Public Abstract

DE-SC0026317: Unravelling Cooperative Gas-Surface Coupling via Dynamic Temperature and Electric Field for Transformative Non-equilibrium Synthesis

Award Status: Active

Institution: Purdue University, West Lafayette, IN
UEI: YRXVL4JYCEF5
DUNS: 072051394

Most Recent Award Date: 09/23/2025
Number of Support Periods: 1
PM: Settersten, Thomas

Current Budget Period: 08/01/2025 - 07/31/2026
Current Project Period: 08/01/2025 - 07/31/2030
PI: Dong, Qi

Supplement Budget Period: N/A

Public Abstract

The synergy between gas-phase and surface chemistries plays an essential role in chemical and material syntheses, such as catalytic transformations of gaseous species (e.g., methane conversion, propane dehydrogenation, ammonia synthesis) and vapor deposition processes (e.g., chemical vapor deposition, atomic layer deposition, sputtering). While recent advances in in-operando characterization, advanced spectroscopic/microscopic analysis, ultrafast laser diagnostics, and multiscale modeling have significantly improved the understanding of reaction mechanisms in the gas phase, on surfaces, or both, the cooperative coupling effects between gas-phase and surface chemistries, especially at the space- and time-resolved molecular level, remain elusive. This challenge partly arises from the lack of methodologies to independently modulate the energetics and kinetics of gas-phase and surface species. Moreover, many conventional thermochemical reactions and material syntheses occur under near-equilibrium or near-steady-state conditions, offering limited control over timescales, energy levels, and their temporal patterns. This research aims to achieve a deeper understanding of the gas-surface coupling under non-equilibrium conditions through synergistic and spatiotemporal modulation of surface and gas-phase energies and their delivery patterns, thereby unlocking new opportunities for chemical synthesis and material fabrication. In parallel, this project aims to develop an active-learning-guided, high-throughput experimental platform to tailor the large parameter space of dynamic reactions, thus accelerating mechanistic explorations under complex reaction conditions. Overall, this project will provide a novel platform to investigate molecular-scale gas-surface chemical and material transformations within an underexplored non-equilibrium and dynamic regime. In addition, the decoupled control on the surficial and gas-phase energetics and kinetics will help elucidate the critical cooperative gas-surface coupling. The insights will be highly relevant to energy conversion and storage technologies, as well as transformative manufacturing of chemicals and semiconductors.

The synergy between gas-phase and surface chemistries plays an essential role in chemical and material syntheses, such as catalytic transformations of gaseous species (e.g., methane conversion, propane dehydrogenation, ammonia synthesis) and vapor deposition processes (e.g., chemical vapor deposition, atomic layer deposition, sputtering). While recent advances in in-operando characterization, advanced spectroscopic/microscopic analysis, ultrafast laser diagnostics, and multiscale modeling have significantly improved the understanding of reaction mechanisms in the gas phase, on surfaces, or both, the cooperative coupling effects between gas-phase and surface chemistries, especially at the space- and time-resolved molecular level, remain elusive. This challenge partly arises from the lack of methodologies to independently modulate the energetics and kinetics of gas-phase and surface species. Moreover, many conventional thermochemical reactions and material syntheses occur under near-equilibrium or near-steady-state conditions, offering limited control over timescales, energy levels, and their temporal patterns. This research aims to achieve a deeper understanding of the gas-surface coupling under non-equilibrium conditions through synergistic and spatiotemporal modulation of surface and gas-phase energies and their delivery patterns, thereby unlocking new opportunities for chemical synthesis and material fabrication. In parallel, this project aims to develop an active-learning-guided, high-throughput experimental platform to tailor the large parameter space of dynamic reactions, thus accelerating mechanistic explorations under complex reaction conditions. Overall, this project will provide a novel platform to investigate molecular-scale gas-surface chemical and material transformations within an underexplored non-equilibrium and dynamic regime. In addition, the decoupled control on the surficial and gas-phase energetics and kinetics will help elucidate the critical cooperative gas-surface coupling. The insights will be highly relevant to energy conversion and storage technologies, as well as transformative manufacturing of chemicals and semiconductors.