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Ni/YO上CO甲烷化机理:漫反射红外傅里叶变换光谱研究

CO methanation mechanism over Ni/YO: an diffuse reflectance infrared Fourier transform spectroscopic study.

作者信息

Hasan Masitah, Asakoshi Toshiki, Muroyama Hiroki, Matsui Toshiaki, Eguchi Koichi

机构信息

Department of Energy and Hydrocarbon Chemistry, Graduate School of Engineering, Kyoto University, Nishikyo-ku, Kyoto 615-8510, Japan.

出版信息

Phys Chem Chem Phys. 2021 Mar 11;23(9):5551-5558. doi: 10.1039/d0cp06257j.

Abstract

Supported Ni catalysts are active in CO2 methanation. It is important to understand the reaction mechanism for the development of highly-active catalysts. In this study, we investigated the reaction pathways of CO2 methanation over Ni/Y2O3 and Ni/Al2O3 based on the adsorbates observed by diffuse reflectance infrared Fourier transform spectroscopy. For Ni/Al2O3, linear and bridged CO adsorbates were converted to nickel carbonyl hydride and/or formyl species, which would be further hydrogenated to methane. In contrast, the formation of formate adsorbates was specifically confirmed over Ni/Y2O3 under the CO2 methanation condition. The hydrogen molecule was activated by dissociatively-adsorbing on Ni particles. Then, the hydrogenation of formate adsorbates by the activated hydrogen species proceeded sequentially to form methane. The observed bridged CO species would not be a major intermediate for Ni/Y2O3.

摘要

负载型镍催化剂对二氧化碳甲烷化具有活性。了解反应机理对于开发高活性催化剂至关重要。在本研究中,我们基于漫反射红外傅里叶变换光谱观察到的吸附质,研究了二氧化碳在Ni/Y2O3和Ni/Al2O3上甲烷化的反应途径。对于Ni/Al2O3,线性和桥式CO吸附质转化为羰基氢化镍和/或甲酰基物种,这些物种会进一步氢化为甲烷。相比之下,在二氧化碳甲烷化条件下,在Ni/Y2O3上特别证实了甲酸盐吸附质的形成。氢分子通过在镍颗粒上解离吸附而被活化。然后,活化的氢物种对甲酸盐吸附质进行顺序氢化以形成甲烷。观察到的桥式CO物种对于Ni/Y2O3不是主要中间体。

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