• 综述 •
葛明, 胡征, 贺全宝. 基于尖晶石型铁氧体的高级氧化技术在有机废水处理中的应用[J]. 化学进展, 2021, 33(9): 1648-1664.
Ming Ge, Zheng Hu, Quanbao He. Application of Spinel Ferrite-Based Advanced Oxidation Processes in Organic Wastewater Treatment[J]. Progress in Chemistry, 2021, 33(9): 1648-1664.
随着我国经济的快速发展和城市化进程的加快,自然水体中的有机污染问题愈加严重。基于自由基反应的高级氧化技术(AOPs)可以高效去除水环境中残留的难生物降解的有机污染物,在催化剂的作用下,高级氧化过程方能有效生成强氧化性的自由基来降解有机污染物。尖晶石型铁氧体(MFe2O4(M=Zn, Ni, Co, Cu, Mn))被广泛用作高级氧化过程中驱动自由基生成的催化剂,同时强磁性及高稳定性保证其容易在外加磁场的作用下实现回收和再利用。本文主要综述了基于尖晶石型铁氧体的非均相类芬顿技术、光催化技术及过硫酸盐高级氧化技术在有机废水处理方面的研究进展,着重介绍了不同铁氧体磁性纳米材料在上述3种高级氧化技术中催化降解水体中有机污染物的作用机制以及催化性能增强的途径;最后指出尖晶石型铁氧体在高级氧化技术应用中存在的一些问题,并对其后续研究方向进行展望。
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Catalyst | Synthetic method | Conditions for Fenton-like reaction | Catlayst dosage | H2O2 dosage | Pollutants and degradation efficiency | ref |
---|---|---|---|---|---|---|
ZnFe2O4 | hydrothermal route | 150 W Xe lamp | 0.5 g/L | 12.0 mM | AOII 100% (2 h) | |
ZnFe2O4/ graphene | solvothermal method | 500 W Xe lamp | 1.0 g/L | 30% H2O2 (1 mL) | RhB 100% (2 h); MO 96% (2 h) | |
porous C/ZnFe2O4 | CO2-mediated ethanol route | 300 W Xe lamp | 1.0 g/L | 30% H2O2 (2 mL) | RhB 100% (1 h); phenol 91% (2 h) | |
NiFe2O4 | co-precipitation method | - | 2.0 g/L | 120.0 mM | phenol 95% (5.5 h) | |
NiFe2O4/C | calcination method | 800 W Xe lamp | 0.1 g/L | 30% H2O2 (0.1 mL) | TC 97.25% (1 h) | |
NiFe2O4/CNTs | hydrothermal route | 150 W Xe lamp | 0.025 g/L | 1 μL/mL | SMX 90% (2 h) | |
CoFe2O4 | co-precipitation route | 125 W Hg lamp | 1.0 g/L | 30% H2O2 (3 mL) | MB 90% (1.25 h) | |
CoFe2O4-rGO | liquid assembly method | ultrasonic irradiation | 0.08 g/L | 3 mM | AO7 90.5% (2 h) | |
rGO/CoFe2O4 | solvothermal method | 5.0 mmol/l NH2OH | 0.1 g/L | 3 mM | MB 100% (0.25 h) | |
CoFe2O4@PPy | oxidization polymerization | 300 W Xe lamp | 0.2 g/L | 30% H2O2 (200 μL) | RhB 100% (2 h) | |
MnFe2O4 | sol-gel method | - | 0.6 g/L | 200 mM | NOR 90.6% (3 h) | |
MnFe2O4/ biochar | co-precipitation method | 300 W Xe lamp | 0.5 g/L | 200 mM | TC 95% (2 h) | |
MnFe2O4@SnS2 | hydrothermal method | 300 W Xe lamp | 0.2 g/L | 30% H2O2 (3 mL) | MB 92% (2 h) | |
CuFe2O4 | nanocasting strategy | - | 0.3 g/L | 40 mM | Imidacloprid 100% (5 h) | |
Cu/CuFe2O4 | solvothermal method | - | 0.1 g/L | 15 mM | MB 99% (4 min) | |
CuFe2O4@C | solvothermal route | 300 W Xe lamp | 0.1 g/L | 30% H2O2 (0.2 mL) | MB 97% (1.5 h) | |
CuFe2O4/rGO | hydrothermal method | 500 W of microwave power | 0.3 g/L | 30% H2O2 (600 μL) | RhB 95.5% (1 min) | |
