Highly effective removal of BPA with boron-doped graphene shell wrapped FeS2 nanoparticles in electro-Fenton process: Performance and mechanism

Highly effective removal of BPA with boron-doped graphene shell wrapped FeS2 nanoparticles in electro-Fenton process: Performance and mechanism
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电芬顿过程中掺硼石墨烯壳包裹 FeS2 纳米粒子高效去除 BPA:性能和机理

DOI:
10.1016/j.seppur.2021.118680
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发表时间:
2021-07
影响因子:
8.6
通讯作者:
Gao Juan
Gao Juan
中科院分区:
工程技术1区
文献类型:
--
作者:
Chu Longgang;Sun Zhaoyue;Fang Guodong;Cang Long;Wang Xinghao;Zhou Dongmei;Gao Juan

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为了防止金属催化剂的团聚和浸出,将金属纳米颗粒包覆在碳壳中成为电芬顿(EF)过程中的研究热点。然而,大多数碳-金属催化剂由于在电极表面不可用的氧化还原反应而遭受缓慢的Fe 2+再生,这阻碍了EF效率。在这里,我们报告了一种新型的硼掺杂石墨烯(BrGO)包裹的FeS 2纳米复合材料(FeS2@BrGO),由于BrGO和FeS 2之间的合成相互作用,以及Fe(II)的有效再生,表现出极高的催化性能。在中性pH条件下,FeS2@BrGO的EF体系可在20 min内完全去除50 mg L-1双酚A. EPR结果表明,体系中存在大量的持久性自由基和还原性硫,可直接向Fe(III)提供电子.电化学测试进一步证明了Fe(III)/Fe(II)的还原电位通过Fe(III)与表面含氧官能团之间的配位而降低。反应性有机自由基在将Fe(III)还原为Fe(II)中也发挥了重要作用。这些发现为石墨烯壳与金属硫化物结合的杂化催化剂提供了一种新的策略,在废水处理中具有巨大的潜力。
To prevent metal catalysts from agglomeration and leaching, encapsulating metal nanoparticles in carbon shells has attracted much attention in electro-Fenton (EF) processes. However, most of the carbon–metal catalysts were suffering from slow regeneration of Fe2+due to the unavailable redox reactions at electrode surface, which hindered the EF efficiency. Here, we report a novel boron doped graphene (BrGO) wrapped FeS2nanocomposite (FeS2@BrGO), which exhibits extremely high catalytic performance due to the synthetic interaction between BrGO and FeS2, as well as the efficient regeneration of Fe(II). The EF system with FeS2@BrGO could completely remove 50 mg L-1bisphenol A within 20 min under neutral pH. EPR results suggest the existing of abundant persistent free radicals and reductive sulfur could directly donate electron to Fe(III). The electrochemical measurements further demonstrated the decreased reduction potential of Fe(III)/Fe(II) by the coordination between Fe(III) and surface oxygen-containing functional groups. Reactive organic radicals also played an important role in reducing Fe(III) to Fe(II). These findings provide a new strategy for hybrid catalysts combining graphene shells with metal sulfide, which has great potential in wastewater treatment.
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