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Bifunctional Catalytic Cooperativity on Nanoedge: Oriented Ce–Fe Bimetallic Fenton Electrocatalysts for Organic Pollutant Control
ACS ES&T Engineering Pub Date : 2021-10-12 , DOI: 10.1021/acsestengg.1c00149
Ying Liu 1, 2 , Yulin Yang 1, 2 , Wei Miao 1, 2 , Ningjie Du 1, 2 , Dandan Wang 1, 2 , Hehe Qin 1, 2 , Shun Mao 1, 2 , Kostya Ken Ostrikov 3
Affiliation  

Electro-Fenton (EF) is one of the promising clean and renewable technologies for organic pollutant control. However, insufficient hydrogen peroxide (H2O2) generation and the subsequent hydroxyl radicals (OH) conversion still prevent the wide applications of EF. Herein, we report a Ce-doped vertically aligned α-FeOOH nanoflakes anchored on a carbon felt (CF) cathode for EF operation. In this system, a high concentration H2O2 (113.6 mg/L on 4 cm2 cathode) is generated in 60 min, and being efficiently catalyzed to OH by virtue of the active nanoedge (1.6 nm thickness) of Ce-doped α-FeOOH. The OH production rate is calculated as high as 4.2 mM/W/cm2/min, which is ∼6.6-fold higher compared with the unmodified CF electrode. Moreover, this novel cathode achieves a complete removal (100% removal rate) of ultrahigh concentration chloramphenicol (1.1 mM, 355 mg/L) in 8 h and a high mineralization rate (94%) in 29 h in a scaled-up EF system. Density functional theory calculations (DFT) reveal that the Ce doping in α-FeOOH greatly promotes the conversion of H2O2 into OH. This study not only offers a novel cathode structure for EF process but also opens radically new prospects for applied environmental catalysis.

中文翻译:

纳米边缘上的​​双功能催化协同作用:用于有机污染物控制的定向 Ce-Fe 双金属芬顿电催化剂

Electro-Fenton (EF) 是一种很有前途的清洁和可再生有机污染物控制技术。然而,过氧化氢 (H 2 O 2 ) 生成不足和随后的羟基自由基 ( OH) 转化仍然阻碍了 EF 的广泛应用。在此,我们报告了一种固定在碳毡 (CF) 阴极上用于 EF 操作的 Ce 掺杂的垂直排列的 α-FeO​​OH 纳米薄片。在该系统中,高浓度 H 2 O 2(4 cm 2阴极上的 113.6 mg/L )在 60 分钟内产生,并通过 Ce 掺杂的活性纳米边缘(1.6 nm 厚度)有效催化为 OH α-FeO​​OH。该计算出的 OH 生成速率高达 4.2 mM/W/cm 2 /min,与未修饰的 CF 电极相比,高约 6.6 倍。此外,这种新型阴极在放大的 EF 系统中实现了在 8 小时内完全去除(100% 去除率)超高浓度氯霉素(1.1 mM,355 mg/L)和在 29 小时内实现高矿化率(94%) . 密度泛函理论计算 (DFT) 表明,α-FeO​​OH 中的 Ce 掺杂极大地促进了 H 2 O 2 OH的转化。这项研究不仅为 EF 工艺提供了一种新的阴极结构,而且为应用环境催化开辟了全新的前景。
更新日期:2021-12-10
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