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使用 Ti 板上结晶 CoP 纳米片阵列通过直接阴极还原和原子 H 深度脱氟氟苯尼考

Deep Dehalogenation of Florfenicol Using Crystalline CoP Nanosheet Arrays on a Ti Plate via Direct Cathodic Reduction and Atomic H.

机构信息

State Key Laboratory of Chemo/Biosensing and Chemometrics , Hunan University , Changsha 410082 , P. R. China.

Research Center for Eco-Environmental Sciences , Chinese Academy of Sciences , Beijing 100085 , P. R. China.

出版信息

Environ Sci Technol. 2019 Oct 15;53(20):11932-11940. doi: 10.1021/acs.est.9b04352. Epub 2019 Sep 24.

Abstract

Efficient elimination of antibacterial activity of halogenated antibiotics by dehalogenation pretreatment is desired for a biochemical treatment process. In this study, crystalline cobalt phosphide nanosheet arrays on a Ti plate (C-CoP/Ti) are fabricated by a simple electrodeposition and phosphorization process. The crystalline structure greatly promotes atomic hydrogen (H*) generation. Moreover, the nanosheet arrays can provide abundant active sites and accelerate electron transfer and mass transport. As a result, the dehalogenation rate of florfenicol (FLO, an emerging organic pollutant) on C-CoP/Ti is 11.1, 2.97, and 13.6 times higher than that on amorphous CoP/Ti, Pd/Ti, and bare Ti, respectively. The C-CoP/Ti electrode achieves 97.4% dehalogenation of FLO (20 mg L) within 30 min at -1.2 V (vs Ag/AgCl). Nearly 100% of Cl and 20% of F are broken away within 120 min, showing the highest electrocatalytic defluorination efficiency reported so far. Both experimental results and theoretical calculations reveal that the dehalogenation of FLO on C-CoP/Ti is synergistically accomplished via direct reduction of electron transfer and indirect reduction of H*. This study develops a highly efficient non-noble metal electrode material for dehalogenation of halogenated organic compounds.

摘要

为了进行生化处理,希望通过脱卤预处理来有效消除卤化抗生素的抗菌活性。在这项研究中,通过简单的电沉积和磷化工艺在 Ti 板上制备了结晶型钴磷纳米片阵列(C-CoP/Ti)。结晶结构极大地促进了原子氢(H*)的生成。此外,纳米片阵列可以提供丰富的活性位点,加速电子转移和质量传输。因此,C-CoP/Ti 上氟苯尼考(FLO,一种新兴的有机污染物)的脱卤速率分别比非晶态 CoP/Ti、Pd/Ti 和裸 Ti 高 11.1、2.97 和 13.6 倍。在-1.2 V(相对于 Ag/AgCl)下,C-CoP/Ti 电极在 30 min 内即可实现 FLO(20 mg/L)的 97.4%脱卤。在 120 min 内,几乎 100%的 Cl 和 20%的 F 被去除,显示出迄今为止报道的最高电催化脱氟效率。实验结果和理论计算都表明,C-CoP/Ti 上 FLO 的脱卤是通过电子转移的直接还原和 H*的间接还原协同完成的。本研究开发了一种高效的非贵金属电极材料,用于卤化有机化合物的脱卤。

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