层状双金属氢氧化物活化过硫酸盐降解有机污染物研究进展

武利园; 王鑫; 郭朋朋; 陈开宇; 李海燕; 刘启芸

doi:10.13801/j.cnki.fhclxb.20210824.001

层状双金属氢氧化物活化过硫酸盐降解有机污染物研究进展

doi: 10.13801/j.cnki.fhclxb.20210824.001

武利园^{1, 2, 3, ,},
王鑫¹,
郭朋朋¹,
陈开宇¹,
李海燕^{1, 3, ,},
刘启芸¹

1.
北京建筑大学北京节能减排与城乡可持续发展省部共建协同创新中心，北京 100044
2.
北京建筑大学城市环境修复研究中心，北京 100044
3.
北京市可持续城市排水系统构建与风险控制工程技术研究中心，北京 100044

基金项目: 国家重点研发计划项目 (2020YFC1808803)；北京节能减排与城乡可持续发展省部共建协同创新中心资助项目；青年北京学者计划 (024)；北京建筑大学市属高校基本科研业务费专项 (X20139; X20086; X20095)

详细信息

通讯作者:
武利园，博士，副教授，硕士生导师，研究方向为水质净化功能材料研发及应用、吸附/高级氧化水处理技术　E-mail：wuliyuan@bucea.edu.cn

李海燕，博士，教授，博士生导师，研究方向为城市径流污染与控制、环境工程材料研发与应用　E-mail: lihaiyan@bucea.edu.cn

中图分类号: X52
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出版历程
- 收稿日期: 2021-07-01
- 修回日期: 2021-08-04
- 录用日期: 2021-08-07
- 网络出版日期: 2021-08-25
- 刊出日期: 2022-03-23

Layered double hydroxides mediated persulfate activation for organic pollutants degradation: A review

WU Liyuan^{1, 2, 3
, ,},
WANG Xin¹,
GUO Pengpeng¹,
CHEN Kaiyu¹,
LI Haiyan^{1, 3
, ,},
LIU Qiyun¹

1.
Beijing Energy Conservation & Sustainable Urban and Rural Development Provincial and Ministry Co-construction Collaboration Innovation Center, Beijing University of Civil Engineering and Architecture, Beijing 100044, China
2.
Center for Urban Environmental Remediation, Beijing University of Civil Engineering and Architecture, Beijing 100044, China
3.
Beijing Engineering Research Center of Sustainable Urban Sewage System Construction and Risk Control, Beijing 100044, China

摘要

摘要: 近代工业的快速发展造成大量难降解的新型有机污染物进入水体，亟需经济、高效的难降解有机污染物污染控制和削减技术。近年来，基于硫酸根自由基(SO₄^•–)的高级氧化技术(SR-AOPs)具有强氧化性、宽pH耐受性以及方便操作性等优势而备受关注。不同种类的金属氧/硫化物、碳基材料、金属-非金属复合材料以及有机金属材料等被用来活化过硫酸盐产生活性氧，从而实现对有机污染物的氧化降解和进一步矿化。其中，层状双金属氢氧化物(Layered double hydroxides, LDHs)因其独特的层状结构优势、阴离子可交换性和客体分子可调节性，在活化过硫酸盐方面表现出优良的反应活性和催化优势。本论文从催化剂类型、催化性能与机制以及降解体系影响因素等方面，综述了LDHs及其复合材料作为非均相催化剂活化过硫酸盐的研究现状，并对催化体系持续改进以及未来发展提出相关展望。
- 层状双金属氢氧化物(LDHs) /
- 非均相活化 /
- 过硫酸盐 /
- 硫酸根自由基(SO₄^•–) /
- 有机污染物
Abstract: The rapid development of modern industry has caused a large number of refractory organic pollutants to enter the water body, there is an urgent need for economic and efficient pollution control and reduction technologies for refractory organic pollutants. In recent years, advanced oxidation technologies (SR-AOPs) based on sulfate radicals (SO₄^•–) have attracted much attention because of their strong oxidizing properties, wide pH tolerance, and ease of operation. Different types of metal oxygen/sulfide, carbon-based materials, metal-non-metal composite materials and organic metal materials are used to activate persulfate to generate active oxygen, thereby achieving oxidative degradation and further mineralization of organic pollutants. Among them, layered double hydroxides (LDHs) show excellent reactivity and catalytic advantages in activating persulfate due to their unique layered structure advantages, anion exchangeability and guest molecule adjustability. This article reviews the current research status of LDHs and their composites as heterogeneous catalysts to activate persulfate from the aspects of catalyst type, catalytic performance and mechanism, and degradation system influencing factors, and proposes relevant prospects for the continuous improvement of the catalytic system and future development.
- layered double hydroxides(LDHs) /
- heterogeneous activation /
- persulfate /
- sulfate radicals (SO₄^•–) /
- organic pollutants

