Thermodynamics and Kinetics of Plasmonic Carrier Harvesting
Prashant Jain a
a University of Illinois Urbana-Champaign, West Green Street, 1304, Urbana, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Fall 2024 Conference (MATSUSFall24)
#ChiNano - Exploring Chiral Nanostructured Materials and Plasmonics for Energy applications
Lausanne, Switzerland, 2024 November 12th - 15th
Organizers: Sascha Feldmann, Magalí Lingenfelder and Giulia Tagliabue
Invited Speaker, Prashant Jain, presentation 039
DOI: https://doi.org/10.29363/nanoge.matsusfall.2024.039
Publication date: 28th August 2024

The visible-light excitation of plasmonic nanostructures is now well known to induce catalytic reactions that are not otherwise observed in the dark. I will describe how catalysts based on plasmonic nanoparticles are allowing light to be used as a redox equivalent in chemical reactions, for driving non-equilibrium chemical processes, for modifying product selectivity, for photosynthesizing fuels, and for boosting electrochemical conversions. One prime example discovered in my group is the conversion of carbon dioxide to hydrocarbons on gold nanoparticles driven by electron–hole pairs generated by plasmonic excitation. This photochemistry constitutes much more than photoenhanced catalysis: rather chemical potential is harvested from plasmonic excitations and stored in the form of energy-rich bonds. The chemical potential is a linear function of the concentration of light, as I will show using a simple model and experimental findings from a diverse set of reactions. However, conversions driven by plasmonically generated carriers can suffer from thermodynamic and efficiency limits. I will describe how such limits can be overcome.

This material is based on work supported by the National Science Foundation under Grant No. CHE-2304910.

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