b″)[46]
图5 Al-Fe合金的XRD图[62]
Fig. 5 The XRD analysis of Al-Fe alloys.[62]
图6 Fe/Al去除Cr(VI)示意图[37]
Fig. 6 Schematic mechanisms of the Cr(VI) removal by Fe/Al[37]
图7 Fe/Al双金属颗粒去除亚砷酸盐和砷酸盐的机理[44]
Fig. 7 Arsenite and arsenate removal mechanism by Fe/Al bimetallic particles[44]
图8 铜催化的铝铁合金颗粒产生原子氢[76]
Fig. 8 The reduction of atomic hydrogen by Al-Fe alloy particles catalyzed by copper[76]
图9 EDTA在Al-Fe-O2体系中参与的反应方程式图[92]
Fig. 9 The main reaction equations of EDTA involved in the Al-Fe-O2[92]
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