Electrocatalytic Self-Healing Mechanisms in Energy Storage Materials
Abstract
Incorporating self-healing and repair mechanisms within batteries, supercapacitors, and other energy storage materials is an important paradigm for enhancing device lifetimes and expanding operating conditions. Success of this approach requires system-specific and tailored chemistry that is commensurate with the operating voltage and temperature windows of the device. Achieving this design paradigm necessitates a detailed understanding of the intrinsic electrochemical interfaces of the device and the ability to tune interfacial redox reactions; for example, compatibility must be ensured between the redox reactions innate to the device operation and the reversible redox reactions that mediate the self-healing and repair mechanisms. We will investigate self-healing mechanisms within carbon nanotube/graphene/polymer composite electrode materials (CNT-PCs), which are an important class of electrodes utilized in Li-ion batteries and supercapacitors. These materials may form cracks or defects upon volume changes during charge/discharge cycles, which may be alleviated with introduction of reversible repair chemistries within the polymer framework. Using first-principles computational approaches, we will evaluate and design electro-catalytically mediated reversible chemistries to be incorporated into the polymer framework that enable dynamic repair. We will obtain accurate predictions of oxidation potentials and transition state free energy barriers for these reactions, examining various functionalization and different device parameters. The goal is to understand how the physics of the electrochemical double layer affects this chemical reactivity, which is essential for bottom-up design of self-healing repair mechanisms. A major thrust will be to develop and benchmark a novel fixed voltage QM/MM approach for computational electrochemistry that incorporates the full physics of the electrochemical double layer.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Jan 21, 2022
- Source ID
- FA95502210025XX0
Entities
People
- Jesse McDaniel
Organizations
- Air Force Office of Scientific Research
- Georgia Tech Research Corporation
- United States Air Force