MoS2 catalyzed peroxymonosulfate activation for organic pollutants degradation: A review
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摘要: 随着城镇化进程加快,大量含难降解有机污染物的工业废水和生活污水因不合理处置而进入水体,对水环境质量造成严重威胁。过渡金属离子催化活化单过硫酸盐(PMS)产生活性氧去除水中难降解有机物的催化体系的研究已有大量文献报道,但存在金属离子二次污染和催化剂难以回收等问题。MoS2作为优异的二维半导体材料,在储能和催化领域颇具优势并实现产业化生产。在水处理领域,研究发现MoS2作为非均相金属催化剂能够有效活化PMS去除水中难降解有机物。本文主要综述了MoS2作为催化剂、金属离子助催化剂或复合型共催化剂活化PMS体系降解水中有机污染物的研究进展,归纳并比较上述催化体系对污染物的降解效能,对催化反应机制进行探讨分析,并针对目前存在的问题提出相关研究展望。Abstract: With the acceleration of urbanization, the massive discharge of industrial wastewater and domestic sewage containing refractory organic pollutants has entered into waterbodies due to unreasonable disposal, which poses a serious threat to the water environment quality. Transition-metal ions mediated peroxymonosulfate (PMS) activation has been extensively studied as their ability to produce various active oxygen species for contaminants removal in water. However, the accompanied problems of secondary pollution and difficulty in catalyst recovery has limited their practical application. MoS2, an excellent two-dimensional semiconductor material of industrial production, has been widely used in energy conversion and catalysis area. In water treatment, MoS2 materials have been reported as an efficient heterogeneous catalyst for PMS activation to degrade refractory organic pollutants. This review summarized recent studies concerning MoS2-catalyzed PMS activation for organic pollutants removal in aqueous solution. The catalysis efficiencies of PMS activation mediated by MoS2, MoS2/metal ions and MoS2 supported materials were comparatively described, the relevant mechanisms were discussed and the development prospect of the current research were expected briefly.
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Key words:
- MoS2 /
- peroxymonosulfate /
- active oxygen /
- degradation /
- organic pollutants
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表 1 不同MoS2/Fe(Ⅱ)/PMS催化体系对有机污染物降解性能及机制比较
Table 1. Comparison of performance and mechanism of different MoS2/Fe(Ⅱ)/PMS systems
Number ① ② ③ ④ Reference [47] [48] [49] [50] Reaction condition [ACT]=20 mg/L, [RhB]=20 mg/L, [TCP]=19.7 mg/L, [SMX]=6.3 mg/L, [Fe(Ⅱ)]=1 mg/L, [MoS2]=0.1 g/L, [PMS]=1 mmol/L pH=3 [Fe(Ⅱ)]=3 mg/L, [MoS2]=0.3 g/L, [PMS]=1 mmol/L pH=3 [Fe(Ⅱ)]=2.26 mg/L, [MoS2]=1 g/L, [PMS]=0.5 mmol/L pH=3 [Fe(Ⅱ)]=3.92 mg/L, [MoS2]=0.3 mg/L, [PMS]=0.075 mmol/L pH=3 Pollutant ACT RhB TCP SMX Main active oxygen 1O2 SO4−·, ·OH SO4−·, ·OH SO4−·, ·OH Efficiency 60 min, 100% 60 min, 94.7% 30 min, >95% 6 min, 88.5% TOC 29.8% 59.8% >25% 33.9% Ion leaching Mo: 60 min, 2.88 mg/L — Mo: 30 min, >8 mg/L — Recycle 6 times, >90% 8 times, >95% 5 times, 93% 6 times, ~90% Mechanism (1) Fe(Ⅱ)+HSO5− → Fe(Ⅲ)+SO4−·+OH−
