Zhou Wei, Rajic Ljiljana, Zhao Yuwei, Gao Jihui, Qin Yukun, Alshawabkeh Akram N
School of Energy Science and Engineering, Harbin Institute of Technology, Harbin, Heilongjiang, P. R. China.
Department of Civil and Environmental Engineering, Northeastern University, Boston, MA, USA.
Electrochim Acta. 2018 Jul 1;277:185-196. doi: 10.1016/j.electacta.2018.04.174. Epub 2018 Apr 30.
The Electro-Fenton process for in-situ HO electrogeneration is impacted by low O utilization efficiency (<0.1%) and the need of acid for pH adjustment. An electrochemical flow-through cell can develop localized acidic conditions, coupled with simultaneous formation and utilization of O to enhance HO formation. Multiple electrode configurations using reticulated vitreous carbon (RVC) foam and Ti/mixed metal oxides (MMO) are proposed to identify the optimum conditions for HO formation in batch and flow-through cells. A pH of 2.75±0.25 is developed locally in the flow-through cell that supports effective O reduction. Up to 9.66 mg/L HO is generated in a 180 mL batch cell under 100 mA, at pH 2, and mixing at 350 rpm. In flow-through conditions, both flow rate and current significantly influence HO production. A current of 120 mA produced 2.27 mg/L HO under a flow rate of 3 mL/min in a 3-electrode cell with one RVC foam cathode at 60 min. The low current of 60 mA does not enable effective HO production, while the high current of 250 mA produced less HO due to parasitic reactions competing with O reduction. Higher flow rates decrease the retention time, but also increase the O mass transfer. Furthermore, 3-electrode flow-through cell with two RVC foam cathodes was not effective for HO production due to the limited O supply for the secondary cathode. Finally, a coupled process that uses both O and H from water electrolysis is proposed to improve the HO yield further.
用于原位生成羟基自由基(HO)的电芬顿工艺受到低氧利用效率(<0.1%)以及调节pH值需要酸的影响。电化学流通池可以产生局部酸性条件,同时形成并利用氧气以增强羟基自由基的生成。提出了使用网状玻璃碳(RVC)泡沫和钛/混合金属氧化物(MMO)的多种电极配置,以确定在间歇式和流通池中生成羟基自由基的最佳条件。在流通池中局部产生了2.75±0.25的pH值,这有利于有效的氧还原。在100 mA、pH值为2且以350 rpm搅拌的条件下,180 mL间歇式电解槽中可产生高达9.66 mg/L的羟基自由基。在流通条件下,流速和电流都会显著影响羟基自由基的产生。在一个带有一个RVC泡沫阴极的三电极电解槽中,在60分钟时,120 mA的电流在3 mL/min的流速下产生了2.27 mg/L的羟基自由基。60 mA的低电流无法实现有效的羟基自由基生成,而250 mA的高电流由于与氧还原竞争的寄生反应而产生的羟基自由基较少。较高的流速会缩短保留时间,但也会增加氧的传质。此外,由于二次阴极的氧气供应有限,带有两个RVC泡沫阴极的三电极流通池对羟基自由基的产生效果不佳。最后,提出了一种利用水电解产生的氧气和氢气的耦合工艺,以进一步提高羟基自由基的产率。