开发原位制备碳Xerogel上的镓锰共基化合物的方法,用于碱性介质中的氧还原反应。

IF 4.4 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Nanomaterials Pub Date : 2024-08-19 DOI:10.3390/nano14161362
Jhony Xavier Flores-Lasluisa, Bryan Carré, Joachim Caucheteux, Philippe Compère, Alexandre F Léonard, Nathalie Job
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引用次数: 0

摘要

含有 La、Mn 和 Co 阳离子的金属氧化物可在电化学过程中催化氧还原反应 (ORR)。然而,这些材料需要碳支持和两种化合物之间的最佳相互作用才能发挥活性。在这项工作中,开发了两种在碳 xerogel 上制备 La-Mn-Co 基化合物复合材料的方法。利用溶胶-凝胶法,将金属基材料沉积在现有的碳 xerogel 上,反之亦然。所选的金属氧化物是 LaMn0.7Co0.3O3 包晶体,它对直接 ORR 具有良好的催化性能和选择性。所有制备的复合材料都在碱性液体电解质中进行了 ORR 测试,并通过 XRD、XPS、SEM 或 N2 吸附等多种物理化学技术进行了表征。虽然使用这些原位方法,包晶结构要么分解了,要么没有形成,但这些材料表现出了很高的催化活性,这可归因于氧化物与碳支持物之间通过 C-O-M 共价键加强了相互作用,以及形成了新的活性位点,如 MnO/Co 异质界面。此外,在碳 xerogel 上合成金属化合物的过程中还形成了 Co-Nx-C 物种。这些物种对 ORR 具有很强的催化活性。因此,在碳 xerogel 上合成金属化合物形成的复合材料在 ORR 中表现出最佳性能,这可归因于 MnO/Co 异质界面和 Co-Nx-C 物种的存在以及两种化合物之间的强相互作用。此外,小尺寸的纳米颗粒可为反应提供更多的活性位点。
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Development of In Situ Methods for Preparing La-Mn-Co-Based Compounds over Carbon Xerogel for Oxygen Reduction Reaction in an Alkaline Medium.

Metal oxides containing La, Mn, and Co cations can catalyze oxygen reduction reactions (ORRs) in electrochemical processes. However, these materials require carbon support and optimal interactions between both compounds to be active. In this work, two approaches to prepare composites of La-Mn-Co-based compounds over carbon xerogel were developed. Using sol-gel methods, either the metal-based material was deposited on the existing carbon xerogel or vice versa. The metal oxide selected was the LaMn0.7Co0.3O3 perovskite, which has good catalytic behavior and selectivity towards direct ORRs. All the as-prepared composites were tested for ORRs in alkaline liquid electrolytes and characterized by diverse physicochemical techniques such as XRD, XPS, SEM, or N2 adsorption. Although the perovskite structure either decomposed or failed to form using those in situ methods, the materials exhibited great catalytic activity, which can be ascribed to the strengthening of the interactions between oxides and the carbon support via C-O-M covalent bonds and to the formation of new active sites such as the MnO/Co heterointerfaces. Moreover, Co-Nx-C species are formed during the synthesis of the metal compounds over the carbon xerogel. These species possess a strong catalytic activity towards ORR. Therefore, the composites formed by synthesizing metal compounds over the carbon xerogel exhibit the best performance in the ORR, which can be ascribed to the presence of the MnO/Co heterointerfaces and Co-Nx-C species and the strong interactions between both compounds. Moreover, the small nanoparticle size leads to a higher number of active sites available for the reaction.

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来源期刊
Nanomaterials
Nanomaterials NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
8.50
自引率
9.40%
发文量
3841
审稿时长
14.22 days
期刊介绍: Nanomaterials (ISSN 2076-4991) is an international and interdisciplinary scholarly open access journal. It publishes reviews, regular research papers, communications, and short notes that are relevant to any field of study that involves nanomaterials, with respect to their science and application. Thus, theoretical and experimental articles will be accepted, along with articles that deal with the synthesis and use of nanomaterials. Articles that synthesize information from multiple fields, and which place discoveries within a broader context, will be preferred. There is no restriction on the length of the papers. Our aim is to encourage scientists to publish their experimental and theoretical research in as much detail as possible. Full experimental or methodical details, or both, must be provided for research articles. Computed data or files regarding the full details of the experimental procedure, if unable to be published in a normal way, can be deposited as supplementary material. Nanomaterials is dedicated to a high scientific standard. All manuscripts undergo a rigorous reviewing process and decisions are based on the recommendations of independent reviewers.
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