Grant: Discovery Grants Program - Individual

This research program focuses on fundamental studies of advanced materials targeted for electrochemical energy systems. Specifically metal/metal-alloy nanoparticles, advanced carbon materials as well as combinations of metals nanoparticles with these carbons. Such materials are at the heart of numerous electrochemical energy technologies, including fuel cells, electrolyzers and electrochemical/super capacitors. These technologies have the potential to be more widely deployed in the energy landscape provided that improvements can be made in the performance-to-cost ratio of the materials, and also in their durability. In addition to improvements in the materials themselves, improvements are needed in diagnostic tools that can readily assess multiple indicators of the electrode state-of-health. This proposal is focused on the study and enhancement of new electrode materials and the refinement of electrochemical impedance spectroscopy (EIS) measurements as a go-to diagnostic tool. We have recently developed an EIS-based diagnostic methods that can clearly elucidate the mode of electrode degradation occurring. Specific changes in the EIS profiles occur upon degradation that are characteristic of specific catalyst layer degradation processes, including the degradation of the carbon support and the ionomer. Furthermore, we have modified the transmission line EIS model so that double-layer capacitance (Cdl) can be separated from faradaic pseudo-capacitance (CF) originating from Hupd on Pt. Moreover, we have been able to show that magnitude of CF originating from Hupd is proportional to the Pt surface area, yielding potential-dependent constants that enable accurate measurements of the electrochemically active surface area of a poly-crystalline Pt electrodes from EIS measurements. Together this suite of EIS-based tools has enormous potential to study both the stability of an electrode and also surface processes in applications beyond typical Pt/C electrodes. Thus, our ongoing studies will focus on novel electrode materials, employing EIS to elucidate how the electrode surface is changing over time and also to quantify active surface species, both metallic and carbon-based, and how this impacts activity. Longer-term objectives include an examination of the relationships between structure and relevant properties such as conductivity, electrochemically active surface area, catalytic activity, capacity and performance. Furthermore, we will seek to extend our EIS methodology so that it can be applied universally in the quantification of electrochemically addressable redox species bound to an electrode surface.