CAREER: Unraveling Chemical and Structural Dynamics in Multi-step Multi-electron Conversion Reactions

About This Grant

A class of chemical reactions called multi-step multi-electron conversion reactions may help improve a variety of energy storage technologies including next generation batteries. However, controlling these chemical reactions is challenging. This CAREER project will conduct experiments to analyze these reactions in a lithium-sulfur battery as a model system. The results will show how the chemistry and material properties of such systems affect their performance. The outcomes will help improve the predictability and efficiency of battery materials and improve resource utilization. The project’s insights will advance foundational knowledge in electrochemistry and materials science. The project will integrate research and education by engaging students in hands-on discovery and by developing new instructional materials based on the research. The activities will expand the future science and engineering workforce and contribute to long-term technological leadership in energy and materials innovation. The primary goal of this project is to elucidate the fundamental redox mechanisms underlying multistep, multielectron conversion reactions by establishing the principles governing the dynamic interplay between chemical evolution and multiscale structural transformations of materials. Using lithium-sulfur batteries as a model system, the project will address critical knowledge gaps and determine how coupled chemical and structural dynamics influence the thermodynamic, kinetic, and transport landscape of the redox system. Specifically, it will (i) investigate how atomic-scale motifs in active materials affect the redox barriers in solid-to-liquid reactions; (ii) establish a generalizable framework linking phase transitions, chemical speciation, and redox barriers within confined environments; (iii) deconvolute the interplay between mass transport and phase transformations to clarify overpotential signatures of liquid-to-solid conversions; and (iv) elucidate how molecular interactions between redox intermediates and local environment control key reaction barriers. These objectives will be pursued using integrated operando electrochemical–spectroscopic methodologies to directly correlate material structure, local chemical environment, and electrochemical behavior. The resulting insights will provide a fundamental, generalizable framework for interpreting complex electrochemical mechanisms and establishing structure–function relationships critical for the rational design of conversion-based redox systems, with principles broadly applicable to electrochemical processes involving coupled redox and phase transformations. This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.