Photocatalysis

In the ever-expanding field of photocatalysis, our group places an emphasis on gaining a thorough understanding of the mechanisms involved in heterogeneous photocatalytic systems at the molecular level. Our approach combines the results of kinetic studies with rigorous in-situ and ex-situ catalyst characterization as well as computational modeling of these systems.

Plasmonic photocatalyst design and implementation

Visible light enhancement
Our lab was one of the first to report and explain the mechanisms behind the use of plasmonic metal nanoparticles (Ag, Au, and Cu) as a driver for photocatalytic enhancement on both semiconductors and directly on plasmonic metals. The unique dielectric properties of plasmonic metal nanoparticles allow them to focus incoming electromagnetic radiation (i.e. light) directly onto the surface of catalyst particles, where chemical transformations occur. By doing so, these catalysts are able to efficiently convert visible light into chemical energy that can be used to drive chemical reactions. Experimentally our group has used plasmonic metal nanoparticles to enhance reaction rates and selectivities for industrially important reactions. We are now working on new catalysts that combine multiple metals to broaden the applications of plasmonic catalysts. We have also coupled plasmonic metals with semiconducters in photoelectrochemical systems to improve the efficiency of processes such as hydrogen evolution.

Mechanistic understanding of photocatalytic systems

Plasmon induced phenomenon
Currently, the complex mechanisms that cause photocatalytic enhancement on plasmonic metal nanoparticle systems are not fully understood. Our group combines experimental characterization studies with computational modeling to gain insight into these mechanisms at the molecular level. Techniques such as in situ UV-visible and Raman spectroscopy allow us to monitor the optical properties of catalysts and how they may change in response to exposure to light or the introduction of reactants. Our group's dedicated computing cluster allows us to perform complex DFT (density functional theory) and FDTD (finite difference time domain) model calculations of the catalyst systems we seek to understand. In combination, these experimental and computational results have continued to shed light on many of the important mechanistic aspects of plasmonic photocatalysts, which in turn leads to better catalyst and reaction system design and implementation.

Selected publications

Elucidating the Roles of Local and Nonlocal Rate Enhancement Mechanisms in Plasmonic Catalysis.

R. Elias, S. Linic, Journal of the American Chemical Society, 2022.
Optimizing Molecular Light Absorption in the Strong Coupling Regime for Solar Energy Harvesting.

S. Chavez, S. Linic, Nano Energy, 2022.
Characterizing the Geometry and Quantifying the Impact of Nanoscopic Electrocatalyst/Semiconductor Interfaces under Solar Water Splitting Conditions.

J.R. Hemmerling, A. Mathur, S. Linic, Advanced Energy Materials, 2022.
Design Principles for Efficient and Stable Water Splitting Photoelectrocatalysts

J.R. Hemmerling, A. Mathur, S. Linic, Accounts of Chemical Research, 2021.
Flow and extraction of energy and charge carriers in hybrid plasmonic nanostructures.

S. Linic, S. Chavez, R. Elias, Nature Materials, 2021.