MOF-derived carbon-based catalysts with enhanced anti-coking property for the dry reforming of methane

Zizhao Chen , Shuai Yan , Guang Yang , Qiang Hu , Yingquan Chen , Hanping Chen , Yonggang Yao , Haiping Yang
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Abstract

To avoid sintering and carbon deposition of conventionally loaded catalysts, a spatial confinement strategy was employed to design a high-performance catalyst for the dry reforming of methane (DRM) reaction. With tri-metallic Ni-Co-Mg metal-organic framework (MOF-74) as a precursor, a novel nanostructured NiCoMg@C catalyst was synthesized, where the active metals Ni and Co were confined within the carbon framework derived from MOF pyrolysis. Characterization results indicate that the catalyst synthesized with MOF as template has a high specific surface area, well-dispersed metals, and strong metal-support interactions. The introduction of a high content of Mg promoted the dispersion of active metal Ni and Co and increased the number and strength of surface basic sites. Among the catalysts, NiCoMg20@C exhibited optimal catalytic activity, with initial CH4 and CO2 conversion rates reaching 75.13 % and 85.29 %, respectively. More importantly, the catalyst showed high stability during 100 h DRM reaction at 700 °C without significant carbon deposition. This research provides a new perspective for the development of DRM catalysts.

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用于甲烷干重整的具有更强防焦性能的 MOF 衍生碳基催化剂
为了避免传统负载催化剂的烧结和碳沉积,我们采用了空间限制策略来设计一种用于甲烷干重整(DRM)反应的高性能催化剂。以三金属镍-钴-镁金属有机框架(MOF-74)为前驱体,合成了一种新型纳米结构的镍钴镁@C 催化剂,其中活性金属镍和钴被限制在 MOF 热解产生的碳框架内。表征结果表明,以 MOF 为模板合成的催化剂具有较高的比表面积,金属分散良好,金属与支撑物之间的相互作用较强。高含量镁的引入促进了活性金属 Ni 和 Co 的分散,增加了表面碱性位点的数量和强度。在这些催化剂中,NiCoMg20@C 表现出最佳的催化活性,CH4 和 CO2 的初始转化率分别达到 75.13% 和 85.29%。更重要的是,该催化剂在 700 °C 下进行 100 h DRM 反应时表现出很高的稳定性,没有明显的碳沉积。这项研究为 DRM 催化剂的开发提供了一个新的视角。
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