Abstract CO2 methanation is a novel way for climate change mitigation by converting CO2 into substitute natural gas. In this study, a highly active fibrous silica-beta zeolite (FS@SiO2-BEA) catalyst was prepared for CO2 methanation by a microemulsion process, and examined by N2 adsorption–desorption, field emission scanning electron microscope (FESEM), transmission electron microscopy (TEM), and electron spin resonance (ESR) spectroscopy techniques. It was found that the FS@SiO2-BEA catalyst possessed a fibrous silica morphology, leading to high surface area (609 m2/g), oxygen vacancies, and basicity. A thermodynamic study was also carried out using Gibbs free energy minimization method, and it was found that low temperatures (25–350 °C) and high H2: CO2 ≥ 4 ratios have enhanced the CO2 methanation activity. The prepared FS@SiO2-BEA catalyst exhibited high CO2 conversion (65%), and CH4 selectivity (61%) with a space–time yield of 3.30 g gcat−1 h−1. The obtained experimental results highly followed the thermodynamic calculations.

中文翻译：

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创新形态的高活性无金属纤维二氧化硅-β沸石（FS@SiO2-BEA）上CO2甲烷化的热力学和实验探索

摘要 CO2 甲烷化是一种通过将 CO2 转化为替代天然气来缓解气候变化的新方法。在这项研究中，通过微乳液工艺制备了一种用于 CO2 甲烷化的高活性纤维状二氧化硅-β 沸石（FS@SiO2-BEA）催化剂，并通过 N2 吸附-解吸、场发射扫描电子显微镜（FESEM）、透射电子显微镜进行了检测。 (TEM) 和电子自旋共振 (ESR) 光谱技术。发现 FS@SiO2-BEA 催化剂具有纤维状二氧化硅形态，导致高表面积（609 m2/g）、氧空位和碱性。还使用吉布斯自由能最小化方法进行了热力学研究，发现低温（25-350°C）和高 H2:CO2 ≥ 4 比率增强了 CO2 甲烷化活性。制备的 FS@SiO2-BEA 催化剂表现出高 CO2 转化率（65%）和 CH4 选择性（61%），时空产率为 3.30 g gcat-1 h-1。获得的实验结果高度符合热力学计算。