Bootstrap Embedding for Molecules, Materials and Electrocatalysis

用于分子、材料和电催化的自举嵌入

• 批准号: 2154938
• 负责人: Troy Van Voorhis
• 金额: $ 51万
• 依托单位: Massachusetts Institute of Technology
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-05-01 至 2025-04-30
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2154938&HistoricalAwards=false
• 关键词: Bootstrap; Embedding; Molecules; Materials; Electrocatalysis

Professor Troy Van Voorhis of Massachusetts Institute of Technology is supported by an award from the Chemical Theory, Models and Computational Methods (CTMC) program in the Division of Chemistry to study computational methods for combining calculations on small molecular fragments to make predictions about complex materials. The primary tool is a concept known as Bootstrap embedding, which allows researchers for the first time to divide a large system (say with thousands of atoms) into a number of overlapping fragments (each containing, say, ten atoms) and then stitch together those calculations to understand properties of the whole system. The resulting tools will apply to a wide range of molecules and materials and Van Voorhis will specifically use these tools to study fuel cell catalysts. Computational tools have revolutionized chemistry in recent decades and the work in this proposal will train part of the next generation of computer-savvy chemists. As part of the proposal, Van Voorhis will engage in activities aimed at improving women and under-represented minorities pursuing careers in science. In this project, we will develop new quantum mechanical fragment embedding tools that are specifically designed to be able to accurately treat both complex molecules and solids. The starting point for the work is Bootstrap Embedding (BE), a method that fundamentally solves the issue of embedding overlapping fragments. In this project, we will extend BE by while improving its accuracy and efficiency in treating large basis sets and intermolecular interactions. In a parallel effort, we will implement BE for extended systems (e.g. surfaces and solids) by incorporating periodic boundary conditions. The bootstrap conditions also naturally lead to a new form of boundary conditions (which we call “impurity boundary conditions”) that approximate the situation in which a single substrate reacts at a semi-infinite surface. As a signature application of these tools, we will study the energetics of O2 binding and subsequent proton coupled electron transfer (PCET) steps in a set of potential ORR catalysts. As the ORR half-reaction is the rate- and potential- determining step in all modern fuel cells, advances in this area have the potential for significant impacts in future fuel cell technologies. In a direct sense, the work outlined here will contribute to the training of the undergraduate, graduate and postdoctoral scholars involved in the project. In a wider sense, the project proposes a set of education, training and outreach activities aimed at increasing the participation of women and underrepresented minorities in STEM fields.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.

马萨诸塞州理工学院的Troy货车Voorhis教授获得了化学系化学理论、模型和计算方法（CTMC）项目的奖励，以研究结合小分子片段计算的计算方法，从而对复杂材料进行预测。主要的工具是一个被称为Bootstrap嵌入的概念，它允许研究人员第一次将一个大型系统（例如具有数千个原子）划分为许多重叠的片段（每个片段包含10个原子），然后将这些计算缝合在一起以了解整个系统的属性。由此产生的工具将适用于广泛的分子和材料，货车沃里斯将专门使用这些工具来研究燃料电池催化剂。近几十年来，计算工具已经彻底改变了化学，这项提案中的工作将培养下一代精通计算机的化学家。作为提案的一部分，货车沃里斯将参与旨在改善妇女和代表性不足的少数民族追求科学事业的活动。在这个项目中，我们将开发新的量子力学碎片嵌入工具，这些工具是专门设计的，能够准确地处理复杂的分子和固体。工作的起点是Bootstrap Embedding（BE），这是一种从根本上解决嵌入重叠片段问题的方法。在这个项目中，我们将扩展BE，同时提高其在处理大基组和分子间相互作用方面的准确性和效率。在一个平行的努力，我们将实现BE扩展系统（如表面和固体），通过纳入周期性的边界条件。自举条件也自然地导致一种新形式的边界条件（我们称之为“杂质边界条件”），近似于单个衬底在半无限表面上反应的情况。作为这些工具的签名应用，我们将研究在一组潜在的ORR催化剂的O2结合和随后的质子耦合电子转移（PCET）步骤的能量学。由于ORR半反应是所有现代燃料电池中的速率和潜力决定步骤，因此该领域的进展有可能对未来燃料电池技术产生重大影响。从直接意义上说，这里概述的工作将有助于培训参与该项目的本科生、研究生和博士后学者。从更广泛的意义上说，该项目提出了一系列教育、培训和推广活动，旨在增加妇女和代表性不足的少数群体在STEM领域的参与。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。