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溶液燃烧法制备的血小板状二氧化铈催化剂及铁掺杂对由一氧化碳合成碳酸二甲酯的影响

Platelet Ceria Catalysts from Solution Combustion and Effect of Iron Doping for Synthesis of Dimethyl Carbonate from CO.

作者信息

Rusta Nicoletta, Mameli Valentina, Ricci Pier Carlo, Porcu Stefania, Seeharaj Panpailin, Marciniak Aryane A, Santos Evelyn C S, Alves Odivaldo Cambraia, Mota Claudio J A, Rombi Elisabetta, Cannas Carla

机构信息

Department of Chemical and Geological Sciences, University of Cagliari, Cagliari, Italy.

National Interuniversity Consortium of Materials Science and Technology (INSTM), Florence, Italy.

出版信息

Chempluschem. 2025 Jan;90(1):e202400521. doi: 10.1002/cplu.202400521. Epub 2024 Nov 1.

Abstract

Solution combustion (SC) remains among the most promising synthetic strategies for the production of crystalline nanopowders from an aqueous medium, due to its easiness, time and cost-effectiveness, scalability and eco-friendliness. In this work, this method was selected to obtain anisometric ceria-based nanoparticles applied as catalysts for the direct synthesis of dimethyl carbonate. The catalytic performances were studied for the ceria and Fe-doped ceria from SC (CeO-SC, CeFeO-SC) in comparison with the ceria nanorods (CeO-HT, CeFeO-HT) obtained by hydrothermal (HT) method, one of the most studied systems in the literature. Indeed, the ceria nanoparticles obtained by SC were found to be highly crystalline, platelet-shaped, arranged in a mosaic-like assembly and with smaller crystallite size (≈6 nm vs. ≈17 nm) and higher surface area (80 m g vs. 26 m g) for the undoped sample with respect to the Fe-doped counterpart. Although all samples exhibit an anisometric morphology that should favor the exposition of specific crystalline planes, HT-samples showed better performances due to higher oxygen vacancies concentration and lower amount of strong basic and acid sites.

摘要

溶液燃烧法(SC)仍是从水性介质中制备结晶纳米粉末最具前景的合成策略之一,因其简便、省时、经济高效、可扩展性强且环保。在本工作中,选择该方法来制备用作直接合成碳酸二甲酯催化剂的各向异性氧化铈基纳米颗粒。与水热法(HT)制备的氧化铈纳米棒(CeO-HT、CeFeO-HT)相比,研究了溶液燃烧法制备的氧化铈和铁掺杂氧化铈(CeO-SC、CeFeO-SC)的催化性能,水热法是文献中研究最多的体系之一。实际上,发现溶液燃烧法制备的氧化铈纳米颗粒高度结晶,呈片状,以镶嵌状组装排列,对于未掺杂样品,其晶粒尺寸更小(约6 nm对约17 nm),比表面积更高(80 m²/g对26 m²/g),相对于铁掺杂对应物而言。尽管所有样品均呈现各向异性形态,这应有利于特定晶面的暴露,但水热法制备的样品由于氧空位浓度更高以及强碱和酸位点数量更少而表现出更好的性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/696a/11734582/0a011de38431/CPLU-90-e202400521-g002.jpg

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