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

在化学系化学催化项目的支持下，旧金山州立大学的邱晶晶博士将进行研究，以更好地了解光源如何与特殊制造的电极相结合，增强水分解反应的活性，以生成其组分氢和氧(氧化半反应也称为放氧反应)。这种光电催化反应与许多重要的储能和工业过程有关。邱博士的实验室将利用金纳米颗粒(Au NP)电极收集太阳能，以影响后续的电催化。邱博士将研究在这些反应中发生的电催化剂表面结构的变化。这项研究在科学和社会上都有更广泛的影响。科学上，预计将促进对等离子体介导的电催化的理解，长期目标是开发有望推动清洁能源生产进展的光学材料和技术。在社会上，该项目将为下一代科学家从事可再生能源研究提供有价值的指导和灵感。该项目将为学生，包括来自代表人数不足的群体的学生提供进入劳动力大军或研究生院的技术技能，以及应对与可再生能源生产相关的挑战所需的能力。在化学系化学催化项目的支持下，旧金山州立大学的邱晶晶博士将致力于对等离子体Au NP电极和等离子体介导式析氧反应(OER)中等离子体Au NP电极和电催化剂之间的界面有一个基本的了解，长期目标是开发新的光学方法来精确调节电催化剂的活性。(照片)电化学表征、电化学表面增强拉曼散射(EC-SERS)测量和密度泛函理论(DFT)模拟将被用来以OER为典型的模型反应来解耦表面等离子体在提高电催化剂活性方面的多种效应。该项目涉及以下具体目标：(I)确定与双层氢氧化物电催化剂界面的Au-NP电极的等离子体激发对OER的影响，(Ii)分离Au-Np电极的光热和电子效应(“热”孔)对OER中电催化剂的贡献，(Iii)测量Au-Np电极界面上电催化剂的动态表面形态及其表面化学信息，以及(Iv)计算过渡金属氢氧化物电催化剂在Au金属表面的电子结构。这项工作有可能揭示OER过程中等离子体激发的机理，并为其他类型的电催化氧化反应提供新的见解。更好地了解等离子体效应的机理基础将为新技术的开发提供重要的基础，提高OER过程的效率，这是至关重要的水分裂反应的关键步骤。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

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.