(PECASE) GUIDING THERMAL CATALYTIC REACTIONS WITH INTERFACIAL ELECTRIC FIELDS
Abstract
Electrostatics have long been known to play an important role in the molecular interactions that mediate chemical transformations, and thus in principle provide a promising mechanism by which to modulate the overall rates and product distributions of catalytic thermal reactions. To this end, this project aims to develop strategies for harnessing the electric fields at electrically polarized interfaces to systematically control the thermodynamics and kinetics of inner-sphere surface reactions. Electrical polarization of solid-liquid interfaces can generate enormous electric fields on the order of 1 V Å?1 . In fact, this very interfacial gradient of electrostatic potential has long been used to drive faradaic redox chemistry and comprises the bedrock of all electrochemical energy conversion technologies. However, there exist few clear experimental examples in which these electric fields have been used to modulate non-faradaic reactivity. This project aims to bridge this gap by elucidating the chemical consequences of three classes of electrostatic interfacial phenomena: (1) interfacial electric field-driven ion excesses to augment reaction selectivity and rate; (2) interfacial electric fields to directly modulate catalyst electronic structure and substrate binding affinity; and (3) interfacial electric field-driven ion binding to surface sites to modulate catalysis. Using electrochemical kinetics and spectroscopic techniques, we will investigate these electrostatic phenomena within the context of catalysis at both metal surfaces and at well-defined molecular catalysts that have been conjugated to graphitic surfaces. This two-pronged approach will enable us to develop a molecular and generalizable framework for how to systematically deploy electrostatics to tune the rate, selectivity, and stability of catalytic processes of practical interest.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Aug 12, 2021
- Source ID
- FA95502010291
Entities
People
- Yogesh Surendranath
Organizations
- Air Force Office of Scientific Research
- Massachusetts Institute of Technology
- United States Air Force