Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2021-06-18 , DOI: 10.1016/j.jhazmat.2021.126434 Shuzhao Pei 1 , Han Shi 1 , Jinna Zhang 1 , Shengli Wang 1 , Nanqi Ren 1 , Shijie You 1
This study reports fluorine-doped titanium suboxide anode for electrochemical mineralization of hydrophobic micro-contaminant, tetrabromobisphenol A. Fluorinated TiSO anode promoted electro-generated hydroxyl radicals (•OH) with higher selectivity and activity, due to increased O2 evolution potential and more loosely interaction with hydrophobic electrode surface. For electro-oxidation process, fluorine doping had an insignificant impact on outer-sphere reaction and exerted inhibition on inner-sphere reaction, as indicated by cyclic voltammogram performed on Ru(NH3)63+/2+, Fe(CN)63−/4− and Fe3+/2+ redox couple. This facilitated electrochemical conversion of TBBPA and intermediates via more efficient outer-sphere reaction and hydroxylation route. Additionally, generated O2 micro-bubbles could be stabilized on hydrophobic F-doped TiSO anode, which extended the three-phase boundary available for interfacial enrichment of TBBPA and subsequent mineralization. Under action of these comprehensive factors, 0.5% F-doped TiSO electrochemically reactive membrane could achieve 99.7% mineralization of TBBPA upon energy consumption of 0.52 kWh m-3 at current density of 7.8±0.24 mA cm-2 (3.75 V vs SHE) and flow rate of 1628 LHM based on flow-through electrolysis. The modified anode exhibited superior performances compared with un-modified one with more efficient TBBPA removal, less toxic intermediate accumulation and lower energy consumption. The results may have important implications for electrochemical removal and detoxification of hydrophobic micro-pollutants.
中文翻译:
掺氟低氧化钛电化学反应膜电化学去除四溴双酚A
本研究报告了氟掺杂的低氧化钛阳极用于疏水性微污染物四溴双酚 A 的电化学矿化。氟化 TiSO 阳极促进了具有更高选择性和活性的电生成羟基自由基 (•OH),因为 O 2析出电位增加且更松散与疏水电极表面相互作用。对于电氧化过程,氟掺杂对外球反应的影响不显着,对内球反应产生抑制作用,如对Ru(NH 3 ) 6 3+/2+ , Fe(CN) 6 的循环伏安图所示3-/4-和 Fe 3+/2+氧化还原对。这通过更有效的外球反应和羟基化途径促进了 TBBPA 和中间体的电化学转化。此外,生成的 O 2微气泡可以稳定在疏水性掺杂 F 的 TiSO 阳极上,这扩展了可用于 TBBPA 界面富集和后续矿化的三相边界。下的这些综合因素作用,0.5%F掺杂TISO电化学反应性膜可以实现TBBPA的在0.52千瓦时米的能量消耗99.7%矿化-3在7.8±0.24电流密度 毫安 厘米-2(3.75 V vs SHE) 和基于流通电解的 1628 LHM 的流速。与未改性阳极相比,改性阳极表现出优异的性能,具有更有效的 TBBPA 去除、更少的有毒中间体积累和更低的能耗。该结果可能对疏水性微污染物的电化学去除和解毒具有重要意义。