碳基材料电氧化去除水体污染物的研究进展

doi:10.11949/0438-1157.20230135

化工学报 ›› 2023, Vol. 74 ›› Issue (5): 1862-1874.DOI: 10.11949/0438-1157.20230135

碳基材料电氧化去除水体污染物的研究进展

郭旭¹^,²(), 张永政³, 夏厚兵¹^,², 杨娜⁴, 朱真珍¹^,², 齐晶瑶¹^,²()

^1.哈尔滨工业大学生物质能源开发利用国家地方联合工程研究中心，黑龙江哈尔滨 150006
^2.哈尔滨工业大学环境学院，黑龙江哈尔滨 150006
^3.哈尔滨工业大学化工与化学学院，黑龙江哈尔滨 150006
^4.陕西科技大学轻工科学与工程学院，陕西西安 710021

收稿日期:2023-02-21 修回日期:2023-04-20 出版日期:2023-05-05 发布日期:2023-06-29
通讯作者: 齐晶瑶
作者简介:郭旭（1996—），男，博士研究生，guox96@163.com
基金资助:
生物质能源开发利用国家地方联合工程研究中心面上项目(2021B001);中央高校基本科研业务费专项资金项目(HIT_NSRIF202216)

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

Xu GUO¹^,²(), Yongzheng ZHANG³, Houbing XIA¹^,², Na YANG⁴, Zhenzhen ZHU¹^,², Jingyao QI¹^,²()

^1.Biomass Energy Development and Utilization National and Local Joint Engineering Research Center, Harbin Institute of Technology, Harbin 150006, Heilongjiang, China
^2.School of Environment, Harbin Institute of Technology, Harbin 150006, Heilongjiang, China
^3.School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150006, Heilongjiang, China
^4.College of Bioresources Chemical and Materials Engineering, Shaanxi University of Science & Technology, Xi’an 710021, Shaanxi, China

Received:2023-02-21 Revised:2023-04-20 Online:2023-05-05 Published:2023-06-29
Contact: Jingyao QI

摘要/Abstract

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

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

中图分类号:

X 703.1

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.

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.

图/表 8

表1 间接氧化（·OH介导）及析氧反应对比

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）

表1 间接氧化（·OH介导）及析氧反应对比

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）

图1 （a）酸预处理的碳纳米管海绵电氧化去除全氟辛酸[26]；（b）碳纳米管/聚氨酯海绵电化学过滤器运行示意图[27]

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]

图2 具有纳米异质结结构的Ni@Ni3S2/CNT电极用于低能耗的析氢(阴极)与电催化去除盐水中的乙醇胺污染物(阳极)的示意图[34]

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]

表2 典型碳纳米管基阳极材料及其降解污染物相关参数对比

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]

图3 （a）通过调控前体和制备方式获得含有边缘硫和骨架硫掺杂石墨烯[20]；（b）掺硫还原氧化石墨烯作为活性层提升Ti/Ce-Mn/SnO2-Sb-La电极电氧化性能和稳定性[48]

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]

图4 双功能负载Co3O4纳米球的氮掺杂还原氧化石墨烯电极电氧化去除亚甲基蓝同时还原CO2选择性生产甲醇的示意图[53]

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]

表3 典型石墨烯基阳极材料及其降解污染物相关参数对比

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]

表3 典型石墨烯基阳极材料及其降解污染物相关参数对比

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]

图5 废弃羊毛衍生碳负载磷化铁钴去除盐酸四环素示意图[70]

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

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碳基材料电氧化去除水体污染物的研究进展

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

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