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通过新型 3D AQS/PPy-GF 阴极增强超氧自由基来实现有机物的剧烈降解和发电。

Dramatic enhancement of organics degradation and electricity generation via strengthening superoxide radical by using a novel 3D AQS/PPy-GF cathode.

机构信息

School of Environmental Science and Engineering, Shanghai Jiao Tong University, No. 800 Dongchuan Rd, Shanghai 200240, PR China.

School of Environmental Science and Engineering, Shanghai Jiao Tong University, No. 800 Dongchuan Rd, Shanghai 200240, PR China.

出版信息

Water Res. 2017 Nov 15;125:259-269. doi: 10.1016/j.watres.2017.08.054. Epub 2017 Aug 24.

DOI:10.1016/j.watres.2017.08.054
PMID:28865375
Abstract

A dramatic enhancement of organics degradation and electricity generation has been achieved in a wastewater fuel cell (WFC) system via strengthening superoxide radical with radical chain reaction by using a novel 3D anthraquinone/polypyrrole modified graphite felt (AQS/PPy-GF) cathode. The AQS/PPy-GF was synthesized by one-pot electrochemical polymerization method and used to in-situ generate superoxide radical by reducing oxygen under self-imposed electric field. Results showed that methyl orange (MO) were effectively degraded in AQS/PPy-GF/Fe system with a high apparent rate constant (0.0677 min), which was 3.9 times that (0.0174 min) in the Pt/Fe system and even 9.4 times that (0.0072 min) in the traditional WFC system (without Fe). Meanwhile, it showed a superior performance for electricity generation and the maximum power density output (1.130 mW cm) was nearly 3.3 times and 5.0 times higher, respectively, when compared with the Pt/Fe system and traditional WFC. This dramatic advance was attributed to 3D AQS/PPy-GF cathode which produces more O via one-electron reduction process. The presence of O cannot only directly contribute to MO degradation, but also promotes the final complete mineralization by turning itself to OH. Additionally, O accelerates the Fe/Fe couple cycling, thus avoiding continuous addition of any external ferrous ions. Inhibition and probe studies were conducted to ascertain the role of several radicals (OH and O) on the MO degradation. Superoxide radicals were considered as the primary reactive oxidants, and the degradation mechanism of MO was proposed. The proposed WFC system provides a more economical and efficient way for energy recovery and wastewater treatment.

摘要

通过强化超氧自由基的自由基链式反应,利用一种新型的 3D 蒽醌/聚吡咯修饰石墨毡(AQS/PPy-GF)阴极,在废水燃料电池(WFC)系统中实现了有机物降解和发电的显著增强。AQS/PPy-GF 通过在自施加电场下还原氧气原位生成超氧自由基,采用一锅电化学聚合方法合成,并用于原位生成超氧自由基。结果表明,在 AQS/PPy-GF/Fe 体系中,甲基橙(MO)被有效降解,表观速率常数(0.0677 min)较高,是 Pt/Fe 体系(0.0174 min)的 3.9 倍,甚至是传统 WFC 体系(无 Fe)的 9.4 倍(0.0072 min)。同时,它表现出优异的发电性能,最大输出功率密度(1.130 mW cm)分别比 Pt/Fe 体系和传统 WFC 高近 3.3 倍和 5.0 倍。这种显著的进步归因于 3D AQS/PPy-GF 阴极通过单电子还原过程产生更多的 O。O 的存在不仅可以直接促进 MO 的降解,而且还可以通过自身转化为 OH 来促进最终的完全矿化。此外,O 加速了 Fe/Fe 循环,从而避免了连续添加任何外部亚铁离子。进行了抑制和探针研究以确定几种自由基(OH 和 O)在 MO 降解中的作用。超氧自由基被认为是主要的反应性氧化剂,并提出了 MO 的降解机制。所提出的 WFC 系统为能量回收和废水处理提供了一种更经济、更高效的方法。

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