Performance and Mechanism of Contaminants Removal by Carbon Materials-Modified Zerovalent Iron

doi:10.7536/PC180726

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

Fig. 1 Illustration of the major mechanisms of contaminants removal by zero-valent iron[14]

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]

Fig. 3 Schematic illustration for the fabrication of GAC/ZVI/Pd[37]

Fig. 4 Schematic illustration for the fabrication of polystyrene resin-supported nZVI[41]

Fig. 5 Schematic illustration for the fabrication of ordered mesoporous carbon-supported nZVI[10]

Fig. 6 Schematic illustration for the fabrication of polystyrene resin-supported nZVI[46]

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]

Fig. 8 Sketch of the Fe-AC composite material Carbo-Iron and its transport in groundwater[39]

Fig. 9 Schematic illustration of the role of AC on TCE reduction by nZVI[67]

Table 1 Summary of data on the removal rate of various contaminants by bare nZVI and carbon-modified nZVI

nZVI type		Cont.	Reaction conditons	$k obs + C$ (h^-1)	$k obs - C$ (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

Table 1 Summary of data on the removal rate of various contaminants by bare nZVI and carbon-modified nZVI

nZVI type		Cont.	Reaction conditons	$k obs + C$ (h^-1)	$k obs - C$ (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

Fig. 10 Summary of the ratio of kinetic constants with and without carbon-modification for currently available data on contaminants removal by nZVI

Fig. 11 Schematic diagram of the electron-transfer processes in the reaction of Ox with ZVI/Fe(Ⅱ) open to the air[70]

Fig. 12 Proposed electron-transfer processes in Cr(Ⅵ) removal using the core-shell nZVI@C@PANI[66]

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
Surfactants	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
Synthetic polymers	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
Natural biopolymers	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

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
Surfactants	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
Synthetic polymers	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
Natural biopolymers	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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Performance and Mechanism of Contaminants Removal by Carbon Materials-Modified Zerovalent Iron

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Performance and Mechanism of Contaminants Removal by Carbon Materials-Modified Zerovalent Iron