Solvent Reorganization Effects on the Kinetics of Electrochemical Hydrogen Evolution

在化学系化学催化项目的支持下，凯斯西储大学的罗伯特·沃伯顿将开发模拟方法来推动电解科学的发展。电解对各种清洁能源应用至关重要，它提供了一种将水转化为重要商品氢气的电催化途径。这项研究的目标将是确定通过调整电解槽中的界面固体和液体属性来控制和提高氢气产生率的策略。沃伯顿博士将在研究生级别的计算材料建模课程中加入新的体验式学习模块。该团队还将邀请大克利夫兰地区的高中生参加暑期研究实习，以鼓励服务不足的学生获得化学和能源科学方面的高等教育机会。拟议的研究将使用第一原理分子模拟来了解依赖于势的溶剂动力学和能量重组对放氢反应(HER)动力学的影响。通过结合使用显式和隐式电解质模型的从头算分子动力学方法，这些研究将能够在广泛的反应条件(例如，外加电位、pH和离子强度)下详细研究电化学系统中的界面动力学。对被吸附的HER反应中间体的研究，以及旨在改变界面电场和破坏界面氢键的设计分子吸附，将被用来建立控制界面静电、溶剂重组能量学和反应动力学的合成方法。从拟议的研究中获得的见解将激励电催化设计原则，超越对催化剂表面位置的吸附。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, Robert Warburton of Case Western Reserve University will develop simulation methods to advance the science of electrolysis. Electrolysis is critical for various clean energy applications, providing an electrocatalytic route to convert water into hydrogen gas, an important commodity. The goal of the research will be to identify strategies to control and enhance hydrogen production rates by tailoring interfacial solid and liquid properties in electrolyzers. Dr. Warburton will incorporate new experiential learning modules into a graduate-level computational materials modeling course. The team will also engage high school students in the Greater Cleveland area in summer research internships to encourage underserved students toward higher education opportunities in the chemical and energy sciences.The proposed research will use first-principles molecular simulations to understand the effects of potential-dependent solvent dynamics and reorganization energetic on the kinetics of the hydrogen evolution reaction (HER). By incorporating ab initio molecular dynamics methods that utilize both explicit and implicit electrolyte models, these studies will enable detailed study of interfacial dynamics in electrochemical systems over a wide range of reaction conditions (e.g., applied potential, pH, and ionic strength). Investigations of adsorbed HER reaction intermediates, as well as designer molecular adsorbates aimed at modifying interfacial electric fields and disrupting interfacial hydrogen bonds, will be used to establish synthetic approaches to control interfacial electrostatics, solvent reorganization energetics, and reaction kinetics. The insights obtained from the proposed research will motivate electro-catalytic design principles beyond adsorption to catalyst surface sites.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.