Research progress in the removal of water pollutants by carbon-based materials via electrooxidation

doi:10.11949/0438-1157.20230135

Abstract

Abstract:

Electrode materials are the key to electro-oxidation technology. Carbon-based materials have the advantages of good stability, adjustable structure, good conductivity, and wide range of sources. Starting from the electrooxidation process of carbon-based materials, this article briefly introduces the degradation behavior of carbon materials under anode current and their ability to enhance free radical generation by composite active materials. The research progress of carbon based materials, such as carbon nanotubes, graphene, and biomass carbon, in regulating the electrooxidation performance through defect control, surface modification, and interface engineering is systematically reviewed. Finally, the development of carbon-based anode materials is prospected.

Key words: electrochemistry, catalyst, electrooxidation, carbon-based materials, water treatment

摘要：

电极材料是电氧化技术的核心关键。碳基材料具有稳定性好、结构可调、导电性佳、来源广泛等优势。从碳基材料电氧化过程出发，简要描述了碳材料在阳极电流下的降解行为及其可复合活性材料增强自由基产生能力。重点综述了碳纳米管、石墨烯、生物质碳为代表的碳基材料通过缺陷调控、表面修饰、界面工程等方式调控电氧化性能的研究进展，最后对发展碳基阳极材料提出展望。

关键词: 电化学, 催化剂, 电氧化, 碳基材料, 水处理

CLC Number:

X 703.1

Xu GUO, Yongzheng ZHANG, Houbing XIA, Na YANG, Zhenzhen ZHU, Jingyao QI. Research progress in the removal of water pollutants by carbon-based materials via electrooxidation[J]. CIESC Journal, 2023, 74(5): 1862-1874.

郭旭, 张永政, 夏厚兵, 杨娜, 朱真珍, 齐晶瑶. 碳基材料电氧化去除水体污染物的研究进展[J]. 化工学报, 2023, 74(5): 1862-1874.

Figures/Tables 8

Table 1 Comparison of indirect oxidation （·OH mediated） and oxygen evolution reactions

项目	反应式	序号
间接氧化	$M + H 2 O → M ∙ O H + H + + e -$	（2）
间接氧化	$M · O H + R → M + p r o d u c t s$	（3）
析氧反应	$M + O H - → M ∙ O H + e -$	（4）
	$M ∙ O H + O H - → M ∙ O + H 2 O + e -$	（5）
	$M ∙ O + O H - → M ∙ O O H + e -$	（6）
	$M ∙ O O H + O H - → M + O 2 + H 2 O + e -$	（7）

Table 1 Comparison of indirect oxidation （·OH mediated） and oxygen evolution reactions

项目	反应式	序号
间接氧化	$M + H 2 O → M ∙ O H + H + + e -$	（2）
间接氧化	$M · O H + R → M + p r o d u c t s$	（3）
析氧反应	$M + O H - → M ∙ O H + e -$	（4）
	$M ∙ O H + O H - → M ∙ O + H 2 O + e -$	（5）
	$M ∙ O + O H - → M ∙ O O H + e -$	（6）
	$M ∙ O O H + O H - → M + O 2 + H 2 O + e -$	（7）

Fig.1 (a) Acid pretreated carbon nanotube sponge electro-oxidation for removal of PFOA[26]； (b) Schematic diagram of carbon nanotube/urethane sponge electrochemical filter operation[27]

Fig.2 Schematic diagram of Ni@Ni3S2/CNT electrode with nanoheterojunction structure for low energy consumption of hydrogen precipitation (cathode) and electrocatalytic removal of ethanolamine contaminants from brine (anode)[34]

Table 2 Comparison of typical carbon nanotube-based anode materials and their parameters related to degradation of pollutants

