源自 Ce 基 MOF 的 Ru/CeO2 催化剂用于高效催化 CO2 甲烷化与可再生氢的结合

IF 7.2 2区工程技术 Q1 CHEMISTRY, APPLIED Fuel Processing Technology Pub Date : 2024-06-20 DOI:10.1016/j.fuproc.2024.108101

Yucan He, Dongsen Mao, Qiangsheng Guo, Jun Yu

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引用次数: 0

摘要

研究人员合成了一系列高度有序的微孔 Ce 基金属有机框架 (MOF)，作为构建催化剂的前体。通过热解 Ce-MOF 得到的 CeO2 上的 Ru 浸渍制备了相应的 Ru 催化剂，并研究了通过 CO2 加氢合成 CH4 的过程。在这些催化剂中，以 Ce-BDC 衍生的 CeO2-B 为载体的 Ru 催化剂对 CO2 甲烷化具有很高的竞争效率，在 275 °C 和 0.1 MPa 条件下，CH4 选择性为 100%，CO2 转化率为 62%，CH4 产率达到 0.49 mol/(molRu-h)。表征结果表明，Ce-BDC 衍生的 CeO2-B 表面形成了更多的氧空位和相应的表面氧物种，导致 Ru 与 CeO2-B 之间的相互作用更强，从而促进了催化剂对 CO2 的吸附和加氢能力，使其具有更好的催化性能。原位漫反射红外傅立叶变换（DRIFT）研究进一步揭示了 HCOO* 转化为 CH4 的途径是一种更具竞争力的 CO2 加氢转化为 CH4 的途径。

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Ru/CeO2 catalyst derived from Ce-based MOF for highly efficient catalytic CO2 methanation integrated with renewable hydrogen

A series of highly ordered microporous Ce-based metal-organic frameworks (MOFs) were synthesized as the precursors for catalyst construction. The corresponding Ru catalysts were prepared by Ru impregnation on the derived CeO₂ by pyrolysis of Ce-MOF, and investigated for the CH₄ synthesis via CO₂ hydrogenation. Among the catalysts, Ru catalyst supported on the CeO₂-B derived from Ce-BDC exhibited a highly competitive efficiency for CO₂ methanation, giving a CH₄ selectivity of 100% with a CO₂ conversion of 62% at 275 °C and 0.1 MPa, and the CH₄ productivity reached 0.49 mol/(mol_Ru·h). Characterization results revealed that more oxygen vacancies and corresponding surface oxygen species formed on the surface of CeO₂-B derived from Ce-BDC caused to the stronger interaction between Ru and CeO₂-B, which promoted the CO₂ adsorption and hydrogenation capacity of the catalyst, resulting in its better catalytic property. In situ diffuse reflectance infrared Fourier transform (DRIFT) studies further revealed that the route of HCOO* into CH₄ is a more competitive way of CO₂ hydrogenation to CH₄.

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来源期刊

Fuel Processing Technology 工程技术-工程：化工

CiteScore

13.20

自引率

9.30%

发文量

398

审稿时长

26 days

期刊介绍： Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.