Monteiro Mariana C O, Dieckhöfer Stefan, Bobrowski Tim, Quast Thomas, Pavesi Davide, Koper Marc T M, Schuhmann Wolfgang
Leiden Institute of Chemistry, Leiden University Einsteinweg 55 2333CC Leiden The Netherlands
Analytical Chemistry-Center for Electrochemical Sciences (CES), Faculty of Chemistry and Biochemistry, Ruhr-Universität Bochum Universitätsstr. 150 D-44780 Bochum Germany
Chem Sci. 2021 Nov 9;12(47):15682-15690. doi: 10.1039/d1sc05519d. eCollection 2021 Dec 8.
Large scale CO electrolysis can be achieved using gas diffusion electrodes (GDEs), and is an essential step towards broader implementation of carbon capture and utilization strategies. Different variables are known to affect the performance of GDEs. Especially regarding the catalyst loading, there are diverging trends reported in terms of activity and selectivity, for CO reduction to CO. We have used shear-force based Au nanoelectrode positioning and scanning electrochemical microscopy (SECM) in the surface-generation tip collection mode to evaluate the activity of Au GDEs for CO reduction as a function of catalyst loading and CO back pressure. Using a Au nanoelectrode, we have locally measured the amount of CO produced along a catalyst loading gradient under conditions. We observed that an optimum local loading of catalyst is necessary to achieve high activities. However, this optimum is directly dependent on the CO back pressure. Our work does not only present a tool to evaluate the activity of GDEs locally, it also allows drawing a more precise picture regarding the effect of catalyst loading and CO back pressure on their performance.
使用气体扩散电极(GDE)可以实现大规模的CO电解,这是更广泛实施碳捕获和利用策略的关键一步。已知不同变量会影响GDE的性能。特别是在催化剂负载方面,关于将CO还原为CO的活性和选择性,有不同的趋势报道。我们使用基于剪切力的金纳米电极定位和扫描电化学显微镜(SECM)在表面产生尖端收集模式下,评估金GDE将CO还原的活性作为催化剂负载和CO背压的函数。使用金纳米电极,我们在一定条件下局部测量了沿催化剂负载梯度产生的CO量。我们观察到,要实现高活性,需要有最佳的局部催化剂负载。然而,这个最佳值直接取决于CO背压。我们的工作不仅提供了一种局部评估GDE活性的工具,还能更精确地描绘催化剂负载和CO背压对其性能的影响。