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气体扩散电极的跨电极压力对电化学产过氧化氢有显著影响。

Trans-electrode pressure of gas-diffusion electrodes significantly influencing the electrochemical hydrogen peroxide production.

作者信息

Xu Anlin, Yang Ziyan, Zhou Zhiyi, Yang Pu, Yu Yang, Liu Jiayang, Zhang Yunhai

机构信息

School of Environmental Science and Engineering, Nanjing Tech University, Nanjing, 211816, China.

School of Environmental Science and Engineering, Nanjing Tech University, Nanjing, 211816, China.

出版信息

Chemosphere. 2024 Aug;361:142464. doi: 10.1016/j.chemosphere.2024.142464. Epub 2024 May 27.

Abstract

Hydrogen peroxide (HO) synthesis by electrochemical two-electron oxygen reduction has garnered increasing interest as a wide range of potential applications. Gas diffusion electrodes (GDEs) can effectively promote the HO production efficiency by overcoming the oxygen mass transfer limitations but strongly influenced by the electrowetting process along the long-term operation. In this study, the effect of trans-electrode pressure (TEP) of GDE cathode on the electrowetting process was further elucidated. We controlled the TEP values of four types of GDEs: two Ni-based GDEs and two carbon cloth GDEs prepared by hot-pressing or brushing carbon black. SBA-15 was further used to regulate the microstructure of one Ni-based GDE. It was found that an optimal range of TEP occurred for all tested GDEs in terms of the max. concentration, the yield efficiency, the energy consumption, and the stability because TEP may change the triple-phase interface and influence the anti-electrowetting effect. The porosity of hot-pressed Ni GDE can maintain the TEP window and thus enhance the production of HO, likely via creating oxygen-containing functional groups and a bimodal pore structure on the electrode, revealed with several characterization techniques including SEM, CA, XPS, Raman spectra, CV and EIS. The porous Ni GDE presented an efficient and stable production of HO for 10 cycles: yielding HO at 4393.2-4602.2 mmol m h with current efficiencies of 94.2-98.7%. The best accumulated HO concentration can reach up to 3.58 ωt% HO at 10 h. The results provide an important reference for the industrial scaleup of electro-production of HO with GDEs.

摘要

通过电化学双电子氧还原合成过氧化氢(HO)作为一种具有广泛潜在应用的方法,已引起越来越多的关注。气体扩散电极(GDE)可以通过克服氧气传质限制来有效提高HO的生产效率,但在长期运行过程中会受到电润湿过程的强烈影响。在本研究中,进一步阐明了GDE阴极的跨电极压力(TEP)对电润湿过程的影响。我们控制了四种类型GDE的TEP值:两种镍基GDE和两种通过热压或刷涂炭黑制备的碳布GDE。SBA-15进一步用于调节一种镍基GDE的微观结构。研究发现,对于所有测试的GDE,在最大浓度、产率效率、能量消耗和稳定性方面都存在一个最佳的TEP范围,因为TEP可能会改变三相界面并影响抗电润湿效果。热压镍GDE的孔隙率可以维持TEP窗口,从而提高HO的产量,这可能是通过在电极上形成含氧官能团和双峰孔隙结构实现的,这通过扫描电子显微镜(SEM)、接触角(CA)、X射线光电子能谱(XPS)、拉曼光谱、循环伏安法(CV)和电化学阻抗谱(EIS)等多种表征技术得以揭示。多孔镍GDE在10个循环中呈现出高效稳定的HO生产:HO产量为4393.2 - 4602.2 mmol m h,电流效率为94.2 - 98.7%。在10小时时,最佳累积HO浓度可达3.58 ωt% HO。这些结果为使用GDE进行HO电生产的工业放大提供了重要参考。

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