期刊
CATALYSIS SCIENCE & TECHNOLOGY
卷 13, 期 7, 页码 2026-2037出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d3cy00055a
关键词
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This study proposes a combined modeling-experimental approach to elucidate the rate-determining step in ammonia decomposition on Ru-based catalysts. The authors characterize and test two supported Ru and Ru-K catalysts and develop microkinetic models based on ab initio calculations. The approach accurately distinguishes the rate-determining step and contributes to the understanding of the critical hydrogen production process.
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.
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