Massively-parallel Electronic Structure Calculations for Energy Applications

Sohrab Ismail-Beigi, Yale University

Usage Details

Sohrab Ismail-Beigi, Eric Bohm, Minjung Kim, Nikhil Jain, Michael Robson, Eric Mikida, Qi Li, Subhasish Mandal, Juan Galvez, Kavitha Chandrasekar, Tobias Wicky, Monika Gangapuram, Nihar Sheth, Samarth Kulshreshtha, Abhishek Srivastava, Shaoqin Lu, Raghavendra Kanakagiri, Dong Hun Lee, Karthik Sudana

It has been estimated that the entire world-wide demand for energy will double in the next two decades, therefore it is critical to investigate revolutionary energy technologies to meet this demand. A potential hydrogen economy is a key player in this market space. However, hydrogen as a fuel requires efficient storage materials that retain and release a great deal of hydrogen as desired. This proposal aims to use large scale and accurate quantum mechanical calculations on an important class of porous hydrogen storage materials: metal-organic frameworks (MOFs). The research team will study the properties of hydrogen inside of MOFs and seek to understand their physical properties and how one can design improved MOFs that should deliver improved storage of hydrogen per unit weight under reasonable and real-world operating conditions.

To understand and improve MOFs for hydrogen storage applications, it is key to study the microscopic physical properties of MOFs that govern hydrogen uptake, release, and diffusion inside 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 dynamics inside of MOFs using first principles density functional theory to describe the electronic state of the system coupled to molecular dynamics of the nuclear degrees of freedom including quantum nuclear effects (via the path integral formalism). The effect due to the quantum fluctuations of the nuclear degrees of freedom are critical for understanding the binding and dynamics of light elements such as hydrogen. The project will use this advanced and accurate theoretical framework to address three questions of key importance to this field: (1) How do quantum nuclear effects alter hydrogen dynamics inside of MOFs? (2) How do the transition metal atoms incorporated into the MOF structure change the hydrogen binding and dynamics properties and which metals are best for real-world applications? (3) How does the flexibility and temperature-dependent fluctuations of the MOF framework affect hydrogen storage?

The scientific outcomes of this research will be of interest and importance to researchers studying MOFs and hydrogen storage. The aim is to provide useful understanding and information that may lead to the creation of materials that will help create a hydrogen economy. The results of the work will be published in high quality journals, presented widely at international conferences, and form the basis for outreach events to the broader public in order to elevate general interest in science and technology as well as how simulations and computations can address important real-world problems. Junior researchers carrying out the research work will 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.