Solid-State Redox Kinetics of CeO2 in Two-Step Solar CH4 Partial Oxidation and Thermochemical CO2 Conversion

氧化还原 热化学循环 氧化剂 化学工程 化学 成核 热力学 材料科学 化学链燃烧 催化作用 无机化学 物理化学 制氢 有机化学 燃烧 工程类 物理
作者
Mahesh Muraleedharan Nair,Stéphane Abanades
出处
期刊:Catalysts [Multidisciplinary Digital Publishing Institute]
卷期号:11 (6): 723-723 被引量:8
标识
DOI:10.3390/catal11060723
摘要

The CeO2/CeO2−δ redox system occupies a unique position as an oxygen carrier in chemical looping processes for producing solar fuels, using concentrated solar energy. The two-step thermochemical ceria-based cycle for the production of synthesis gas from methane and solar energy, followed by CO2 splitting, was considered in this work. This topic concerns one of the emerging and most promising processes for the recycling and valorization of anthropogenic greenhouse gas emissions. The development of redox-active catalysts with enhanced efficiency for solar thermochemical fuel production and CO2 conversion is a highly demanding and challenging topic. The determination of redox reaction kinetics is crucial for process design and optimization. In this study, the solid-state redox kinetics of CeO2 in the two-step process with CH4 as the reducing agent and CO2 as the oxidizing agent was investigated in an original prototype solar thermogravimetric reactor equipped with a parabolic dish solar concentrator. In particular, the ceria reduction and re-oxidation reactions were carried out under isothermal conditions. Several solid-state kinetic models based on reaction order, nucleation, shrinking core, and diffusion were utilized for deducing the reaction mechanisms. It was observed that both ceria reduction with CH4 and re-oxidation with CO2 were best represented by a 2D nucleation and nuclei growth model under the applied conditions. The kinetic models exhibiting the best agreement with the experimental reaction data were used to estimate the kinetic parameters. The values of apparent activation energies (~80 kJ·mol−1 for reduction and ~10 kJ·mol−1 for re-oxidation) and pre-exponential factors (~2–9 s−1 for reduction and ~123–253 s−1 for re-oxidation) were obtained from the Arrhenius plots.

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