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图 1 层状双金属氢氧化物 (LDHs) 结构示意图

Figure 1. Schematic diagram of layered double hydroxides (LDHs) structure

M=Fe, Ni, Co, et al; Aⁿ^–=CO₃^2–, SO₄^2–, Cl^–, et al

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图 2 LDHs/PMS或LDHs/PS体系降解污染物机制

Figure 2. Mechanism of pollutants degradation by LDHs/PMS or LDHs/PS system

N=Fe, Ni, Mn, Co, et al

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图 3 CuFe-LDH/PS/Vis复合体系中可见光作用机制

Figure 3. Mechanism of activation by visible light in CuFe-LDH/PS/Vis composite system

h⁺—Electron hole

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图 4 活性炭@CoFe-LDH/PS (AC@CoFe-LDH/PS) 体系降解污染物机制

Figure 4. Mechanism of pollutants degradation by actived carbon@CoFe-LDH/PS (AC@CoFe-LDH/PS) system

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表 1 不同单一型LDHs催化剂非均相活化过硫酸盐体系去除有机污染物效能对比

Table 1. Comparison of the removal efficiency of different single-type LDHs catalysts in heterogeneously activated persulfate systems

Catalyst	Contaminants	Reaction condition	Removal efficiency	TOC removal	Dominant ROS	Ion leaching	Ref.
FeCo-LDH	RhB	c(RhB)=20 mg/L, c(Catalyst)=0.2 g/L, c(PMS)= 0.15 g/L, pH=3.42, T=25℃	10 min, 100%	—	SO₄^•−	—	[36]
Fe₂Co-LDH	BPA	c(BPA)=30 mg/L, c(Catalyst)=0.3 g/L, c(PS)=4 mmol/L, pH=7, T=25℃	60 min, 99.38%	58.99%	SO₄^•−, •OH	—	[37]
MgMnCo-LDH	SMX	c(SMX)=0.05 mmol/L, c(Catalyst)=0.1 g/L, c(PMS)=0.40 mmol/L, pH=5.0	10 min, 99%	67.8%	SO₄^•−, ¹O₂	—	[38]
CuFe-LDH	MV	c(Catalyst)=0.2 g/L, c(MV)=20 mg/L c(PS)=0.2 g/L, Visible light>420 nm, T=25℃	18 min, 100%	—	SO₄^•−, •OH	c(Fe)≤0.1 mg/L	[46]
CoFeLa-LDH	TC	c(TC)=30 mg/L, c(Catalyst)= 0.05 g/L, c(PMS)=1.0 mmol/L, pH=5.4, T=25℃	10 min, 81.6%-90.1%	—	SO₄^•−, •OH, ¹O₂	—	[47]
CoMn-LDH	AOG	c(AOG)=0.05 g/L, c(Catalyst)=0.025 g/L, c(PMS)=0.1 g/L, pH=6.87, T=25℃	120 s, 99.8%	50.5% (30 min)	SO₄^•−	c(Co)=0.53 mg/L, c(Mn)=0.16 mg/L (After 4 cycles)	[48]
FeMn-LDH	ODA	c(Catalyst)=0.4 g/L, c(ODA)=0.01 g/L, c(PMS)=0.4 g/L, pH=1.8, T=25℃	25 min, 85%	—	SO₄^•−, •OH	c(Mn)=772 µg/L, c(Fe)=13 µg/L	[49]
CoFeNi-LDH	CR/RhB	c(Catalyst)=0.2 g/L, c(CR)=20 mg/L or c(RhB)=20 mg/L, c(PMS)=0.15 m g/L, pH=7, T=25℃	6 min(CR), 100%; 10 min(RhB), 100%	—	SO₄^•−	c(Co)=0.68 mg/L	[50]
CuCoFe-LDH	NB	c(Catalyst)=0.1 g/L, c(NB)=2.0 mg/L, c(PMS)=0.5 mmol/L, pH=6.5, T=25℃	6 min, >99%	—	•OH	c(Co)=34 μg/L, c(Cu)=92 μg/L	[51]
MgCuFe-LDH	Acetaminophen	c(Catalyst)=0.3 g/L, c(Acetaminophen)=5 g/L, c(PMS)=0.5 mmol/L, pH=6.0, T=25℃	20 min, 93%	64.5% (2 h)	SO₄^•−, •OH	c(Cu)=0.77 mg/L, c(Mg)=4.98 mg/L (30 min)	[52]
Notes: RhB—Rhodamine B; BPA—Bisphenol A; MV—Methyl violet; TC—Tetracycline; AOG—Acid orange G; ODA—Octadecylamine; CR—Congo red; NB—Nitrobenzene; PMS—Peroxymonosulfate; PS—Persulfate; SMX—Sulfamethoxazole; TOC—Total organic carbon;ROS—Reactive oxygen species.

