首页|载体氧空位提升Sabatier反应钌基催化剂性能研究

载体氧空位提升Sabatier反应钌基催化剂性能研究

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通过尿素的掺杂,有效诱导Al2O3载体氧空位的形成,进而通过金属-载体之间的相互作用,提升Al2O3载体表面Ru基活性物种的分散度,调控Ru基活性中心的电子性质,从而达到有效提升Sabatier反应Ru基催化剂性能的目的.在此过程中,借助27Al核磁(27Al-NMR)验证了尿素的掺杂可有效诱导Al2O3载体中氧空位的形成.通过透射电子显微镜(TEM)发现,富含氧空位的Al2O3载体可将负载的Ru颗粒稳定在3.7 nm左右,且粒径分布集中.通过X射线光电子能谱(XPS)和H2程序升温还原(H2-TPR)发现,载体氧空位可有效调控Al2O3载体表面Ru基活性位点的电子性质.经过Sabatier反应性能测试发现,在300 ℃,nCO2∶nH2=1∶4,空速为6 000 mL·g-1·h-1的反应条件下,CO2转化率可达61.25%,CH4选择性可达92.31%,而且,在20 h的反应时间内,催化活性没有明显衰减.
Research on the property enhancement of Ru-based catalyst for Sabatier reaction by oxygen vacancy from the support
In this paper,the formation of oxygen vacancy in the Al2O3 support was induced by urea doping.Through metal-support interaction,the dispersion of Ru-based active species on the surface of the Al2O3 sup-port was improved.The electronic properties of Ru-based active centers was regulated,and then the catalytic performance of the Ru-based catalyst for Sabatier reaction was effectively improved.In this process,it was veri-fied by nuclear magnetic resonance spectroscopy(27Al-NMR)that urea doping can effectively induce the forma-tion of oxygen vacancy in the Al2O3 support.Transmission electron microscopy(TEM)showed that,the loaded Ru particles could be stabilized at about 3.7 nm on the surface of the Al2O3 support rich in oxygen vacancy,and the distribution of particle size was concentrated.By X-ray photoelectron spectroscopy(XPS)and H2pro-grammed temperature reduction(H2-TPR),it was found that the oxygen vacancy from the Al2O3 support can effectively regulate the electronic property of the Ru-based active sites.Sabatier reaction performance test showed that under the reaction condition of 300 ℃,nCO2∶nH2=1∶4 and 6000 mL/(g·h),the conversion rate of CO2 could be reached at 61.25%and the selectivity of CH4 could be reached at 92.31%.Moreover,the cata-lytic performance did not decrease within 20 hours of the reaction time.

Sabatier reactionRu-based catalystelectronic propertyoxygen vacancyCO2 conversion rate

陈志强、方涛、孙海云、王青、蒋榕培、刘梦然、项锴

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北京航天试验技术研究所航天绿色推进剂研究与应用北京市重点实验室,北京 100074

北京航天试验技术研究所航天液体推进剂研究中心,北京 100074

Sabatier反应 Ru基催化剂 电子性质 氧空位 CO2转化率

2024

功能材料
重庆材料研究院 中国仪器仪表学会仪表材料学会

功能材料

CSTPCD北大核心
影响因子:0.918
ISSN:1001-9731
年,卷(期):2024.55(5)