Collaborative Research: U.S.-Ireland R&D Partnership: Full Atomistic Understanding of Solid-Liquid Interfaces via an Integrated Experiment-Theory Approach

可再生能源的全球部署需要高效的电化学系统，如电池、超级电容器和燃料电池。在大多数这些系统中，能量转换和存储过程关键地依赖于固体电极和液体电解质之间的界面。然而，这些带电界面的基本原子和分子结构仍然难以捉摸。该项目的目标是实现对电极-电解质界面的结构和反应动力学的原子理解，并为各种低成本碳基电化学系统提供设计原则。通过与都柏林大学学院和阿尔斯特大学的国际合作，PI将开发一种综合实验成像-原子模拟方法。该项目的技术成果将促进高效电化学能量转换和存储系统的设计和工程。该项目的教育工作将建立并将电化学电池和材料成像平台的演示设备纳入国内和国际的一系列教育和推广活动中。该项目将培养研究生和本科生的实验和模拟方法的技能，并为他们提供国际合作研究的经验。该项目将有助于教育公众了解可再生能源转换和储存的基本机制，其目的是通过确定电极-电解质界面的3D结构，包括固体电极表面和液体溶剂化层，实现对电化学过程的彻底原子理解。该项目的方法将分子动力学和密度泛函理论模拟与3D原子分辨率力显微镜实验相结合，以实现精确理解和预测电化学界面的联合实验-理论平台。该平台将用于解开负责碳基超级电容器中能量存储的溶剂化层结构，以及单原子催化剂上电催化反应的溶剂化原子动力学。该项目将产生考虑固有的原子尺度不均匀性的固液界面的基本模型。此外，原子界面结构和单原子催化剂的催化活性的彻底测定将揭示非均匀结构的催化剂的非常规标度关系。这将是一个重要的一步，更具有预测性，分子水平的理论超越了广泛接受的“萨巴捷原则”的多相催化和电催化。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

The worldwide deployment of renewable energy requires efficient electrochemical systems, such as batteries, supercapacitors, and fuel cells. In most of these systems, the energy conversion and storage processes rely crucially on the interface between solid electrodes and liquid electrolytes. However, the fundamental atomic and molecular structure at these electrified interfaces remains elusive. The goal of the project is to achieve an atomistic understanding of the structure and reaction dynamics of electrode-electrolyte interfaces, and provide design principles for various low-cost, carbon-based electrochemical systems. Through international collaborations with the University College Dublin and Ulster University, the PIs will develop an integrated experimental imaging - atomistic simulation method. The technical outcomes of the project will facilitate the design and engineering of efficient electrochemical energy conversion and storage systems. The educational efforts of the project will build and incorporate demo devices of electrochemical cells and materials imaging platforms into a series of education and outreach activities both domestically and internationally. The project will train the graduate and undergraduate students with skills in both experimental and simulation methods and provide them with an international collaborative research experience. The project will contribute to efforts to educate the public on the basic mechanisms of renewable energy conversion and storage.The project’s aim is to achieve a thorough atomistic understanding of electrochemical processes by determining the 3D structure of electrode-electrolyte interfaces, including both the surface of the solid electrodes and the liquid solvation layers. The project’s approach will integrate molecular dynamics and density functional theory simulations with 3D atomic-resolution force microscopy experiments to achieve a joint experiment-theory platform for precise understanding and prediction of electrochemical interfaces. The platform will be used to unravel the solvation layer structure that is responsible for energy storage in carbon-based supercapacitors, and the solvent-included atomistic kinetics of electrocatalytic reactions on single-atom catalysts. The project will produce fundamental models of solid-liquid interfaces that consider the inherent atomic-scale heterogeneities. Furthermore, the thorough determination of the atomistic interfacial structure and catalytic activities of single-atom catalysts will shed light on the unconventional scaling relationships of catalysts with nonuniform structures. This will be an important step towards a more predictive, molecular-level theory beyond the widely accepted "Sabatier Principle" for heterogeneous catalysis and electrocatalysis. The results will significantly foster the design and engineering of electrochemical interfaces for low-cost, highly efficient renewable energy applications.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.