材料名称	析氧过电位	电解质	污染物	去除率/%	矿化度	活性位点	活性物种	能耗	文献
酸处理后 SWCNT海绵	—	Na₂SO₄	100 μg·L^-1 PFOA	90(60 min)	—	含氧官能团、疏水碳骨架	—	—	[26]
聚氨酯海绵负载MWCNT	—	Na₂SO₄	0.2 mmol·L^-1 TCH	92	—	—	—	5~100 kW·h·kg^-1	[27]
聚氨酯海绵负载MWCNT	—	Na₂SO₄	0.06 mmol·L^-1 MO	94	—	—	—	—	[27]
CNT-EO	—	Na₂SO₄	1.0 mmol·L^-1 PhOH	—	去除0.22 mg·h^-1·cm^-2	—	·OH	—	[31]
CNT-HNO₃	—	Na₂SO₄	1.0 mmol·L^-1 PhOH	—	去除0.06 mg·h^-1·cm^-2	—	·OH	—	[31]
Pt/CNT	—	NaOH	1 mmol·L^-1 DCF	74(6 h)	48%(8 h)	Pt	直接氧化	—	[33]
Ru/CNT	—	NaHCO₃/ Na₂CO₃	1 mmol·L^-1 DCF	88(8 h)	27%(8 h)	Ru	直接氧化	—	[33]
Ni@Ni₃S₂/MWCNT	—	NaCl	0.5 mol·L^-1 ETA	约38(20 h)	—	Ni	直接氧化	—	[34]
Ti/SnO₂-Sb₂O₃/ CNT-PbO₂	1.79 V （vs SCE）	Na₂SO₄	100 mg·L^-1 MO	78.6(2 h)	58.2%(2 h)	—	·OH	225.40 kW·h·kg^-1	[35]
Ti/SnO₂-Sb₂O₃/ Bi-CNT-PbO₂	1.89 V （vs SCE）	Na₂SO₄	100 mg·L^-1 MO	84.8(2 h)	81.8%(2 h)	—	·OH	165.57 kW·h·kg^-1	[35]
Bi-Sb-SnO₂-CNT	—	Na₂SO₄	0.5 mmol·L^-1 PhOH	约40 (100 min)	22%(100 min)	—	·OH	—	[37]
Sb-SnO₂-CNT	—	Na₂SO₄	0.5 mmol·L^-1 PhOH	约30 (100 min)	13%(100 min)	—	·OH	—	[37]
Ti/MWCNTs/ SnO₂-Sb-Er	2.15 V （vs SCE）	Na₂SO₄	50 mg·L^-1 Cefotaxime	83.7 (60 min)	约80% (60 min)	—	·OH	—	[38]
Ti/MWCNTs/ SnO₂-Sb	约1.9 V (vs SCE)	Na₂SO₄	50 mg·L^-1 Cefotaxime	100 (60 min)	约65% (60 min)	—	·OH	—	[38]

Fig.3 (a) The edge sulfur containing and skeletal sulfur doped graphene by modulating the precursors and preparation[20]； (b) Sulfur doped reduced graphene oxide as an active layer to enhance the electrooxidation performance and stability of Ti/Ce-Mn/SnO2-Sb-La electrodes[48]

Fig.4 Schematic diagram of a bifunctional Co3O4 nanosphere-loaded nitrogen-doped reduced graphene oxide electrode for simultaneous electro-oxidation of methylene blue removal and CO2 reduction for selective methanol production[53]

Table 3 Comparison of typical graphene-based anode materials and their parameters related to degradation of pollutants

