Redefining Charge-Transfer Interfaces for Next-Generation Electrochemical Power Sources
Abstract
The ability to realize next-generation electrochemical power sources with unprecedented energy and power capability requires fundamental insights into the physicochemical processes at nanoscale electrode interfaces. The electrodes in practical power sources comprise complex 3D multifunctional structures that are challenging to characterize and model. The key objective of this research program was to create and analyze well-defined two-dimensional (2D) planar electrodes that effectively mimic the functionality of their 3D counterparts, but in forms that are amenable to a range of surface-sensitive spectroscopy, microscopy, and electroanalytical tools, coupled to new computational understanding of these simplified interfaces. Pyrolytic carbon (pyC) films prepared by chemical vapor deposition served as a planar stand-in for technologically relevant disordered carbons (from powder blacks to advanced 3D carbon architectures). Heteroatom doping of these pyC substrates with elements such as sulfur provided a means to tune their electronic and electrochemical properties, as well as enhancing their adsorptive characteristics for electrocatalytic functionalities such as precious-metal nanoparticles. Nanoscale manganese oxides at pyC substrates were investigated for mechanistic insights into key energy-relevant electrochemical reactions including pseudocapacitive charge-storage, zinc-ion charge storage, and electrocatalytic oxygen reduction. Ruthenium oxide nanoparticulate coatings were used to enhance electron-transfer kinetics at pyC, and also demonstrated effective oxygen-evolution activity and stability when applied to pyrolytic carbon surfaces. We have developed a perturbation theory to model electron transfer in a degenerate system.
Document Details
- Document Type
- Technical Report
- Publication Date
- Oct 23, 2020
- Accession Number
- AD1113833
Entities
People
- Christopher N Chervin
- Christopher R. So
- Daniel Gunlycke
- Debra R. Rolison
- Jeffrey W Long
- Joseph F Parker
- Mark C Palenik
- Megan B. Sassin
Organizations
- United States Naval Research Laboratory