Investigation of the kinetics of methanation of a post-coelectrolysis mixture on a Ni/CZP oxide catalyst

IF 7.2 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY Journal of CO2 Utilization Pub Date : 2024-07-01 DOI:10.1016/j.jcou.2024.102864
Audrey Waldvogel , Andrea Fasolini , Francesco Basile , Sebastien Thomas , Anne-Cecile Roger
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Abstract

The use of synthetic natural gas (SNG) as a plug-and-play fuel coming from renewables can help to overcome the limitations given by the intermittency of renewable energy. A way to implement the production of SNG pass through the co-electrolysis of CO2 to a mixture of hydrogen, carbon monoxide and carbon dioxide, steam and small amounts of methane, followed by CO and CO2 methanation. The presence of different reactants and processes requires the comprehension and quantification of the kinetics of the reactions involved with the aim of optimizing methanation. In this work a kinetic model that considers both the direct CO2 methanation and the indirect RWGS + CO methanation pathways has been developed over a Ni(10 %wt)/Ce0.33Zr0.63Pr0.04O2. The kinetic study made it possible to understand the influence of the reactants and products on the reactions through the calculation of reaction rates. This allowed to test, by linearization, the models found in the literature and their adjustment permitted to calculate sixteen kinetic parameters (activation energies, heats of adsorption and pre-exponential factors) present in the rate laws of methanation of CO2, CO and the Reverse Water Gas Shift reaction. The models then made it possible to simulate the evolution of partial flow rates in an isothermal plug flow reactor and were compared to experimental data.

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Ni/CZP 氧化物催化剂上的后电解混合物甲烷化动力学研究
使用合成天然气(SNG)作为可再生能源的即插即用燃料,有助于克服可再生能源间歇性带来的限制。生产合成天然气(SNG)的一种方法是通过二氧化碳共电解生成氢气、一氧化碳和二氧化碳、蒸汽和少量甲烷的混合物,然后进行一氧化碳和二氧化碳甲烷化。由于存在不同的反应物和过程,因此需要了解和量化相关反应的动力学,以优化甲烷化过程。在这项工作中,我们在 Ni(10 %wt)/Ce0.33Zr0.63Pr0.04O2 上建立了一个动力学模型,该模型同时考虑了直接 CO2 甲烷化和 RWGS + CO 间接甲烷化途径。动力学研究通过计算反应速率,了解了反应物和产物对反应的影响。这样就可以通过线性化对文献中的模型进行测试,并对其进行调整,从而计算出二氧化碳、一氧化碳和反向水气变换反应甲烷化速率定律中的 16 个动力学参数(活化能、吸附热和预指数)。这些模型可以模拟等温塞流反应器中部分流速的变化,并与实验数据进行比较。
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来源期刊
Journal of CO2 Utilization
Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.90
自引率
10.40%
发文量
406
审稿时长
2.8 months
期刊介绍: The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.
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