材料名称	析氧过电位	电解质	污染物	去除率/%	矿化度/%	活性位点	活性物种	能耗	文献
P-N-GN	—	NaCl	10 mg·L^-1 APAP	98.2±1.8 (60 min)	78.5(180 min)	含磷、氮元素的官能团	活性氯和 $· O 2 -$	0.017 kW·h·g^-1	[46]
A-SGO	—	NaCl	10×10^-6 BPA	97(120 min)	78.5(60 min)	—COOH，—OH和C—SO₃	活性氯和 $· O 2 -$	—	[20]
S-GO/Pt/TiO₂	—	NaCl	10 mg·L^-1 APAP	98(90 min)	44.1(4 h)	—SO _x 旁边的碳原子	直接氧化	0.069 kW·h·g^-1	[47]
S-GO/Pt/TiO₂	—	NaCl	10 mg·L^-1 APAP	98(90 min)	44.1(4 h)	—SO _x	活性氯和·OH	0.069 kW·h·g^-1	[47]
Ti/Ce-Mn/ SnO₂-Sb-La-S-rGO	2.12 V	Na₂SO₄	100 mg·L^-1 PhOH	89.5(120 min)	79.8(120 min)	—	·OH	—	[48]
GNP-PbO₂	2.05 V （vs SCE）	Na₂SO₄	100 mg·L^-1 ENO	92.69(120 min)	62.5(120 min)	—	·OH	—	[49]
Borophene-rGO	—	磷酸盐缓冲液和NaCl	1 µmol·L^-1 DTR	89±1	—	—O—C— B—N—	·OH和¹O₂	4.13 kW·h·m^-3	[50]
hBN-rGO	—	磷酸盐缓冲液和NaCl	1 µmol·L^-1 DTR	76±1	—	—O—C— B—N—	·OH和¹O₂	5.73 kW·h·m^-3	[50]
Cu-rGO-PC	—	Na₂SO₄	20 mg·L^-1 DCF	100(60 min)	—	rGO	直接氧化	—	[51]
Cu-rGO-PC	—	Na₂SO₄	20 mg·L^-1 DCF	100(60 min)	—	Cu	·OH和活性氯	—	[51]
Co₃O₄/N-rGO	—	KOH	100 mg·L^-1 MB	100(30 min)	—	Co	·OH	—	[53]

Table 3 Comparison of typical graphene-based anode materials and their parameters related to degradation of pollutants

材料名称	析氧过电位	电解质	污染物	去除率/%	矿化度/%	活性位点	活性物种	能耗	文献
P-N-GN	—	NaCl	10 mg·L^-1 APAP	98.2±1.8 (60 min)	78.5(180 min)	含磷、氮元素的官能团	活性氯和 $· O 2 -$	0.017 kW·h·g^-1	[46]
A-SGO	—	NaCl	10×10^-6 BPA	97(120 min)	78.5(60 min)	—COOH，—OH和C—SO₃	活性氯和 $· O 2 -$	—	[20]
S-GO/Pt/TiO₂	—	NaCl	10 mg·L^-1 APAP	98(90 min)	44.1(4 h)	—SO _x 旁边的碳原子	直接氧化	0.069 kW·h·g^-1	[47]
S-GO/Pt/TiO₂	—	NaCl	10 mg·L^-1 APAP	98(90 min)	44.1(4 h)	—SO _x	活性氯和·OH	0.069 kW·h·g^-1	[47]
Ti/Ce-Mn/ SnO₂-Sb-La-S-rGO	2.12 V	Na₂SO₄	100 mg·L^-1 PhOH	89.5(120 min)	79.8(120 min)	—	·OH	—	[48]
GNP-PbO₂	2.05 V （vs SCE）	Na₂SO₄	100 mg·L^-1 ENO	92.69(120 min)	62.5(120 min)	—	·OH	—	[49]
Borophene-rGO	—	磷酸盐缓冲液和NaCl	1 µmol·L^-1 DTR	89±1	—	—O—C— B—N—	·OH和¹O₂	4.13 kW·h·m^-3	[50]
hBN-rGO	—	磷酸盐缓冲液和NaCl	1 µmol·L^-1 DTR	76±1	—	—O—C— B—N—	·OH和¹O₂	5.73 kW·h·m^-3	[50]
Cu-rGO-PC	—	Na₂SO₄	20 mg·L^-1 DCF	100(60 min)	—	rGO	直接氧化	—	[51]
Cu-rGO-PC	—	Na₂SO₄	20 mg·L^-1 DCF	100(60 min)	—	Cu	·OH和活性氯	—	[51]
Co₃O₄/N-rGO	—	KOH	100 mg·L^-1 MB	100(30 min)	—	Co	·OH	—	[53]

Fig.5 Schematic diagram of the removal of tetracycline hydrochloride by waste wool-derived carbon-loaded iron-cobalt[70]

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