Catalysts for ethanol dry reforming based on high-entropy perovskites

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-02-17 DOI:10.1016/j.jcat.2025.116028
Nikita F. Eremeev , Semon A. Hanna , Ekaterina M. Sadovskaya , Aleksandra A. Leonova , Olga A. Bulavchenko , Arcady V. Ishchenko , Igor P. Prosvirin , Vladislav A. Sadykov , Yuliya N. Bespalko
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Abstract

Ethanol dry reforming is a promising way to produce syngas and hydrogen due to utilization of carbon dioxide and ability to produce ethanol using renewable sources. Main problem associated with ethanol dry reforming reaction is coke formation. Coking suppression can be achieved in a few ways including use of catalysts possessing required oxygen transport properties. High entropy oxides are of interest in application as catalysts for ethanol dry reforming and other reactions due to their structural stability, disordering features and tunability of functional properties. In this work, the catalysts based on Ni and multiple doped La manganites are studied. The oxides are synthesized by modified Pechini and citrate techniques, and the catalysts are prepared by wetness impregnation. The samples are characterized by XRD, TEM with EDX analysis, XPS. Oxygen transport and redox properties are studied by temperature-programmed isotope exchange of oxygen and reduction. According to structural and morphological studies, the samples are nanosized and form perovskite-like structure. The surface features of samples were characterized by XPS. The samples demonstrate a moderate oxygen mobility (D* up to ∼10–12 cm2/s at 700 °C) required for catalytic operation and coking suppression. Tests in ethanol dry reforming demonstrated fine performance and good stability in the reaction conditions.

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基于高熵钙钛矿的乙醇干重整催化剂
乙醇干重整是一种很有前途的合成气和氢气生产方法,因为它利用二氧化碳和利用可再生能源生产乙醇的能力。乙醇干重整反应的主要问题是焦炭的形成。抑制焦化可以通过几种方式实现,包括使用具有所需氧传输特性的催化剂。高熵氧化物由于其结构稳定性、无序性和功能性质的可调性,在乙醇干重整和其他反应中具有广泛的应用前景。本文主要研究了Ni和多掺杂La锰矿石的催化剂。采用改性佩奇尼法和柠檬酸法合成了氧化物,采用湿浸渍法制备了催化剂。采用XRD、TEM、EDX、XPS对样品进行了表征。通过氧和还原的程序升温同位素交换,研究了氧的输运和氧化还原性质。结构和形态研究表明,样品为纳米级,呈钙钛矿样结构。用XPS表征了样品的表面特征。样品表现出适度的氧迁移率(D*在700 °C时高达~ 10-12 cm2/s),这是催化操作和焦化抑制所需的。乙醇干重整试验表明,该工艺性能优良,稳定性好。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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