由[Co(NH3)6][Fe(CN)6]热解衍生的 Fe-Co 双金属催化剂的二氧化碳加氢反应

IF 3.8 3区 化学 Q2 CHEMISTRY, PHYSICAL
Catalysts Pub Date : 2023-11-28 DOI:10.3390/catal13121475
A. Gosteva, Mayya V. Kulikova, M. I. Ivantsov, A. A. Grabchak, Yulya P. Semushina, S. Lapuk, A. Gerasimov, N. Tsvetov
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引用次数: 0

摘要

减少大气中的二氧化碳含量是一项非常重要的任务。因此,开发和寻找新的催化系统合成方法,将二氧化碳催化转化为有价值的产品,是一项紧迫的任务。在这项工作中,催化剂是通过热解双复合物获得的。为此,还利用非等温动力学的等转化法和模型法对双络合盐-[Co(NH)3]6][Fe(CN)6]的热解过程参数进行了动力学研究。催化剂的研究采用了多种物理化学方法--X 射线衍射 (XRD)、红外光谱 (IR)、拉曼光谱和 X 射线光电子能谱 (XPS)。结果表明,在催化剂制备阶段,形成了 CoFe 合金,而表面主要由 sp2 杂化的碳组成,金属以尖晶石 CoFe2O4 的形式存在。研究表明,基于双金属盐的催化剂在二氧化碳加氢过程中具有活性,无需预活化阶段(二氧化碳转化率达到 28%,比活性为 4.0 µmolCO2/gMe-s)。实验证明,通过用氢气预处理催化剂,可以改变二氧化碳氢化过程的选择性(在未还原催化剂存在的情况下,甲烷生成的选择性为 46.4-68.0%,而在还原催化剂存在的情况下,甲烷生成的选择性为 5.1-16.5%)。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
CO2 Hydrogenation over Fe-Co Bimetallic Catalyst Derived from the Thermolysis of [Co(NH3)6][Fe(CN)6]
Reducing the amount of CO2 in the atmosphere is a very important task. Therefore, the development and search for new approaches to the synthesis of catalytic systems, allowing for the catalytic conversion of CO2 into valuable products, is an urgent task. In this work, the catalyst was obtained by the thermolysis of a double complex compound. In this regard, kinetic studies of the parameters of the thermolysis process of double complex salts-[Co(NH)3]6][Fe(CN)6] were additionally determined using isoconversion and model approaches of non-isothermal kinetics. The catalyst was studied using various physicochemical methods—X-ray diffraction (XRD), infrared (IR)-spectroscopy, Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). It was shown that, at the stage of catalyst preparation, the formation of a CoFe alloy occurred, while the surface mainly consisted of carbon in sp2-hybridization, and the metals existed in the form of spinel CoFe2O4. It was shown that catalysts based on bimetallic salts were active in the process of hydrogenation of carbon dioxide without a pre-activation stage (CO2 conversion reached 28%, with a specific activity of 4.0 µmolCO2/gMe·s). It was established that it was possible to change the selectivity of the carbon dioxide hydrogenation process by pre-treating the catalyst with hydrogen (selectivity for methane formation in the presence of an unreduced catalyst is 46.4–68.0%, whereas in the presence of a reduced catalyst it is 5.1–16.5%).
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来源期刊
Catalysts
Catalysts CHEMISTRY, PHYSICAL-
CiteScore
6.80
自引率
7.70%
发文量
1330
审稿时长
3 months
期刊介绍: Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.
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