Massively-parallel Electronic Structure Calculations for Energy Applications

据估计，全球对能源的需求在未来20年将翻一番，因此研究革命性的能源技术以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，作为燃料的氢需要高效的存储材料来保留和释放所需的大量氢。这项提议旨在对一类重要的多孔性储氢材料：金属有机骨架(MOF)进行大规模和准确的量子力学计算。研究小组将研究MOF中氢的性质，并试图了解它们的物理性质，以及如何设计改进的MOF，以便在合理和真实的操作条件下提高单位重量的氢存储。要了解和改进MOF的储氢应用，关键是研究MOF的微观物理性质，这些性质支配着MOF中氢的吸收、释放和扩散。这就需要在原子尺度上模拟MOF内部的氢气。该项目建议使用第一性原理密度泛函理论对MOF内部的氢动力进行高精度的量子力学模拟，以描述包括量子核效应在内的核自由度的分子动力学系统的电子态(通过路径积分形式)。原子核自由度的量子涨落对理解氢等轻元素的束缚和动力学至关重要。该项目将使用这个先进而准确的理论框架来解决这一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)过渡金属原子如何改变MOF结构中的氢键和动力学性质，以及哪些金属最适合实际应用？(3)MOF框架的灵活性和随温度变化的波动如何影响氢存储？这项研究的科学成果将对研究MOF和氢存储的研究人员产生兴趣和重要意义。其目的是提供有用的理解和信息，以帮助创造有助于创造氢经济的材料。这项工作的成果将发表在高质量的期刊上，在国际会议上广泛发表，并成为面向更广泛公众的外联活动的基础，以提高人们对科学和技术的普遍兴趣，以及模拟和计算如何解决重要的现实世界问题。开展研究工作的初级研究人员将接受使用先进计算方法、随之而来的软件基础设施和材料设计方法的培训，这些都是在21世纪非常有用的技能。

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.