CuFe2O4@PDA | self-polymerization | - | 0.2 g/L | 0.5 M | MB 97% (0.5 h) | |
CuFe2O4@ g-C3N4 | self-assembly method | 500 W Xe lamp | 0.1 g/L | 0.01 M | OII 98% (3.5 h) |
Photocatalyst | Synthetic method | Light source | Catalyst dosage | Pollutants and degradation efficiency | ref |
---|---|---|---|---|---|
hollow cube ZnFe2O4 | template method | 300 W Xe lamp | 0.5 g/L | TCHC 85% (20 min) | |
ZnFe2O4(111) | hydrothermal route | 500 W Xe lamp | 1.0 g/L | RhB 90% (1 h) | |
ZnFe2O4-TiO2 | a reflux route | 8 W visible-light lamp | 1.0 g/L | BPA 98.7% (30 min) | |
ZnFe2O4-ZnO | co-precipitation method | 500 W halogen lamp | 0.5 g/L | MB 98% (6 h) | |
Ag/ZnO/ZnFe2O4 | facile calcination route | 250 W Xe lamp | 0.5 g/L | MB 93% (100 min) | |
BiOBr-ZnFe2O4 | precipitation method | 300 W Xe lamp | 1.0 g/L | RhB 90% (25 min) | |
biochar @ZnFe2O4/BiOBr | solvothermal method | 300 W Xe lamp | 0.5 g/L | CIP 65% (1 h) | |
p-BiOI/n-ZnFe2O4 | solvothermal method | 400 W halogen lamp | 1.0 g/L | AO7 96% (3 h) | |
Ag3PO4/ZnFe2O4 | precipitation route | 10 W LED light | 1.0 g/L | MB 100% (1 h) | |
C@ZnFe2O4/Ag3PO4 | precipitation method | 300 W Xe lamp | 1.0 g/L | 2,4-DCP 95% (2.5 h) | |
ZnFe2O4/AgBr/Ag | precipitation and photoreduction | 300 W Xe lamp | 0.4 g/L | MO 92% (30 min) | |
g-C3N4-ZnFe2O4 | solvothermal method | 500 W Xe lamp | 0.25 g/L | MO 98% (3 h) | |
Ag/NiFe2O4 | combustion method | 300 W Xe lamp | 0.25 g/L | MB 70% (2 h) | |
Ag/CuFe2O4 | impregnation strategy | 500 W Xe lamp | 0.1 g/L | 4-CP 81% (2 h) | |
rGO-CoFe2O4 | hydrothermal route | Solar light | 0.4 g/L | 4-CP 100% (2 h) | |
Pd-NiFe2O4/rGO | hydrothermal route | 300 W Xe lamp | 1.0 g/L | RhB 99% (2 h) | |
BiOBr/NiFe2O4 | hydrothermal route | 500 W Xe lamp | 1.0 g/L | RhB 100% (30 min) | |
Ag3PO4@CoFe2O4 | precipitation approach | 500 W halogen lamp | 0.4 g/L | MB 100% (40 min) | |
Ag3PO4/CuFe2O4 | deposition method | 300 W Xe lamp | 0.2 g/L | RhB 100% (35 min) | |
Ag3PO4/GO/NiFe2O4 | deposition route | 300 W Xe lamp | 0.2 g/L | RhB 100% (30 min) | |
Ag3PO4/CoFe2O4/GO | precipitation process | 300 W Xe lamp | 0.3 g/L | MO 91% (15 min) | |
biochar@CoFe2O4/Ag3PO4 | in-situ precipitation method | 300 W Xe lamp | 0.5 g/L | BPA 91% (60 min) | |
AgBr/NiFe2O4 | a precipitation method | 10 W LED lamp | 1.0 g/L | RhB 100% (60 min) | |
AgBr/CoFe2O4 | a precipitation method | 10 W LED lamp | 1.0 g/L | MO 95% (60 min) | |
AgBr-Cu-CuFe2O4 | a precipitation method | 10 W LED lamp | 1.0 g/L | RhB 95.2% (60 min) | 16] |
