Galbicsek Noémi V, Kormányos Attila, Samu Gergely Ferenc, Ayyub Mohd M, Kotnik Tomaž, Kovačič Sebastijan, Janáky Csaba, Endrődi Balázs
Department of Physical Chemistry and Materials Science, University of Szeged, Rerrich Square 1, Szeged H-6720, Hungary.
ELI-ALPS, ELI-HU Non-Profit Ltd., Wolfgang Sandner Street 3, 6728, Szeged H-6728, Hungary.
Energy Fuels. 2024 Nov 5;38(22):22307-22314. doi: 10.1021/acs.energyfuels.4c04058. eCollection 2024 Nov 21.
Electrochemical reduction of carbon monoxide offers a possible route to produce valuable chemicals (such as acetate, ethanol or ethylene) from CO in two consecutive electrochemical reactions. Such deeply reduced products are formed via the transfer of 4-6 electrons per CO molecule. Assuming similar-sized CO and CO electrolyzers, 2-3-times larger current densities are required in the latter case to match the molar fluxes. Such high reaction rates can be ensured by tailoring the structure of the gas diffusion electrodes. Here, the structure of the cathode catalyst layer was systematically varied using different polymeric binders to achieve high reaction rates. Simple linear polymers, bearing the same backbone but different functional groups were compared to highlight the role of different structural motifs. The comparison was also extended to simple linear, partially fluorinated polymers. Interestingly, in some cases similar results were obtained as with the current state-of-the-art binders. Using different surface-wetting characterization techniques, we show that the hydrophobicity of the catalyst layer-provided by the binder- is a prerequisite for high-rate CO electrolysis. The validity of this notion was demonstrated by performing CO electrolysis experiments at high current density (1 A cm) for several hours using PVDF as the catalyst binder.
一氧化碳的电化学还原提供了一条可能的途径,可通过两个连续的电化学反应从一氧化碳生产有价值的化学品(如醋酸盐、乙醇或乙烯)。此类深度还原产物是通过每个一氧化碳分子转移4至6个电子形成的。假设一氧化碳和一氧化碳电解槽尺寸相似,在后一种情况下需要大2至3倍的电流密度才能匹配摩尔通量。通过调整气体扩散电极的结构可以确保如此高的反应速率。在此,使用不同的聚合物粘合剂系统地改变阴极催化剂层的结构,以实现高反应速率。比较了具有相同主链但不同官能团的简单线性聚合物,以突出不同结构基序的作用。该比较还扩展到简单的线性部分氟化聚合物。有趣的是,在某些情况下,获得了与当前最先进的粘合剂相似的结果。使用不同的表面润湿性表征技术,我们表明由粘合剂提供的催化剂层的疏水性是高速率一氧化碳电解的先决条件。通过使用聚偏氟乙烯作为催化剂粘合剂在高电流密度(1 A/cm²)下进行数小时的一氧化碳电解实验,证明了这一观点的正确性。