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表 2 不同单一型层状复合氧化物 (LDOs) 催化剂非均相活化过硫酸盐体系去除有机污染物效能对比

Table 2. Comparison of the removal efficiency of different single-type layered double oxides (LDOs) catalysts in heterogeneously activated persulfate

Catalyst	Contaminants	Reaction condition	Removal efficiency	TOC removal	Dominant ROS	Ion leaching	Ref.
CuMgAl-LDO	SMD	c(SMD)=10 mg/L, c(Catalyst)=0.3 g/L, c(PS)=0.7 mmol/L, pH=6.4, T=25℃	120 min, 99.49%	—	SO₄^•−	c(Cu)=0.89 mg/L (After 5 cycles)	[39]
MgMn-LDO	TC	c(TC)=44.4 mg/L, c(Catalyst)=0.1 g/L, c(PMS)=0.50 mmol/L, pH=5.0	20 min, 97.1%	47%	¹O₂	—	[61]
CuCo-LDO	LOM	c(LOM)=10 mg/L, c(Catalyst)=0.04 g/L, c(PMS)=0.15 g/L, pH=6.67, T=25℃	30 min, 96.19%	—	SO4^•−, ¹O₂, •OH	—	[62]
Co₂FeAl-LDO	CBZ	c(CBZ)=10 mg/L, c(Catalyst)=60 mg/L, c(PMS)=0.2 mmol/L, pH=6.1	30 min, >99%	30%	SO₄^•−	c(Co)=0.4 mg/L; c(Fe)≈0 (After 5 cycles)	[63]
CoMgFe-LDO	CBZ	c(CBZ)=5 mg/L, c(Catalyst)=20 mg/L, c(PMS)=0.2 mmol/L, pH=5.8, T=30℃	20 min, 100%	21.3%	SO₄^•−	—	[64]
CoCuAl-LDO	AO₇	c(AO₇)=20 mg/L, c(Catalyst)=0.1 g/L, c(PMS)=0.1 g/L, pH=6.7, T=25℃	30 min, >99%	—	SO₄^•−	c(Co)<0.03 mg/L; c(Cu)<0.3 mg/L	[65]
CuMgFe-LDO	Phenol	c(Phenol)=0.1 mmol/L, c(Catalyst)=0.5 g/L, c(PS)=0.5 mmol/L, pH=6.4, T=25℃	30 min, 59.3%	—	SO₄^•−, •OH	c(Cu)=0.19 mg/L (After 3 cycles)	[66]
CoMgAl-LDO	ATZ	c(ATZ)=10 mg/L, c(Catalyst)=75 mg/L, c(PMS)=0.4 mmol/L, pH=6.3, T=30℃	15 min, 98.7%	26.5%	SO₄^•−	c(Cu)=0.35 mg/L (After 4 cycles)	[67]
Notes: SMD—Sulfa p-methoxypyrimidine; LOM—Lomefloxacin; CBZ—Carbamazepine; AO₇—Acid orange 7; ATZ—Atrazine; LDO—Layered double oxides.

