Boosting the CO2 methanation over Ni/Ce0.90RE0.10Oδ by regulating of oxygen vacancy density

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL
Jingyi Zhang , Liang Yuan , Yue Li , Yuntao Liang , Lulu Zhou , Yongdong Chen
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引用次数: 0

Abstract

The oxygen vacancies are significant defects that serve as reactive sites in several catalytic reactions. The CO2 methanation catalysts were facilely designed through tailoring the local electron density on oxygen vacancies by introducing different electron acceptors (Pr, La and Y). We prepared a series of Ni/Ce0.90RE0.10Oδ (RE = rare earth element) catalysts to boost catalytic activity of CO2 methanation at low temperature. It demonstrated the concentration of oxygen vacancies could be significantly regulated by doping strategy, hence altering the local microelectronic structure of catalyst and strengthening the MSI effect. The Ni/Ce0.90Y0.10Oδ catalyst demonstrated the greatest density of oxygen vacancies and optimal CO2 methanation performance. The CO2 conversion and CH4 selectivity achieved 84.6 % and 99.8 % at 270 °C, respectively. In situ DRIFTS revealed Ni/Ce0.90Y0.10Oδ catalyst enhanced the formate pathway. These results can provide better guidance for CO2 utilization technology to develop more efficient catalysts.

Abstract Image

通过调节氧空位密度促进Ni/Ce0.90RE0.10Oδ上的CO2甲烷化
氧空位是重要的缺陷,在许多催化反应中充当活性位点。通过引入不同的电子受体(Pr, La和Y)来调整氧空位上的局部电子密度,从而方便地设计了CO2甲烷化催化剂。我们制备了一系列Ni/Ce0.90RE0.10Oδ (RE =稀土元素)催化剂,以提高CO2甲烷化的低温催化活性。结果表明,掺杂策略可以显著调节氧空位的浓度,从而改变催化剂的局部微电子结构,增强MSI效应。Ni/Ce0.90Y0.10Oδ催化剂表现出最大的氧空位密度和最佳的CO2甲烷化性能。在270℃下,CO2转化率和CH4选择性分别达到84.6%和99.8%。原位漂移显示Ni/Ce0.90Y0.10Oδ催化剂增强了甲酸途径。这些结果可以为CO2利用技术开发更高效的催化剂提供更好的指导。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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