Collaborative Research: Multiscale atomistic modeling tools for electrocatalytic systems

合作研究：电催化系统的多尺度原子建模工具

• 批准号: 1263951
• 负责人: Michael Janik
• 金额: $ 22.65万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-09-01 至 2016-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1263951&HistoricalAwards=false
• 关键词: Collaborative; Research; Multiscale; atomistic; modeling

ABSTRACTCollaborative Proposals #1264104 - Susan B. Sinnott #1263951 - Michael J. Janik Scientific Merit: As traditional fossil fuel sources of energy are depleted, new energy conversion and chemical energy storage approaches will be needed to supply energy for both portable and stationary applications. Fuel cells offer efficient conversion of chemical to electrical energy. Electrolysis applications reverse this process and store electricity from renewable sources, such as the wind or sun, in chemical form for later use. The efficiency of converting energy between chemical and electrical forms is dictated by atomistic processes that occur at device electrodes. These processes are difficult to probe with conventional experiments. The characterization of these processes is enabled using atomic and quantum level computational methods. There are two major limitations in current modeling approaches for evaluating reactivity of electrode surfaces: the inability to estimate rates for electron transfer reactions and the lack of atomistic force fields that can describe chemical reactions and charge transfer, yet retain the thickness required to capture relevant interfacial phenomena. Professors Michael Janik and Janna Maranas of Pennsylvania State University and Susan Sinnott of the University of Florida have received an award from the National Science Foundation Catalysis & Biocatalysis Program to tackle these limitations. The first limitation will be addressed through the development of a transferable method for electron transfer rate constants using methods based on quantum mechanics. This method will be applied and validated versus experimental data for the carbon dioxide reduction reaction (of relevance for converting electrical energy and waste carbon dioxide into a chemical fuel) and the oxygen reduction reaction (of relevance in fuel cells). The method will be further applied, in collaboration with experiment, to evaluate the reaction mechanism in the electrocatalytic synthesis of high value chemicals from bio-derived feedstock. The second limitation will be addressed through a reactive molecular force field with variable partial charges for both electrode and solvent. Charge optimized many-body reactive potentials will be developed for copper and platinum electrodes in contact with alkali hydroxide electrolytes. Molecular dynamics calculations will evaluate electrochemical interface, including solvent structure and charge distribution. These multiscale atomistic modeling tools enable definitive identification of electrochemical reaction mechanisms. They will be applied to three specific electrocatalytic applications to evaluate a series of reaction specific hypotheses. Broader Impacts: The broader impacts of this work secure a clean energy future in which renewable energy and chemical energy storage work together to provide an efficient, practical approach to sustainable energy. This project develops a joint quantum chemistry and reactive molecular dynamics framework to model electrochemical interfaces, facilitating rational design of materials for improved batteries, fuel cells, and grid-level electrochemical energy storage. With this in mind, educational activities are designed to motivate students to pursue careers in energy related fields. Graduate students will benefit from an inter-disciplinary research project at two universities, and become skilled in multiple computer simulation methods. Portions of the proposed work will be packaged as undergraduate projects at both Penn State and the University of Florida, including underrepresented groups through the Penn State Minority Undergraduate Research Experience and Women in Science and Engineering Research programs. Research opportunities will be provided to high school students through the U. of Florida. The developed computer simulation methods will be broadly distributed to the computational community, allowing others to apply the techniques developed to electrochemical problems outside the scope of this proposal.

摘要企业提案＃1264104 -Susan B. Sinnott＃1263951 -Michael J. Janik Scientific Feerit：由于传统的化石燃料能源被耗尽，因此将需要新的能源转换和化学能源存储方法来为便携式和固定应用提供能源。 燃料电池可有效地转化化学能源为电能。 电解应用逆转了此过程，并以化学形式从可再生能源（例如风或太阳）中存储电力，以供以后使用。 化学和电形式之间能量转化的效率取决于设备电极处发生的原子过程。这些过程很难通过常规实验进行探测。这些过程的表征是使用原子和量子级计算方法启用的。当前建模方法评估电极表面的反应性有两个主要局限性：无法估计电子转移反应的速率以及缺乏可以描述化学反应和电荷转移的原子力场，但保留了捕获相关界面​​现象所需的厚度。宾夕法尼亚州立大学的迈克尔·贾尼克（Michael Janik）和詹娜·马拉纳斯（Janna Maranas）和佛罗里达大学的苏珊·辛诺特（Susan Sinnott）获得了国家科学基金会催化与生物催化计划的奖励，以应对这些限制。第一个限制将通过使用基于量子力学的方法开发电子传输速率常数的可转移方法来解决。 该方法将用于二氧化碳还原反应（将电能和废物二氧化碳转换为化学燃料的相关性）和氧还原反应（燃料电池中的相关性）。 该方法将与实验合作进一步应用，以评估来自生物衍生原料的高价值化学物质的电催化合成中的反应机理。 第二个限制将通过反应性分子力场来解决，并具有可变的部分电荷的电极和溶剂。 电荷优化的多体反应电位将用于与碱氢氧化物电解质接触的铜和铂电极。 分子动力学计算将评估电化学界面，包括溶剂结构和电荷分布。 这些多尺度原子建模工具可实现电化学反应机制的明确识别。它们将应用于三个特定的电催化应用，以评估一系列反应特定的假设。更广泛的影响：这项工作的更广泛的影响确保了清洁能源的未来，可再生能源和化学能源储存共同提供了一种可持续能源的有效，实用的方法。该项目开发了一个联合量子化学和反应性分子动力学框架，以建模电化学接口，促进改进电池，燃料电池和网格级电化学能源存储的材料的合理设计。 考虑到这一点，教育活动旨在激励学生从事与能源有关的领域的职业。 研究生将从两所大学的跨学科研究项目中受益，并熟练使用多种计算机模拟方法。 拟议工作的一部分将在宾夕法尼亚州立大学和佛罗里达大学作为本科项目，包括通过宾夕法尼亚州少数群体本科生研究经验以及科学与工程研究计划中的妇女的代表性群体。 通过佛罗里达大学，将向高中生提供研究机会。 开发的计算机仿真方法将广泛分发给计算界，使其他人能够将开发的技术应用于本提案范围之外的电化学问题。