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表 3 不同碳复合型LDHs催化剂非均相活化过硫酸盐体系去除有机污染物效能对比

Table 3. Comparison of the removal efficiency of different carbon composite type LDHs catalysts in heterogeneously activated persulfate

Catalyst	Contaminants	Reaction condition	Removal efficiency	TOC removal	Dominant ROS	Ion leaching	Ref.
AC@CoFe-LDH	LMF	c(Catalyst)=0.2 g/L, c(Catalyst)=0.2 g/L, c(PS)=1.0 g/L, pH=4.5, T=25℃	60 min, 93.2%	—	SO₄^•−	—	[40]
LDH-GO	GAT	c(GAT)=38 mg/L, c(Catalyst)=40 mg/L, c(PMS)=400 mg/L, pH=7.0, T=25℃	45 min, 100%	5 h, 55.5%	SO₄^•−	—	[76]
DOM-FeAl-LDH	BPA	c(BPA)=20 mg/L, c(Catalyst)=200 mg/L, c(PMS)=200 mg/L, pH=5.58, T=25℃	6 min, 93%	—	•OH	c(Fe)=50 μmol/L	[77]
LDH@PVDF	SMX	c(SMX)=10 mg/L, c(Catalyst)=17.5 mg/L, c(PMS)= 25 mg/L, T=25℃	60 min, 92.8%	—	—	c(Co)=0.044 mg/L; c(Cu)=0.026 mg/L	[78]
CuCo-LDH@PAN	SMX	c(SMX)=10 mg/L, c(Catalyst)=60 m/L, c(PMS)=0.24 mmol/L, pH=5.77, T=25℃	5 min, 83.9%	59.40%	SO₄^•−, •OH	c(Co)=0.014 mg/L; c(Cu)=0.010 mg/L	[79]
CMK-LDH	SMX	c(SMX)=25 mg/L, c(Catalyst)=0.15 g/L, c(PS)=0.5 g/L, pH=5, T=25℃	150 min, 84.9%	—	•OH	—	[80]
Co₇Fe₃/CoFe₂O₄@C	RhB; p-Nitrophenol	c(Pollutant)=50 mg/L, c(Catalyst)=0.1 g/L, c(PMS)=0.5 g/L, pH=7, T=25℃,	RhB: 10 min, 100%; p-Nitropheno: 30 min, 99%	p-Nitropheno: 180 min, 72%	SO₄^•−, •OH	c(Fe)=0.068 mg/L; c(Co)=0.0592 mg/L	[81]
CoAl-LDH/g-C₃N₄	SDZ	c(SDZ)=10 μmol/L, c(Catalyst)=0.1 g/L, c(PMS)=0.5 mmol/L, pH=6.0	15 min， 87.1%	—	h⁺	c(Co)≈0	[82]
Notes: AC—Activate carbon; LMF—Lomefloxacin; GO—Graphene oxide; DOM—Dissolved organic matter; BPA—Bisphenol A; PVDF—Polyvinylidene fluoride; PAN—Polyacrylonitrile; CMK—Mesoporous carbon; GAT—Gatifloxacin; SDZ—Sulfadiazine.

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