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负载镍的二氧化铈纳米结构催化剂上的热催化CO转化:一项非弹性电子隧道谱X射线光电子能谱研究

Thermocatalytic CO Conversion over a Nickel-Loaded Ceria Nanostructured Catalyst: A NAP-XPS Study.

作者信息

Barroso-Bogeat Adrián, Blanco Ginesa, Pérez-Sagasti Juan José, Escudero Carlos, Pellegrin Eric, Herrera Facundo C, Pintado José María

机构信息

Department of Materials Science and Metallurgical Engineering and Inorganic Chemistry, Faculty of Sciences, University of Cádiz, Campus Río San Pedro s/n, 11510 Puerto Real (Cádiz), Spain.

Institute for Research in Electron Microscopy and Materials (IMEYMAT), Faculty of Sciences, University of Cádiz, Campus Río San Pedro s/n, 11510 Puerto Real (Cádiz), Spain.

出版信息

Materials (Basel). 2021 Feb 3;14(4):711. doi: 10.3390/ma14040711.

Abstract

Despite the increasing economic incentives and environmental advantages associated to their substitution, carbon-rich fossil fuels are expected to remain as the dominant worldwide source of energy through at least the next two decades and perhaps later. Therefore, both the control and reduction of CO emissions have become environmental issues of major concern and big challenges for the international scientific community. Among the proposed strategies to achieve these goals, conversion of CO by its reduction into high added value products, such as methane or syngas, has been widely agreed to be the most attractive from the environmental and economic points of view. In the present work, thermocatalytic reduction of CO with H was studied over a nanostructured ceria-supported nickel catalyst. Ceria nanocubes were employed as support, while the nickel phase was supported by means a surfactant-free controlled chemical precipitation method. The resulting nanocatalyst was characterized in terms of its physicochemical properties, with special attention paid to both surface basicity and reducibility. The nanocatalyst was studied during CO reduction by means of Near Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS). Two different catalytic behaviors were observed depending on the reaction temperature. At low temperature, with both Ce and Ni in an oxidized state, CH formation was observed, whereas at high temperature above 500 °C, the reverse water gas shift reaction became dominant, with CO and HO being the main products. NAP-XPS was revealed as a powerful tool to study the behavior of this nanostructured catalyst under reaction conditions.

摘要

尽管用富含碳的化石燃料替代能源有着越来越多的经济激励因素和环境优势,但预计至少在未来二十年甚至更久之后,富含碳的化石燃料仍将是全球主要的能源来源。因此,控制和减少二氧化碳排放已成为国际科学界主要关注的环境问题和巨大挑战。在为实现这些目标而提出的策略中,通过将二氧化碳还原为高附加值产品(如甲烷或合成气)来转化二氧化碳,从环境和经济角度来看,已被广泛认为是最具吸引力的策略。在本工作中,研究了在纳米结构二氧化铈负载的镍催化剂上用氢气对二氧化碳进行热催化还原。使用二氧化铈纳米立方体作为载体,而镍相通过无表面活性剂的可控化学沉淀法负载。对所得的纳米催化剂进行了物理化学性质表征,特别关注了表面碱性和还原性。通过近常压X射线光电子能谱(NAP-XPS)研究了该纳米催化剂在二氧化碳还原过程中的情况。根据反应温度观察到了两种不同的催化行为。在低温下,铈和镍均处于氧化态时,观察到甲烷生成,而在高于500℃的高温下,逆水煤气变换反应占主导,一氧化碳和水是主要产物。NAP-XPS被证明是研究这种纳米结构催化剂在反应条件下行为的有力工具。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d159/7913549/811c59897a07/materials-14-00711-g001.jpg

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