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Alkaline-assisted Ni nanocatalysts with largely enhanced low-temperature activity toward CO2 methanation

机译:Alkaline-assisted倪nanocatalysts很大程度上对二氧化碳的低温活性增加甲烷化

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摘要

The CO2 methanation reaction is a promising approach for the chemical transformation of carbon dioxide into useful fuels or products. The key challenge at present relies on the design and exploration of non-noble metal catalysts so as to achieve high activity at a low reaction temperature. In this work, we have obtained alkaline-assisted Ni nanocatalysts supported on Mg/Al mixed metal oxides (denoted as Nix/Mg-2-xAl-MMO) derived from Ni-Mg-Al hydrotalcite precursors. The catalytic performance toward CO2 methanation was studied in detail, and the best low-temperature reaction activity was obtained over Ni/MgAl-MMO (CO2 conversion: 97.9%; selectivity: 97.5%; 250 degrees C). By establishing the correlation between the catalytic performance and the alkaline site structure, it is found that the Ni nanoparticles and MgO base sites at the interface serve as dual active centers to cooperatively catalyze CO2 methanation, resulting in low-temperature reaction activity. Moreover, in situ diffuse reflectance Fourier transform infrared spectroscopy (in situ DRIFTS) demonstrates that MgO acts as the active site for CO2 activation to give carbonate/hydrocarbonate species, while Ni provides H-species for further hydrogenation of intermediates. Therefore, this work rationalizes the significant influence of alkaline-assisted Ni nanoparticles on CO2 methanation, which provides a promising heterogeneous catalyst for this reaction.
机译:二氧化碳甲烷化反应是一种很有前途的的化学转换的方法二氧化碳转化为有用的燃料或产品。目前依赖于设计和关键挑战探索非贵金属催化剂等实现高活动在低反应温度。alkaline-assisted倪nanocatalysts支持毫克/ Al混合金属氧化物(表示无/ Mg-2-xAl-MMO)来自Ni-Mg-Al水滑石前体。性能对二氧化碳甲烷化进行了研究细节,最好的低温反应活动得到了镍/ MgAl-MMO(二氧化碳转换:97.9%;摄氏度)。通过建立相关性与催化性能之间的碱性站点结构,发现倪纳米颗粒和采用基地网站的界面作为双活性中心合作催化二氧化碳甲烷化,导致低温反应活动。原位漫反射傅里叶变换原位红外光谱(飘)表明,分别充当的活性部位二氧化碳活化碳酸/重碳酸盐物种,而镍提供了进一步H-species加氢的中间体。工作成为合理化的重要影响alkaline-assisted镍纳米颗粒在二氧化碳甲烷化,它提供了一种有前途的异构反应的催化剂。

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