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王舒畅, 宋亚丹, 孙远奎. 碳基材料修饰零价铁去除污染物的效能与机理[J]. 化学进展, 2019, 31(2/3): 422-432.
Shuchang Wang, Yadan Son, Yuankui Sun. Performance and Mechanism of Contaminants Removal by Carbon Materials-Modified Zerovalent Iron[J]. Progress in Chemistry, 2019, 31(2/3): 422-432.
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。
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nZVI type | Cont. | Reaction conditons | (h-1) | (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 |
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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