2024 AIChE Annual Meeting

(514a) Increasing Precision in Surface Catalysis By Quantum Monte Carlo

Authors

Bajdich, M., SLAC STANFORD
There is a need for accuracy of the surface adsorption in heterogeneous catalysis on Transition Metals (TM) and Transition Metal Oxides (TMOs)1. The Quantum Monte Carlo method (QMC) can provide a variational estimate of near exact electronic energy of the system. Recent studies2,3 highlight the use of the Quantum Monte Carlo method (QMC), in catalytic scenarios like the CO adsorption puzzle on TM surfaces.

In our work, we utilize QMCPACK4,5 on the NERSC Perlmutter supercomputer to explore the performance of GPU implementation and to affirm the overall method's viability. With the QMC method, we successfully replicated the CO adsorption puzzle on copper (111) surface and newly we confirmed the correct adsorption site for COH, an important step in CO2 reduction processes. We discuss the computational cost and workflow of these calculations. Another aspect of our research evaluates the fundamental precision of Density Functional Theory (DFT) when applied to RuO2 surfaces, a well-known catalytic system for oxygen evolution reaction (OER). Leveraging these insights, we delve into the potential of applying QMC techniques to broader aspects of heterogeneous catalysis and electrochemistry, highlighting QMC's broad applicability in calculating surface adsorption, formation, and reaction energies.

1. Comer, B.M., J. Li, F. Abild-Pedersen, M. Bajdich, and K.T. Winther, The Journal of Physical Chemistry C, 126 (18), pp. 7903–7909 (2022).
2. Hsing, C.-R., C.-M. Chang, C. Cheng, and C.-M. Wei, The Journal of Physical Chemistry C, 123 (25), pp. 15659–15664 (2019).
3. Iyer, G.R., and B.M. Rubenstein, The Journal of Physical Chemistry A, 126 (28), pp. 4636–4646 (2022).
4. Kim, J., A.D. Baczewski, T.D. Beaudet, et al., Journal of Physics: Condensed Matter, 30 (19), p. 195901 (2018).
5. Kent, P.R.C., A. Annaberdiyev, A. Benali, et al., The Journal of Chemical Physics, 152 (17), (2020).