RUI: Mechanistic Understanding of the Electrode-catalyst Interface in Plasmon-mediated Oxygen Evolution Reaction

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With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Jingjing Qiu of San Francisco State University will conduct studies to better understand how light sources can, in combination with specially fabricated electrodes, enhance the activity of the water-splitting reaction to generate its components hydrogen and oxygen (the oxidation half-reaction is also known as the oxygen evolving reaction). Such photo-electrocatalytic reactions are of relevance to many important energy-storage and industry processes. Dr. Qiu’s laboratory will utilize gold nanoparticle (Au NP) electrodes to harvest solar energy to influence the subsequent electrocatalysis. Dr. Qiu will probe changes at the electrocatalyst surface structure that occur during these reactions. This research has broader impact both scientifically and societally. Scientifically, it is expected to advance the understanding of plasmon-mediated electrocatalysis with the long-term goal to develop optical materials and technologies that are expected to drive forward the progress for clean energy production. Societally, this project will provide valuable instruction and inspiration for the next generation of scientists to pursue renewable energy research. The project will provide students, including those from underrepresented groups, with technical skills to enter the workforce or graduate school with the competencies that are required to address the challenges associated with renewable energy production. Dr. Qiu and her students will also develop short videos on electrochemistry topics in Spanish to help disseminate research in this area to a broader audience.With the support of the Chemical Catalysis program in the Division of Chemistry, Dr. Jingjing Qiu of San Francisco State University will work to develop a fundamental understanding of the interface between plasmonic Au NP electrodes and electrocatalysts in the plasmon-mediated oxygen-evolving reaction (OER) with the long-term goal of developing new optical methods to precisely tune the activity of electrocatalysts. (Photo)electrochemical characterization, in operando electrochemical surface enhanced Raman scattering (EC-SERS) measurements and density functional theory (DFT) simulations will be applied to decouple the multi-effects of surface plasmons in enhancing the activity of electrocatalysts using the OER as a representative model reaction. The project involves the following specific objectives: (i) to determine the impact of plasmon excitation of Au NP electrodes interfaced with double layer hydroxide electrocatalysts on the OER, (ii) to decouple the contributions of the photothermal and electronic effects (“hot” holes) of Au NP electrodes on electrocatalysts in the OER, (iii) to measure the dynamic surface morphology of the electrocatalysts at the Au NP electrode interface and their surface chemical information, and (iv) to compute the electronic structures of the transition metal hydroxide electrocatalysts at the Au metal surfaces. This work has the potential to shed light on the mechanisms of plasmon excitation in the OER process and to provide new insights for other types of electrocatalytic oxidation reactions. A better understanding of the mechanistic basis for plasmonic effects would provide an important foundation for the development of new technologies increase the efficiency of the OER process, a key step in the all-important water-splitting reaction.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.