Elucidating the rate-determining step of ammonia decomposition on Ru-based catalysts using ab initio-grounded microkinetic modeling,Catalysis Science & Technology

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Elucidating the rate-determining step of ammonia decomposition on Ru-based catalysts using ab initio-grounded microkinetic modeling
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2023-02-08 , DOI: 10.1039/d3cy00055a
Shekhar R. Kulkarni ₁ , Natalia Realpe ₁ , Attada Yerrayya ₁ , Vijay Kumar Velisoju ₁ , Salvador Sayas ₁ , Natalia Morlanes ₁ , Jose Cerillo ₁ , Sai P. Katikaneni ₂ , Stephen N. Paglieri ₂ , Bandar Solami ₂ , Jorge Gascon ₁ , Pedro Castaño ₁

Affiliation

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.

中文翻译：

使用从头算的微观动力学模型阐明 Ru 基催化剂上氨分解的决速步骤

使当前的能源系统脱碳需要转向可再生能源，其中氨是一种出色的氢载体。然而，仍然需要开发一种有效的氨催化分解工艺。在这里，我们提出了一种组合的建模-实验方法来阐明 Ru 基催化剂上氨分解的决速步骤。我们在反应中表征并测试了两种负载型 Ru 和 Ru-K 催化剂。我们开发了几种基于从头算的微观动力学模型考虑不同的速率决定步骤的计算，并用填充床实验的结果验证它们。对于方法验证，我们开发了一种拟合策略，该策略基于从理论上最初获得的参数中修改最少数量的参数。在模拟和测量的实验氨转化率之间获得了很好的一致性，从而拓宽了我们对这一关键制氢过程的理解。这里介绍的方法可以准确地区分决速步骤，并且可以应用于氨分解中使用的其他催化系统，以避免过度依赖经验模型。

更新日期：2023-02-08

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