Understanding plasmonic electrode reshaping
Abstract
Achieving a fundamental understanding of the physics and chemistry that underlie light-assisted electrochemical redox reactions at nanoscale metal electrodes is crucial to improvements in light-weight, rechargeable energy sources. The objective of this proposal is to characterize the electrochemically and optically aided reshaping of single nanostructured metallic electrodes using single particle spectro-electrochemical microscopy in order to develop means to prevent or direct selective shape and size changes. This project will build on our expertise in developing spectroscopic imaging tools to understand the dynamics that occur at plasmonic nanoparticle electrode surfaces. In addition, we will study how these reactions relate, at the nanoscale, to changes in electrode structure and electrolyte interactions at the interface. These experiments will address the important recent observation that nanoscale interfacial redox processes are heterogeneous in that each nanoparticle electrode is unique in its surface chemistry and structure. Single particle methods are crucial to achieve an accurate descriptions of the heterogeneous and often irreversible processes occurring during electrochemical redox reactions. To accomplish our objective, we will pursue the following project goals (1) Determine the kinetics of electrode reshaping under electrochemical bias and strongly corrosive electrolytes while also illuminating with light. (2) Understand the role of surface chemistry on the reshaping of single nanoelectrodes and develop methods to prevent and/or direct shape and size changes. (3) Apply the knowledge gained in Goals 1 and 2 to control electrode reshaping of large area nanostructured electrodes made from a variety of metals. Key outcomes of this project include the determination of dissolution and reshaping mechanisms to allow for optimum device configuration. Also, knowledge gained from this project will lead to the ability to direct shape changes at the nanoscale for more efficient and/or targeted electrode functionality. Finally, we will pursue large area control of electrode arrays composed of earth abundant metals. If we can remove inter-particle and intra-particle heterogeneities and unambiguously correlate shape changes of nanoelectrode arrays with their morphology, local surface chemistry and hot carrier physics, this new knowledge could lead to the rational design of compact, reusable power generation and storage applications with direct benefit to the ArmyÕs mission.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Jun 10, 2019
- Source ID
- W911NF1910363
Entities
People
- Christy F Landes
Organizations
- Army Contracting Command
- Rice University
- United States Army