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Ni/Sm2O3-CeO2/Al2O3催化剂氧空位对二氧化碳低温甲烷化的影响OA北大核心CSTPCD

Effect of oxygen vacancies in Ni/Sm2O3-CeO2/Al2O3 catalyst on CO2 methanation at low temperature

中文摘要英文摘要

通过水热合成法将Mn、Sm和Ce作为助剂,掺入水滑石(LDHs)前体后经焙烧-还原分别得到Ni/Sm2O3-CeO2/Al2O3和Ni/MnOx-Sm2O3-CeO2/Al2O3催化剂,研究了两种结构催化剂的二氧化碳低温甲烷化反应.研究结果表明,相较于Ni/Sm2O3-CeO2/Al2O3,MnOx的引入使Ni/MnOx-Sm2O3-CeO2/Al2O3在225℃以下表现出优异的性能,CO2转化率达到68%,CH4选择性达到100%,且在100h内具有良好的稳定性,150℃时TOF为0.087s-1,大于Ni/Sm2O3-CeO2/Al2O3(0.013s-1).这主要是由于引入MnOx,在保持金属颗粒高度分散的同时,借助MnOx在催化剂表面连续还原,提高了Ni/MnO-Sm2O3-CeO2/Al2O3表面氧空位浓度且增加了催化剂的碱性位点,促进了二氧化碳的吸附和活化.原位红外结果进一步表明,低温下催化剂表面氧空位促进甲酸盐和甲氧基中间物种的生成,进而提高了二氧化碳甲烷化活性.

Ni/Sm2O3-CeO2/Al2O3 and Ni/MnOx-Sm2O3-CeO2/Al2O3 catalysts were obtained by using Mn,Sm and Ce sources in the form of LDHs precursor by hydrothermal synthesis after a standard calcination and reduction treatment.Subsequently,the catalytic performance of the two catalysts were investigated at low temperature in CO2 methanation.Compared to Ni/Sm2O3-CeO2/Al2O3,Ni/MnOx-Sm2O3-CeO2/Al2O3 with the introduction of MnOx showed an excellent performance below 225℃,with 68%of CO2 conversion and 100%of CH4 selectivity,and 0.087s-1 of TOF,which was higher than that of Ni/Sm2O3-CeO2/Al2O3(0.013s-1).Meanwhile,Ni/MnOx-Sm2O3-CeO2/Al2O3 maintained stable CO2 conversion and CH4 selectivity in long-term test for 100h.This was mainly due to the fact that the introduction of M nO increased the oxygen vacancies on Ni/MnOx-Sm2O3-CeO2/Al2O3 with a high degree of Ni particle dispersion.Meanwhile,MnOx could also increase the basic sites of the resultant catalyst,which promoted CO2adsorption and activation.In situ DRIFTS analysis further revealed that oxygen vacancies on Ni/MnOx-Sm2O3-CeO2/Al2O3 promoted the formation of formate and methoxy intermediates at low temperatures,leading to an enhanced catalytic properties in CO2 methanation.

郭潇东;毛玉娇;刘相洋;邱丽;于峰;闫晓亮

太原理工大学化学工程与技术学院,山西太原 030024||太原理工大学省部共建煤基能源清洁高效利用国家重点实验室,山西太原 030024

化学工程

二氧化碳加氢甲烷催化剂催化(作用)

carbon dioxidehydrogenationmethanecatalystcatalysis

《化工进展》 2024 (004)

1840-1850 / 11

国家自然科学基金(22108189,21878203).

10.16085/j.issn.1000-6613.2023-0571

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