Key Laboratory of Catalysis and Materials Science of the State Ethnic Affairs Commission & Ministry of Education, Hubei Province, College of Resources and Environmental Science, South-Central University for Nationalities, Wuhan 430074, PR China.
National Demonstration Center for Experimental Ethnopharmacology Education (South-Central University for Nationalities), Wuhan, 430074, China.
Environ Sci Technol. 2021 Jan 19;55(2):1260-1269. doi: 10.1021/acs.est.0c06825. Epub 2021 Jan 8.
Heterogeneous electro-Fenton (HEF) reaction has been considered as a promising process for real effluent treatments. However, the design of effective catalysts for simultaneous HO generation and activation to achieve bifunctional catalysis for O toward •OH production remains a challenge. Herein, a core-shell structural Fe-based catalyst (FeNC@C), with FeC and FeN nanoparticles encapsulated by porous graphitic layers, was synthesized and employed in a HEF system. The FeNC@C catalyst presented a significant performance in degradation of various chlorophenols at various conditions with an extremely low level of leached iron. Electron spin resonance and radical scavenging revealed that •OH was the key reactive species and Fe would play a role at neutral conditions. Experimental and density function theory calculation revealed the dominated role of FeC in HO generation and the positive effect of FeN sites on HO activation to form •OH. Meanwhile, FeNC@C was proved to be less pH dependence, high stability, and well-recycled materials for practical application in wastewater purification.
非均相电芬顿(HEF)反应已被认为是一种很有前途的实际废水处理方法。然而,设计同时产生 HO 和激活 HO 以实现 O 向 •OH 生产的双功能催化的有效催化剂仍然是一个挑战。本文合成了一种具有核壳结构的 Fe 基催化剂(FeNC@C),其中多孔石墨层包裹着 FeC 和 FeN 纳米颗粒,并将其应用于 HEF 体系中。在各种条件下,FeNC@C 催化剂在降解各种氯酚方面表现出优异的性能,且铁浸出量极低。电子自旋共振和自由基清除实验表明,•OH 是关键的反应性物质,Fe 在中性条件下起作用。实验和密度泛函理论计算表明,FeC 主要负责 HO 的生成,而 FeN 位则有利于 HO 的激活以形成 •OH。同时,FeNC@C 还表现出较低的 pH 依赖性、较高的稳定性和良好的可回收性,可实际应用于废水净化。