Li Huihui, Quispe-Cardenas Estefanny, Yang Shasha, Yin Lifeng, Yang Yang
State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, China.
Department of Civil and Environmental Engineering, Clarkson University, Potsdam, New York 13699, United States.
ACS ES T Eng. 2022 Feb 11;2(2):242-250. doi: 10.1021/acsestengg.1c00366. Epub 2021 Dec 14.
Hydrogen peroxide (HP) production via electrochemical oxygen reduction reaction (ORR-HP) is a critical reaction for energy storage and environmental remediation. The onsite production of high-concentration HO using gas diffusion electrodes (GDEs) fed by air is especially attractive. However, many studies indicate that the air-GDE combination could not produce concentrated HO, as the [HO] leveled off or even decreased with the increasing reaction time. This study proves that the limiting factors are not the oxygen concentration in the air but the anodic and cathodic depletion of the as-formed HO. We proved that the anodic depletion could be excluded by adopting a divided electrolytic cell. Furthermore, we demonstrated that applying poly(tetrafluoroethylene) (PTFE) as an overcoating rather than a catalyst binder could effectively mitigate the cathodic decomposition pathways. Beyond that, we further developed a composite electrospun PTFE (E-PTFE)/carbon black (CB)/GDE electrode featuring the electrospun PTFE (E-PTFE) nanofibrous overcoating. The E-PTFE coating provides abundant triphase active sites and excludes the cathodic depletion reaction, enabling the production of >20 g/L HO at a current efficiency of 86.6%. Finally, we demonstrated the efficacy of the ORR-HP device in lake water remediation. Cyanobacteria and microcystin-LR were readily removed along with the onsite production of HO.
通过电化学氧还原反应(ORR-HP)生产过氧化氢(HP)是能量存储和环境修复的关键反应。利用空气供给的气体扩散电极(GDEs)现场生产高浓度的HO尤其具有吸引力。然而,许多研究表明,空气-GDE组合无法产生浓缩的HO,因为随着反应时间的增加,[HO]趋于平稳甚至下降。本研究证明,限制因素不是空气中的氧浓度,而是所生成的HO的阳极和阴极消耗。我们证明,采用分隔电解池可以排除阳极消耗。此外,我们证明,将聚四氟乙烯(PTFE)用作外涂层而非催化剂粘合剂可以有效减轻阴极分解途径。除此之外,我们进一步开发了一种复合电纺PTFE(E-PTFE)/炭黑(CB)/GDE电极,其具有电纺PTFE(E-PTFE)纳米纤维外涂层。E-PTFE涂层提供了丰富的三相活性位点并排除了阴极消耗反应,能够以86.6%的电流效率生产>20 g/L的HO。最后,我们展示了ORR-HP装置在湖水修复中的功效。蓝藻和微囊藻毒素-LR随着HO的现场生产而被轻易去除。