Massively-parallel Electronic Structure Calculations for Energy Applications

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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.