编者按:
高级氧化技术常用于高浓度有毒难降解有机污染物的预处理和微量新兴污染物的深度处理，本专题将从新型催化材料可控制备、催化氧化还原工艺和机制、降解机理、毒性产物分析和调控等方面介绍国内青年学者在高级氧化方面的研究进展. 具体研究工作包括：活化过硫酸盐、活化过氧乙酸、光催化氧化、电催化、助催化(类)芬顿等高级氧化技术在高浓度有机物污染物的预处理、微量药物类污染物的深度处理以及病原微生物杀灭方面的研究. 现将相关研究成果集中发表，以期为高浓度有机工业废水预处理和医疗污水同步消毒降解技术的研究提供参考.
Research Progress in Degradation of Organic Pollutants by Inorganic Co-Catalytic Fenton and Fenton-Like Reactions
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摘要: 芬顿技术常用于去除水中的有机污染物，通过向溶液中加入Fe2+和H2O2便可以产生自由基并进一步氧化有机物，但传统的芬顿技术总是伴随着诸如铁泥、较窄的pH适用范围等缺点. 近年来，以MoS2为代表的一类无机助催化剂可以有效地促进(类)芬顿反应中Fe2+/Fe3+的循环以及反应中自由基的生成，MoS2因其表面存在的还原态金属活性中心可以有效地还原Fe3+或Co3+等金属离子并减少元素的流失. 为了进一步明确无机助催化剂的性能和微观机制，本文综述了以MoS2为代表的助催化剂在均相和非均相芬顿反应中对于H2O2及PMS的活化效果. 结果表明：无论是在均相还是非均相(类)芬顿反应中，MoS2、CoS2等表面存在的还原态金属活性中心均能显著促进(类)芬顿反应中金属离子的循环，并提高反应中强氧化性活性氧物种的浓度，而一些助催化剂在助催化芬顿反应的同时，甚至可以自产活性氧物种或是自主活化PMS. 但目前的研究仍存在一些不足，如无机助催化剂极有可能会给反应体系带来重金属离子的二次污染，一般的非均相催化剂及助催化剂的使用时限较短，并不能满足实际工业化的应用. 因此在未来的研究中，提高催化剂和助催化剂的反应稳定性和进一步提高反应活性应作为研究的重点. 其中，将纳米技术与催化剂和助催化剂的制备相结合，或进一步改善助催化剂的效能均可能有效推进无机催化剂及助催化剂在工业应用上的进程.
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关键词:
- 助催化剂 /
- 芬顿反应 /
- 污染物降解 /
- 二硫化钼(MoS2)
Abstract: The Fenton process has been widely employed to treat organic pollutants in water since its development. By adding Fe2+ and H2O2 to the solution, free radicals are generated to oxidize organic compounds. However, the traditional Fenton process is accompanied by shortcomings such as a narrow adaptable pH range and the formation of iron sludge. In recent years, novel inorganic co-catalysts represented by MoS2 have been found to effectively promote the circulation of Fe2+/Fe3+ and the generation of free radicals in Fenton and Fenton-like reaction. MoS2 can effectively reduce metal ions such as Fe3+ or Co3+ and abate the loss of elements due to the reduced metal active centers on the surface of MoS2. In order to further clarify the performance and micro-mechanism of inorganic co-catalysts, the activation effects of co-catalyst represented by MoS2 on H2O2 and PMS in homogeneous and heterogeneous Fenton reactions were reviewed. The results showed that whether in homogeneous or heterogeneous Fenton-like reaction, the reduced metal active centers on the surface of MoS2 or CoS2 could significantly promote the circulation of metal ions in Fenton-like reaction and increase the concentration of oxidizing active oxygen species in the reaction system, and some co-catalysts could even produce additional active oxygen species or activate PMS autonomously while promoting the Fenton reactions. However, there are still some shortcomings in the current research. For example, inorganic co-catalysts may cause secondary pollution of heavy metals. In addition, the service lives of common heterogeneous catalysts and co-catalysts are relatively short and inadequate for practical industrial applications. Therefore, future research should focus on improving the reaction stability and overall activity of catalysts and co-catalysts. Thereinto, the combination of nanotechnologies with the preparation of catalysts and co-catalysts, or further improvement of the efficiency of co-catalysts may greatly promote their industrial applications.-
Key words:
- co-catalyst /
- Fenton reaction /
- degradation of pollutant /
- molybdenum disulfide (MoS2)
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图 1 (类)芬顿反应的几种催化剂以及助催化剂和芬顿反应的大致反应历程
Figure 1. Several catalysts and co-catalysts for Fenton and Fenton-like reactions and the reaction process of Fenton reaction
表 1 无机助催化剂助催化(类)芬顿体系降解有机污染物活性
Table 1. The activity of inorganic co-catalyst to promote Fenton and Fenton-like reaction to degrade organic pollutants
助催化剂 铁源 活性物质 污染物 pH 反应时间/min 降解率/% 污染物浓度/(mg/L) 数据来源 MoS2 FeSO4·7H2O H2O2 RhB 3.4 0.33 96 20 文献[28] MoS2 FeCl3·6H2O H2O2 RhB 3~5 60 80 10 文献[44] MoS2 FeS H2O2 RhB 6.5 30 90 10 文献[46] MoS2 FeVO4 H2O2 四环素 — 10 70 50 文献[47] SMG FeSO4·7H2O H2O2/PMS 磺胺嘧啶 4.0 15 98.3 20 文献[48] MoS2 — PMS 苯酚 3.0 25 80 10 文献[55] MoS2 — PS 卡马西平 5.8 40 95.3 20 文献[56] MoS2 FeSO4·7H2O PMS 磺胺甲恶唑 3.0 6 88.5 6.3 文献[58] MoS2 Fe3O4 PMS 磺酰胺 3.0 15 99.8 20 文献[59] WS2 FeSO4·7H2O H2O2 苯酚 3.8 1 81 10 文献[60] WS2 FeCl3·6H2O PMS 卡马西平 4.0 10 100 8 文献[61] WS2 ZVI H2O2 L-RhB 4.12 12 100 20 文献[63] Co8S9QD FeSO4·7H2O H2O2 RhB 4.0 10 100 20 文献[72] CoSx FeSO4·7H2O — RhB 4.5 120 73.7 20 文献[73] MoO2 — PMS 1-氯萘 4.4 180 97.87 1 文献[75] MoO2 FeSO4·7H2O PMS L-RhB 3.0 15 100 20 文献[77] MoO2 FeSO4·7H2O H2O2 L-RhB 3.4 3 100 20 文献[78] Mo FeSO4·7H2O H2O2 L-RhB 3.8 5 100 20 文献[79] Mo FeSO4·7H2O PMS RhB 5.6 10 100 20 文献[80] 
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