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化学进展 2019, Vol. 31 Issue (2/3): 422-432 DOI: 10.7536/PC180726 前一篇   后一篇

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碳基材料修饰零价铁去除污染物的效能与机理

王舒畅1,2, 宋亚丹1,2, 孙远奎1,2,**()   

  1. 1. 同济大学环境科学与工程学院 污染控制与资源化研究国家重点实验室 上海 200092
    2. 上海污染控制与生态安全研究院 上海 200092
  • 收稿日期:2018-07-21 出版日期:2019-02-15 发布日期:2018-12-20
  • 通讯作者: 孙远奎
  • 基金资助:
    国家自然科学基金项目(21876129); 国家自然科学基金项目(51608431)
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Performance and Mechanism of Contaminants Removal by Carbon Materials-Modified Zerovalent Iron

Shuchang Wang1,2, Yadan Son1,2, Yuankui Sun1,2,**()   

  1. 1. State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, Shanghai 200092, China
    2. Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
  • Received:2018-07-21 Online:2019-02-15 Published:2018-12-20
  • Contact: Yuankui Sun
  • About author:
    ** E-mail:
  • Supported by:
    National Natural Science Foundation of China(21876129); National Natural Science Foundation of China(51608431)

纳米零价铁(nZVI)因具有良好的还原活性及吸附性能,在土壤和地下水修复中具有广阔的应用前景。然而由于高表面能及固有磁力等因素的影响,nZVI易团聚而导致迁移性、反应活性降低,制约了其推广应用。研究表明利用表面活性剂、高分子聚合物对nZVI进行表面修饰或将nZVI负载于多孔碳材料上均可提高nZVI的分散性和稳定性。鉴于此,本文系统总结比较了不同碳材料修饰nZVI的方法,分析了不同修饰方法对nZVI迁移性、反应活性及选择性(即电子效率)的影响规律与机制。迁移性及选择性是制约nZVI实际应用的瓶颈因素,羧甲基纤维素、淀粉等高分子聚合物及活性炭等多孔材料均能在一定程度上提高nZVI的迁移性及选择性,然而提升程度及相关机理仍有待明确,是今后的研究热点方向。

关键词： 碳基材料, 零价铁, 反应活性, 选择性, 稳定性

Nanoscale zero-valent iron(nZVI) is always considered to be a promising technology for water and soil remediation, due to its high reactivity and good adsorption ability. However, given the high surface energy and intrinsic magnetic interactions, unstabilized nZVI tends to aggregate and thus causes poor mobility and lower reactivity, which limits its further development and application. To address these issues, prior and ongoing research efforts have provided several promising strategies that can potentially improve the performance of nZVI. Among of them, carbon based materials such as surfactants, polymers and porous carbon materials are commonly used to modify the surface properties of nZVI, considering carbon based materials always have superior adsorption ability, stability, electron conductivity, etc. Accordingly, this review comprehensively summarizes the modification methods with different carbon materials. Moreover, the influence of surface modification on the mobility, reactivity and especially the selectivity(electron efficiency) of nZVI is discussed in detail. It can be concluded that, for the successful application of nZVI, the mobility and selectivity of nZVI are still the bottleneck factors, although they can be enhanced by the modification with carboxymethyl cellulose, starch, activated carbon and also other carbon based materials. Therefore, future research may attempt to explore some more effective modification methods, such as with the combination of different carbon materials, to improve the mobility and selectivity of nZVI.