catalyst | Synthetic method | PMS or PDS dosage | Catalyst dosage | Pollutants and degradation efficiency | ref |
---|---|---|---|---|---|
CoFe2O4 | hydrothermal method | 0.8 mM PMS | 0.4 g/L | ATZ 99% (30 min) | |
CoFe2O4 | sol-gel method | 0.5 mM PMS | 0.25 g/L | TPhP 99.5% (6 min) | |
CoFe2O4/Al2O3 | sol-gel method | 0.5 mM PMS | 1.0 mM | SCP 97.8% (15 min) | |
CoFe2O4/TiO2 | impregnation-calcination method | 4.0 g/L PMS | 0.01 g/L | RhB 100% (30 min) Phenol 97.2% (60 min) | |
CoFe2O4-rGO | solvothermal route | 10 mg/150 mL | 0.3 g/150 mL | Phenol 100% (30 min) | |
CoFe2O4-GO | hydrothermal method | 0.5 mM PMS | 0.3 g/L | NOR 100% (20 min) | |
CoFe2O4-EG | co-precipitation method | 0.4 mM PMS | 0.5 g/L | SMX ~92% (20 min) | |
CoFe2O4-x | hydrogen calcination method | 3 mM PDS | 0.1 g/L | BPA 98% (60 min) | |
CuFe2O4 | sol-gel combustion method | 0.2 mM PMS | 0.1 g/L | TBBPA 99% (30 min) | |
CuFe2O4 | a citrate combustion method | 20 μM PMS | 0.1 g/L | IPM ~80% (10 min) | |
CuFe2O4 | a citrate combustion method | 0.5 g/L PMS | 0.4 g/L | BPA 100% (60 min) | |
CuFe2O4 | co-precipitation-calcination method | 0.5 mM PMS | 0.2 g/L | NOR 90% (120 min) | |
CuFe2O4 | a coprecipitation method | 0.2 mM PMS | 0.1 g/L | PCB28 89% (8 h) | |
CuFe2O4-OMS-2 | a solvent-free process | 0.65 mM PMS | 0.2 g/L | AO7 95.8% (20 min) | |
CuFe2O4-Fe2O3 | a co-precipitation method | 0.36 g/L PMS | 0.2 g/L | BPA 100% (10 min) | |
CuFe2O4/MWCNTs | a sol-gel combustion method | 0.6 mM PMS | 0.2 g/L | TMP 90% (24 min) | |
CuFe2O4-NG | a hydrothermal route | 1.0 g/L PMS | 0.05 g/L | OⅡ 100% (70 min) | |
CuFe2O4/ kaolinite | a facile citrate combustion method | 0.5 mM PMS | 0.5 g/L | BPA 100% (60 min) | |
CuFe2O4 | a sol-gel combustion method | 8 mM PDS | 30 g/L | PNP 89% (60 min) | |
CuFe2O4/MWCNTs | a sol-gel combustion route | 1.0 g/L PDS | 0.1 g/L | DEP 100% (30 min) | |
CuFe2O4-Cu | a solvothermal method | 1.5 g/L PDS | 0.3 g/L | TC 80% (120 min) | |
MnFe2O4 | the nanocasting strategy | 2 mM PMS | 0.2 g/L | OⅡ 100% (30 min) | |
MnFe2O4 | - | 0.1 mM PMS | 0.2 g/L | BPA 90% (30 min) | |
MnFe2O4 | - | 0.75 mM PMS | 0.25 g/L | TCS 100% (20 min) | |
MnFe2O4-rGO | a precipitation method | 0.5 g/L PMS | 0.05 g/L | OⅡ 90% (120 min) | |
MnFe2O4-MX | a solvothermal method | 0.5 g/L PMS | 0.05 g/L | OⅡ 100% (6 min) | |
MnFe2O4-MnO2 | a hydrothermal method | 0.4 g/L PMS | 0.2 g/L | RhB 100% (40 min) | |
