Hydrogen by being light and energy-dense is a strategic green fuel and industrial chemical, however, majority of it (≥95 %) is produced via very energy intense steam reforming of fossil fuels at high-temperatures of 700°C – 1000°C and in presence of mostly Ni-based catalysts. Efficient “one-pot” carbon capture, separation, and catalytic transformation of light hydrocarbons via catalytic C-H activation processes has therefore the potential to reduce overall energy costs for production of not only H2 but also other valuable chemicals. Here, we have studied hydrogen production from dehydrogenation of the shale gas using single-atom and single-atom alloyed heterogeneous catalysts (SACs and SAACs) deposited on different metal-organic frameworks (MOFs). MOFs are ideal platforms as supports for these catalytic reactions by providing tunable 3D voids and preventing catalyst deactivation via agglomeration and sintering. To expedite catalyst “design and discovery” and reduce the computational burden of exploring configurational space of all possible active site motifs in presence of water, we have exploited a workflow comprised of empirical potentials in conjunction with global optimization techniques for locating the global minima as well as ensemble of all thermodynamically accessible low-energy meta-stable isomers within a certain energy window. Combining these theoretical schemes have enabled us to efficiently model complex chemical spaces of these materials orders of magnitude faster than the conventionally employed methods such as Density Functional Theory (DFT). Using this methodology, we have studied catalytic dehydrogenation of propane and butane, taken here as a representative of the light hydrocarbons present in the shale gas, to H2 as well as propene and butene. Results obtained from this project are used to answer the most immediate open questions including (i) the precise nature of the active sites including changes in coordination environment during the catalytic process and (ii) effects of structural defects including linker and node vacancies on the catalytic process in gas and aqueous phases. In addition to improve the kinetics and thermodynamics of the catalyst for producing hydrogen, results from this project are used to tune the catalyst for selectively producing linear alpha-olefins with a plethora of industrial applications.

Computer aided heterogeneous catalyst design and discovery of single-atom and single-atom alloyed transition metal catalysts deposited on metal-organic frameworks with applications in hydrogen production from the shale gas

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.