Key words: carbon materials, zero-valent iron, reactivity, selectivity, stability
()
图1 零价铁体系去除污染物的主要机理示意图[14]
Fig. 1 Illustration of the major mechanisms of contaminants removal by zero-valent iron[14]
图2 包覆型纳米零价铁的制备及稳定机理示意图(a)改变表面电荷以引起颗粒互斥,(b)构建网格结构以提供空间位阻[30]
Fig. 2 Schematic representation of(a) surface modification stabilization(where surface coating facilitates particle repulsion), and(b) network stabilization(where a medium network is formed due to hydrogen bonding and polymer entanglements)[30]
图3 活性炭负载纳米铁钯双金属的合成示意图[37]
Fig. 3 Schematic illustration for the fabrication of GAC/ZVI/Pd[37]
图4 聚苯乙烯负载纳米零价铁的合成示意图[41]
Fig. 4 Schematic illustration for the fabrication of polystyrene resin-supported nZVI[41]
图5 有序介孔碳负载纳米零价铁的合成示意图[10]
Fig. 5 Schematic illustration for the fabrication of ordered mesoporous carbon-supported nZVI[10]
图6 石墨烯负载纳米零价铁的合成示意图[46]
Fig. 6 Schematic illustration for the fabrication of polystyrene resin-supported nZVI[46]
图7 CMC/nZVI在不同距离监测井处随时间的迁移分布情况[50]。黄色、黑色分别代表被氧化后的CMC/nZVIox及未反应的CMC/nZVI,颜色的深浅示意浓度的高低
Fig. 7 Composite photograph of water samples taken from the first three sample wells over the time period of the injection test. Rectangular markers highlight the location of the two color transitions that indicate breakthrough of CMC/nZVIox(yellow) and CMC/nZVI(black)[50]
图8 Carbo-Iron?的结构示意及其在地下水中的迁移情况[39]
Fig. 8 Sketch of the Fe-AC composite material Carbo-Iron and its transport in groundwater[39]
图9 活性炭在nZVI去除TCE中的吸附与电子传递作用[67]
Fig. 9 Schematic illustration of the role of AC on TCE reduction by nZVI[67]
表1 碳材料修饰对nZVI去除不同污染物速率常数的影响
Table 1 Summary of data on the removal rate of various contaminants by bare nZVI and carbon-modified nZVI
nZVI type Cont. Reaction conditons kobs+C(h-1) kobs-C(h-1) ref
Coated nZVI CMC TCE TCE=50 mg/L, Fe0=0.1 g/L,0.1%Pd, CMC90 K 0.381 0.022 54
TCE=50 mg/L, Fe0=0.1 g/L,0.1%Pd, CMC250 K 0.557 0.022
TCE=50 mg/L, Fe0=0.1 g/L,0.1%Pd, CMC700 K 0.497 0.022
PVP TCE=50 mg/L, Fe0=0.1 g/L,0.1%Pd, PVP360 K 0.219 0.022
GG TCE=50 mg/L, Fe0=0.1 g/L,0.1%Pd, GG 0.05% 0.051 0.022
CMC TCE TCE=50 mg/L, Fe0=0.1 g/L 7.4 0.44 27
Starch TCE TCE=25 mg/L, Fe0=0.1 g/L 0.11 0.034 55
TCE=25 mg/L, Fe0=0.1 g/L, 0.1%Pd 3.7 0.9
PCB PCB=2.5 mg/L, Fe0=0.1 g/L, 0.1%Pd 0.029 0.017
CMC Pb(Ⅱ) Pb(Ⅱ)=200 mg/L, Fe0=0.75 g/L, pH=5.0 1.12 0.204 56
Starch Pb(Ⅱ)=200 mg/L, Fe0=0.75 g/L, pH=5.0 1.46 0.204
Agar Pb(Ⅱ)=200 mg/L, Fe0=0.75 g/L, pH=5.0 5.60 0.204
CMC NO3- NO3-=200 mg/L, Fe0=0.7 g/L, pH=~7.0 7.8 1.5 57
CMC ClO4- ClO4-=10 mg/L, Fe0=1.8 g/L, pH=~7.0, 110 ℃ 0.33 0.18 58
Starch ClO4-=10 mg/L, Fe0=1.8 g/L, pH=~7.0, 110 ℃ 0.984 0.1
Supported nZVI Graphene oxide CT CT=3 mg/L, Fe0=0.5 g/L, pH=5.5, T=10 ℃ 1.308 0.834 46
CT=3 mg/L, Fe0=0.5 g/L, pH=5.5, T=20 ℃ 2.166 1.404
CT=3 mg/L, Fe0=0.5 g/L, pH=5.5, T=30 ℃ 2.844 2.292
CT=3 mg/L, Fe0=0.5 g/L, pH=5.5, T=35 ℃ 3.618 2.862
CT=3 mg/L, Fe0=0.5 g/L, pH=5.5, T=40 ℃ 4.776 3.342
