Efficient electrochemical dehalogenation of florfenicol without discharging toxic intermediates via direct electron transfer over electrochromic WO3
Efficient electrochemical dehalogenation of florfenicol without discharging toxic intermediates via direct electron transfer over electrochromic WO3
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通过电致变色 WO3 上的直接电子转移，对氟苯尼考进行高效电化学脱卤，而不释放有毒中间体
DOI：
10.1016/j.cej.2020.127481
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发表时间：
2020-10
影响因子：
15.1
通讯作者：
Luo Shenglian
中科院分区：
文献类型：
--
作者：
Yang Lixia;Chen Zhenglin;Ma Tianzhu;Zhang Shuqu;Dai Weili;Xiao Xiao;Luo Xubiao;Zou Jianping;Tu Xinman;Yang Liming;Luo Shenglian
采用阳极氧化法制备了自负载型电致变色WO_3纳米簇电催化剂，实现了氟苯尼考(Flo)的完全脱卤化，有效地抑制了有毒中间体的产生。由WO_3纳米片组成的三维全方位WO_3团簇是在W网衬底上生长的，由于其固有的电子储存和自支撑性质，它可以作为催化剂和电极，通过直接电子转移实现完全脱卤化。在偏置电势的辅助下，在多孔的WO_3界面上产生并保留了连续的电子流，为激活C-Cl和C-F键分离卤素基团创造了一个富含电子的环境。最优的WO_3/W在25 V时的电催化脱卤率最高，为99.7%。用Fukui指数预测了可能的电子攻击位置，并从氟化氢分解中间产物的MS中得到了印证。ECOSAR模拟和。共生评价证明，不含-F和-Cl的化学品对生态系统无危害。特别是，自负载型WO_3纳米簇电催化剂表现出优异的耐久性，运行20小时后活性不会下降，这表明在建立一种可行的、经济有效的、持久的抗生素脱卤化电化学策略方面具有广阔的前景。
Complete dehalogenation of florfenicol (FLO) was realized on a self-supporting, electrochromic WO3nanocluster electrocatalyst prepared by anodization, effectively inhibiting the generation of toxic intermediates that can pose harmful influence on the ecosystem. Three dimensional, omnidirectional WO3clusters made up of WO3nanoflakes are grown from a W mesh substrate, which can work as catalyst and electrode enable the complete dehalogenation via a direct electron transfer because of the inherent electron-storage and self-supporting nature. Assisted by bias potential, continuous electron streams are generated and reserved in the porous WO3interface, building an electron-rich circumstance for activating the C–Cl and C–F bonds to detach the halogen groups. The best electrocatalytic dehalogenation performance, 99.7% in 120 min was acquired using the optimal WO3/W anodized at 25 V. The possible sites attacked by electrons is predicted by Fukui index, that is evidenced by the MS of intermediates originated from FLO decomposition. ECOSAR simulation andE. colisurviving evaluation verifies that there is no hazard on ecosystem of the chemicals without –F and –Cl. Particularly, the self-supporting WO3nanocluster electrocatalyst exhibits a superior durability with no decay in activity after 20 h running, indicating a promising prospect in establishing a feasible, cost-effective, and durable electrochemical strategy for antibiotic dehalogenation.
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