Enhancing the performance of a novel CoRu/CeO2 bimetallic catalyst for the dry reforming of methane via a mechanochemical process

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-12-23 DOI:10.1016/j.apcatb.2023.123624

Marina Armengol-Profitós , Andrea Braga , Laia Pascua-Solé , Ilaria Lucentini , Xènia Garcia , Lluís Soler , Xavier Vendrell , Isabel Serrano , Ignacio J. Villar-Garcia , Virgina Pérez-Dieste , Carlos Escudero , Núria J. Divins , Jordi Llorca

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Abstract

A mechanochemical synthesis method has been used to synthesize CoRu nanoparticles supported on CeO₂ for methane dry reforming. In this work, we study the effect of Ru addition to Co/CeO₂-based catalysts and of the synthesis method by screening their catalytic activity, using synchrotron X-ray diffraction (XRD), and operando near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS). Ruthenium addition directly impacts the reducibility of cobalt species and results in smaller particle sizes, as demonstrated by H₂-temperature programmed reduction and XRD. NAP-XPS shows that Ru modifies the metal-support interaction, as evidenced by the higher Ce³⁺/Ce ratios for the bimetallic samples and tuning the oxidation state of Ru. The synthesis method also influences the dispersion of Co and Ru on the surface. Mechanochemically-prepared samples (mono- and bimetallic) outperformed the conventionally-synthesized counterparts by reaching higher CH₄ and CO₂ conversions, resulting in a stable CoRu/CeO₂ catalyst for 24 h at 700 °C and yielding an H₂/CO ratio close to 1.

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通过机械化学工艺提高新型 CoRu/CeO2 双金属催化剂在甲烷干转化中的性能

我们采用机械化学合成法合成了以 CeO2 为载体的 CoRu 纳米粒子，用于甲烷干转化。在这项工作中，我们利用同步辐射 X 射线衍射 (XRD) 和操作性近常压 X 射线光电子能谱 (NAP-XPS)，通过筛选催化活性，研究了在 Co/CeO2 基催化剂中添加 Ru 以及合成方法的影响。如 H2 温度编程还原和 XRD 所示，钌的添加直接影响了钴的还原性，并导致颗粒尺寸变小。NAP-XPS 显示，Ru 改变了金属与支撑物之间的相互作用，双金属样品中更高的 Ce3+/Ce 比率和 Ru 氧化态的调整都证明了这一点。合成方法也会影响 Co 和 Ru 在表面的分散。机械化学法制备的样品（单金属和双金属）的性能优于传统合成法制备的样品，其 CH4 和 CO2 转化率更高，在 700 °C 下 24 小时仍能保持 CoRu/CeO2 催化剂的稳定性，H2/CO 比率接近 1。

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来源期刊

Applied Catalysis B: Environmental 环境科学-工程：化工

CiteScore

38.60

自引率

6.30%

发文量

1117

审稿时长

24 days

期刊介绍： Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.