Collaborative Research: RUI: Instrument Development: Ångström-Scale Operando Spectroscopic Imaging at Heterogeneous Electrochemical Interfaces

在化学系化学测量和成像 (CMI) 项目以及刺激竞争性研究 (EPSCoR) 项目的支持下，休斯敦大学的 Naihao Jiang 和科尔比学院的 Lindsey Madison 正在利用先进的高光谱成像和模拟工具来研究溶液相异质电化学系统。电极表面发生的化学反应由分子混合物组成，这导致原子尺度的成分、电子结构和形态发生变化。为了更好地理解这些复杂的系统，Chiang 博士和他的学生将构建一个定制的电化学尖端增强拉曼光谱 (EC-TERS) 仪器，以通过实验表征电极表面，而 Madison 博士和她的学生将提供补充信息来确定和预测电极表面上的分子结构。蒋和麦迪逊还在开展课外外展活动，以吸引中小学学生的参与。在这个合作项目中，将通过开发电化学尖端增强拉曼光谱（EC-TERS）成像仪器来研究原子水平电化学反应的协同计算和实验研究。将使用从头算分子动力学 (AIMD) 和时间相关密度泛函理论 (TD-DFT) 来预测小分子氧化态对表面结合构型及其非共振拉曼响应的影响。通过仪器的进步提高空间分辨率的能力，将研究 EC 界面处的电势、吸收分子和电解质之间的相互作用。将探索概念验证系统，以指导电池和催化剂等先进电化学应用的未来应用。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 support from the Chemical Measurement and Imaging (CMI) Program in the Division of Chemistry and the Established Program to Stimulate Competitive Research (EPSCoR) Program, Naihao Chiang from the University of Houston and Lindsey Madison from Colby College are studying solution phase heterogeneous electrochemical systems using advances in hyperspectral imaging and simulation tools. Chemical reactions that occur at an electrode surface are composed of a mixture of molecules, which leads to varying atomic scale heterogeneity in composition, electronic structure, and morphology. To better understand these complex systems, Dr. Chiang and his students will construct a custom-built electrochemical tip-enhanced Raman spectroscopy (EC-TERS) instrument to experimentally characterize electrode surfaces while Dr. Madison and her students will provide complementary information to determine and predict molecular structures on the electrode surfaces. Chiang and Madison are also developing after-school outreach activities to engage with students in primary and secondary education.In this collaborative project, synergistic computational and experimental studies of electrochemical reactions at the atomic level will be studied through the development of an electrochemical tip-enhanced Raman spectroscopy (EC-TERS) imaging instrument. Predictions on the effect of small molecule oxidation states on surface binding configurations and their non-resonant Raman response will be made using ab initio molecular dynamics (AIMD) and by time dependent density functional theory (TD-DFT). By improving capabilities in spatial resolution through advances in instrumentation, the interplay between electrical potential, absorbed molecules, and electrolytes at EC interfaces will be studied. Proof-of-concept systems will be explored to guide future applications in advanced electrochemistry applications such as batteries and catalysts.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.