Massively-parallel Electronic Structure Calculations for Energy Applications

能源应用的大规模并行电子结构计算

• 批准号: 1614491
• 负责人: Sohrab Ismail-Beigi
• 金额: $ 1.4万
• 依托单位: Yale University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-05-01 至 2018-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1614491&HistoricalAwards=false
• 关键词: Massively; parallel; Electronic; Structure; Calculations

It has been estimated that the entire world-wide demand for energy will double in the nexttwo decades, therefore it is critical to investigate revolutionary energy technologiesto meet this demand. A potential hydrogen economy is a key player in this marketspace. However, hydrogen as a fuel requires efficient storage materials that retain and releasea great deal of hydrogen as desired. This proposal aims to use large scale and accurate quantummechanical calculations on an important class of porous hydrogen storage materials: metal-organicframeworks (MOFs). The research team will study the properties of hydrogen inside of MOFsand seek to understand their physical properties and how one can design improved MOFs thatshould deliver improved storage of hydrogen per unit weight under reasonable and real-worldoperating conditions.To understand and improve MOFs for hydrogen storage applications, it is key to study the microscopicphysical properties of MOFs that govern hydrogen uptake, release, and diffusioninside the MOFs. This requires simulation of hydrogen inside of MOFs at the atomistic scale.The project propose to perform highly accurate quantum mechanical simulations of hydrogen dynamicsinside of MOFs using first principles density functional theory to describe the electronicstate of the system coupled to molecular dynamics of the nuclear degrees of freedom includingquantum nuclear effects (via the path integral formalism). The effect due to the quantumfluctuations of the nuclear degrees of freedom are critical for understanding the bindingand dynamics of light elements such as hydrogen. The project will use this advanced and accurate theoreticalframework to address three questions of key importance to this field: (1) How do quantumnuclear effects alter hydrogen dynamics inside of MOFs? (2) How do the transition metal atomsincorporated into the MOF structure change the hydrogen binding and dynamics properties andwhich metals are best for real-world applications? (3) How does the flexibility and temperature-dependentfluctuations of the MOF framework affect hydrogen storage?The scientific outcomes of this research will be of interest and importance to researchersstudying MOFs and hydrogen storage. The aim is to provide useful understanding and informationthat may lead to the creation of materials that will help create a hydrogen economy. Theresults of the work will be published in high quality journals, presented widely at internationalconferences, and form the basis for outreach events to the broader public in order to elevategeneral interest in science and technology as well as how simulations and computations canaddress important real-world problems. Junior researchers carrying out the research workwill be trained in the use of advanced computational methods, attendant software infrastructures,and materials design approaches that are all highly useful skills in the twenty-first century.

据估计，未来二十年全球能源需求将翻一番，因此研究革命性的能源技术来满足这一需求至关重要。潜在的氢经济是这个市场空间的关键参与者。然而，氢作为燃料需要有效的存储材料，以根据需要保留和释放大量氢。该提案旨在对一类重要的多孔储氢材料：金属有机框架（MOF）进行大规模且精确的量子力学计算。研究小组将研究 MOF 内部氢的特性，并寻求了解它们的物理特性，以及如何设计改进的 MOF，从而在合理和真实的操作条件下提高每单位重量的氢存储量。了解和改进用于氢存储的 MOF在应用中，研究 MOF 的微观物理特性是控制氢在 MOF 内部吸收、释放和扩散的关键。这需要在原子尺度上模拟 MOF 内部的氢。该项目建议使用第一原理密度泛函理论对 MOF 内部的氢动力学进行高精度量子力学模拟，以描述系统的电子态与核度的分子动力学耦合。自由，包括量子核效应（通过路径积分形式主义）。核自由度的量子涨落造成的效应对于理解氢等轻元素的结合和动力学至关重要。该项目将利用这一先进而准确的理论框架来解决该领域的三个关键问题：（1）量子核效应如何改变MOF内部的氢动力学？ (2) 纳入 MOF 结构的过渡金属原子如何改变氢键和动力学特性以及哪些金属最适合实际应用？ (3) MOF框架的灵活性和温度依赖性波动如何影响储氢？这项研究的科学成果将对研究MOF和储氢的研究人员产生兴趣和重要性。目的是提供有用的理解和信息，可能有助于创造有助于创造氢经济的材料。这项工作的结果将发表在高质量期刊上，在国际会议上广泛展示，并构成向更广泛公众宣传活动的基础，以提高人们对科学技术以及模拟和计算如何解决重要的现实问题的普遍兴趣。开展研究工作的初级研究人员将接受先进计算方法、附带软件基础设施和材料设计方法的使用培训，这些都是二十一世纪非常有用的技能。