Issue 7, 2023

Elucidating the rate-determining step of ammonia decomposition on Ru-based catalysts using ab initio-grounded microkinetic modeling

Abstract

Decarbonizing the current energy system requires a shift toward renewable energy sources, among which ammonia is a remarkable hydrogen carrier. However, developing an efficient process for the catalytic decomposition of ammonia is still required. Here, we propose a combined modeling–experimental approach to elucidate the rate-determining step in ammonia decomposition on Ru-based catalysts. We characterize and test two supported Ru and Ru–K catalysts in the reaction. We develop several microkinetic models based on ab initio calculations considering different rate-determining steps and validate them with the results of packed bed experiments. For the method validation, we develop a fitting strategy based on modifying the lowest number of parameters from those initially obtained theoretically. A good agreement between the simulated and measured experimental ammonia conversions is obtained, thus widening our understanding of this critical hydrogen production process. The approach presented here allows distinguishing the rate-determining step accurately, and it could be applied to other catalytic systems used in ammonia decomposition to avoid over-relying on empirical models.

Graphical abstract: Elucidating the rate-determining step of ammonia decomposition on Ru-based catalysts using ab initio-grounded microkinetic modeling

Supplementary files

Article information

Article type
Paper
Submitted
12 jan 2023
Accepted
07 feb 2023
First published
08 feb 2023
This article is Open Access
Creative Commons BY-NC license

Catal. Sci. Technol., 2023,13, 2026-2037

Elucidating the rate-determining step of ammonia decomposition on Ru-based catalysts using ab initio-grounded microkinetic modeling

S. R. Kulkarni, N. Realpe, A. Yerrayya, V. K. Velisoju, S. Sayas, N. Morlanes, J. Cerillo, S. P. Katikaneni, S. N. Paglieri, B. Solami, J. Gascon and P. Castaño, Catal. Sci. Technol., 2023, 13, 2026 DOI: 10.1039/D3CY00055A

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