GAC TCE TCE=80 mg/L, Fe0=0.15 g/L, GAC-105 ℃ 339.6 9 36
TCE=80 mg/L, Fe0=0.15 g/L, GAC-700 ℃ 374.4 9
AC BrO3- BrO3-=0.2 mg/L, Fe0=5 g/L, pH=~7.0 13.62 8.84 59
BrO3-=0.2 mg/L, Fe0=5 g/L, pH=~7.0 29.4 8.84
BrO3-=0.2 mg/L, Fe0=5 g/L, pH=~7.0 36.7 8.84
Graphene oxide Cr(Ⅵ) Cr(Ⅵ)=25 mg/L, Fe0=1.0 mg/L 4.38 1.56 60
图10 碳材料修饰对nZVI去除不同污染物反应速率的影响
Fig. 10 Summary of the ratio of kinetic constants with and without carbon-modification for currently available data on contaminants removal by nZVI
图11 活性炭在nZVI去除TCE中的吸附与电子传递作用[70]
Fig. 11 Schematic diagram of the electron-transfer processes in the reaction of Ox with ZVI/Fe(Ⅱ) open to the air[70]
图12 核壳结构nZVI@C@PANI去除Cr(Ⅵ)过程中的电子传递机制[66]
Fig. 12 Proposed electron-transfer processes in Cr(Ⅵ) removal using the core-shell nZVI@C@PANI[66]
表2 典型碳材料修饰nZVI效果的比较
Table 2 Summary of the effects of typical carbon materials on modifying nZVI
Carbon-based materials Key properties Remarks ref
Surfactants SDBS Anionic surfactants electrostatic repulsion Relative weak stabilization effect; limited transportability in real soil; the introduced surfactants in the subsurface may solubilize/mobilize non-targeted contaminants 33
Tween 20 Nonionic surfactant Network stabilization 34
Synthetic polymers CMC Food grade polysaccharide. Nontoxic and biodegradable. Weak anionic functional groups(pKa=4.3). MW=90 or 700 kDa. CMC binds with nZVI through bidentate bridging. Very effective stabilization effect; better transportability than surfactant-coated nZVI; no enhancing effect on nZVI selectivity 23, 35, 40, 49, 50
PVP Neutral polyelectrolyte. MW=40 or 360 kDa. Less effective than CMC; may enhance transportability of nZVI; no enhancing effect on nZVI selectivity 54
Natural biopolymers Starch Neutral polysaccharide. nZVI-starch interactions and formation of intrastarch Fe clusters play a fundamental role in stabilizing nZVI. Effective stabilization effect; may enhance transportability of nZVI; no enhancing effect on nZVI selectivity 55, 58
Guar gum Neutral polysaccharide. It binds with nZVI via the hydroxyl groups. More effective stabilization effect than starch; may enhance transportability of nZVI; no enhancing effect on nZVI selectivity 54, 56
Solid supports AC Highly porous internal structure; ideal adsorption property. Ideal supports or vehicles for stabilizing and delivering nZVI into porous media; Carbo-Iron? could highly enhance ZVI selectivity; inexpensive 25, 39
Mesoporous carbon Ordered mesoporous carbon, high surface area, good electroconductivity. Good supports for stabilizing and delivering nZVI into porous media; may enhance ZVI selectivity; expensive 10, 43
Graphene oxide Consisting of a single layer of carbon atoms arranged in a hexagonal lattice. Good supports for stabilizing and delivering nZVI into porous media; could enhance ZVI reactivity and selectivity; expensive 45, 46
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