MnFe2O4 | thermal decomposition | 0.5 g/L PDS | 3 g/L | Phenol 90% (360 min) | |
MnFe2O4/AC | a solvothermal method | 0.5 g/L PDS | 0.2 g/L | OG 100% (30 min) | |
CuO/MnFe2O4 | an impregnation method | 1.0 g/L PDS | 1.0 g/L | LVF 87% (120 min) |
Catalyst | Application in AOPs | Mechanism for organic pollutants degradation | Methods for the enhancement of activity |
---|---|---|---|
ZnFe2O4 | (1)Fenton [ | ≡Fe3+ + e- → ≡Fe2+; ≡Fe2+ + H2O2→·OH + ≡Fe3+ + OH- ·OH + pollutants → degradation products | Carbon modification[ |
(2)Photocatalysis [ | ZnFe2O4 + hν → e- + h+O2 + e- → /h+ + pollutants → degradation products | Carbon modification [ Construction of heterojunction [ | |
NiFe2O4 | (1)Fenton [ | ≡Fe3+ + e- → ≡Fe2+; ≡Ni2+ + ≡Fe3+ → ≡Fe2+ + ≡Ni3+ ≡Fe2+ + H2O2→·OH + ≡Fe3+ + OH- ·OH + pollutants → degradation products | Carbon modification[ |
(2)Photocatalysis [ | NiFe2O4 + hν → e- + h+O2 + e- → /h+ + pollutants → degradation products | Metal deposition [ Construction of heterojunction [ | |
CoFe2O4 | (1)Fenton [ | ≡Co2+ + H2O2→·OH + ≡Co3+ + OH- ≡Fe2+ + H2O2→·OH + ≡Fe3+ + OH- ·OH + pollutants → degradation products | Carbon modification[ |
(2)Photocatalysis [ | CoFe2O4 + hν → e- + h+O2 + e- → /h+ + pollutants → degradation products | Carbon modification[ Construction of heterojunction [ | |
(3)Persulfate oxidation [ | ≡Co2+-OH-+ →≡CoO++ +H2O ≡Fe3+ + → ≡Fe2+ + + H+ ≡Fe2+ + → ≡Fe3+ + + OH- +H2O → + ·OH + H+ /·OH + pollutants → degradation products | Metallic oxide modification [ Carbon modification [ | |
CuFe2O4 | (1)Fenton [ | ≡Cu+ + H2O2→·OH + ≡Cu2+ + OH- ≡Fe2+ + H2O2→·OH + ≡Fe3+ + OH- ·OH + pollutants → degradation products | Carbon modification [ Metal modification [ |
(2)Photocatalysis [ | CuFe2O4 + hν → e- + h+O2 + e- → /h+ + pollutants → degradation products | Construction of heterojunction [ Metal deposition [ | |
(3)Persulfate oxidation [ | ≡Cu+ + → ≡Cu2+ + + OH- ≡Fe2+ + → ≡Fe3+ + + OH- ≡Fe2+ + → ≡Fe3+ + + ·OH ≡Cu+ + → ≡Cu2+ + + ·OH S2 + ≡Cu+→≡Cu2+ + + S2 + ≡ →≡Fe3++ + /·OH + pollutants → degradation products | Metal modification [ Carbon modification [ Metallic oxide modification [ | |
MnFe2O4 | (1)Fenton [ | ≡ + H2O2→·OH + ≡ + OH-≡Fe2+ + H2O2→·OH + ≡Fe3+ + OH- ·OH + pollutants → degradation products | Carbon modification [ |
(2)Persulfate oxidation [ | ≡ + → ≡ + + OH- ≡Fe2+ + → ≡Fe3+ + + OH- S2 + ≡ → ≡Mn3++ + +H2O → + ·OH + H+ /·OH + pollutants → degradation products | Carbon modification [ Metallic oxide modification [ |
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