(2) Mo(Ⅳ)+ 2Fe(Ⅲ) → 2Fe(Ⅱ)+Mo(Ⅵ)
(3) Mo(Ⅵ) → … → MoO3
(4) MoO3+H+→HMoO3+ +2HSO5− → MoO(OH)(O2)2−+2SO3+H2O
(5) MoO(OH)(O2)2−+ H2O→MoO42−+1O2+H+
(6) 1O2+ACT→H2O+CO2+others(1) Fe(Ⅱ)+HSO5− → Fe(Ⅲ)+SO4−·+OH−
(2) Fe(Ⅱ)+HSO5− → Fe(Ⅲ)+SO4−+·OH
(3) Mo(Ⅳ)+2Fe(Ⅲ) → 2Fe(Ⅱ)+Mo(Ⅵ)
(4) Fe(Ⅲ)+HSO5− → Fe(Ⅱ)+SO5−·+H+
(5) Mo(Ⅵ)+2HSO5−→Mo(Ⅳ)+2SO5−·+ H+
(6) ·OH/SO4−·+RhB/TCP/SMX → H2O+CO2+othersNotes: TOC—Total organic carbon; ACT—Acetaminophen; RhB—Rhodamine B; TCP—2,4,6-Trichlorophenol; SMX—Sulfamethoxazole. 表 2 非均相MoS2/PMS降解有机污染物催化体系汇总
Table 2. Summary of heterogeneous MoS2/PMS system for degradation of organic pollutants
Category System Pollutant Reaction condition Efficiency Ref. Single MoS2 1T-MoS2/PMS BPA [BPA]=2 mg/L,
[MoS2]=15 mg/L,
[PMS]=50 mg/L
pH=4, T=25℃10 min, 91% [36] 2H-MoS2/PMS CBZ [CBZ]=5 mg/L,
[MoS2]=0.2 g/L,
[PMS]=0.2 mmol/L
pH=3~9, T=30℃40 min, > 95% [42] Co-catalytic
MoS2/PMSMoS2/Fe(Ⅱ)/PMS ACT [ACT]=20 mg/L,
[Fe(Ⅱ)]=3 mg/L,
[MoS2]=0.3 g/L,
[PMS]=1 mmol/L
pH=3, T=25℃60 min, 100% [47] MoS2/Fe(Ⅱ)/PMS RhB [RhB]=20 mg/L,
[Fe(Ⅱ)]=1 mg/L,
[MoS2]=0.1 g/L,
[PMS]=1 mmol/L
pH=3, T=25℃60 min, 100% [48] MoS2/Fe(Ⅱ)/PMS TCP [TCP]=19.7 mg/L,
[Fe(Ⅱ)]=2.26 mg/L,
[MoS2]=1 g/L,
[PMS]=0.5 mmol/L
pH=3, T=25℃60 min, 100% [49] MoS2/Fe(Ⅱ)/PMS SMX [SMX]=6.3 mg/L,
[Fe(Ⅱ)]=3.92 mg/L,
[MoS2]=0.3 g/L,
[PMS]=0.075 mmol/L
pH=3, T=25℃60 min,100% [50] MoS2/Fe(Ⅲ)/PMS RhB [RhB]=20 mg/L,
[Fe(Ⅲ)]=5.6 mg/L,
[MoS2]=0.3 g/L,
[PMS]=1.5 mmol/L
pH=3, T=25℃60 min, 95% [51] MoS2/Co(Ⅱ)/PMS RhB [RhB]=30 μmol/L,
[Co(Ⅱ)]=2 μmol/L,
[MoS2]=0.5 g/L,
[PMS]=0.2 mmol/L pH=5.55 min, 100% [53] Loaded MoS2/PMS SMG/Fe(Ⅱ)/PMS SD [SD]=20 mg/L,
[Fe(Ⅱ)]=0.25 mg/L,
[SMG loaded MoS2]=1 g/L,
[PMS]=150 mg/L, T=25℃30 min, 98.3% [59] MoS2/CuFe2O4/PMS Fluoxetine [Fluoxetine]=20 mg/L,
[MoS2/CuFe2O4]=0.1 g/L,
[PMS]=1 mmol/L
pH=6.9, T=25℃20min, 97.3% [60] Vis/3D urchin-like MoS2/C/PMS LEV [LEV]=70 mg/L,
[3D urchin-like MoS2/C]=0.1 g/L,
[PMS]=0.9 g/L
Vis: 30 mW·cm−2, 420 nm
pH=7, T=25℃80min, 100% [61] Vis/WO3/MoS2/Ag/PMS BPA [BPA]=10 mg/L,
[WO3/MoS2/Ag]=0.8 g/L,
[PMS]=1 g/L
Vis: 2 000 mW·cm−2, 420 nm
pH=9, T=25℃140 min, > 90% [62] Vis/MoS2/Ag/g-C3N4/PMS TC [TC]=20 mg/L,
[MoS2/Ag/g-C3N4]=0.2 g/L,
[PMS]=0.1 mmol/L
Vis: 300 W, 420 nm
pH=5.5, T=20℃50 min, 98.9% [63] Doped MoS2/PMS FexMo1−xS2/PMS PPA [PPA]=10 μmol/L
[FexMo1−xS2]=0.1 g/L,
PMS=1 mmol/L,pH=4.030 min, 90% [65] Vis/Co-MoS2/PMS OFX [OFX]=20 mg/L,
[Co-MoS2]=0.1 g/L,
[PMS]=0.75 g/L
Vis: 300 W, 420 nm pH=9, T=20℃30 min, 91.1% [66] Notes: BPA—Bisphenol A; CBZ—Carbamazepine; SD—Sulfadiazine; LEV—Levofloxacin; TC—Tetracycline; PPA—Propranolol; OFX—Ofloxacian; T—Temperature. -
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