载体氧空位提升Sabatier反应钌基催化剂性能研究  

Research on the property enhancement of Ru-based catalyst for Sabatier reaction by oxygen vacancy from the support

作　　者：陈志强 方涛[1,2] 孙海云[1,2] 王青 蒋榕培[1,2] 刘梦然 项锴 CHEN Zhiqiang;FANG Tao;SUN Haiyun;WANG Qing;JIANG Rongpei;LIU Mengran;XIANG Kai(Beijing Key Laboratory of Research and Application for Aerospace Green Propellants,Beijing Institute of Aerospace Testing Technology,Beijing 100074,China;Aerospace Liquid Propellant Research Center,Beijing Institute of Aerospace Testing Technology,Beijing 100074,China)

机构地区：[1]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 [2]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

出　　处：《功能材料》2024年第5期5161-5168,共8页Journal of Functional Materials

摘　　要：通过尿素的掺杂,有效诱导Al_(2)O_(3)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Al_(2)O_(3)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^(27)Al核磁(^(27)Al-NMR)验证了尿素的掺杂可有效诱导Al_(2)O_(3)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Al_(2)O_(3)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H_(2)程序升温还原(H_(2)-TPR)发现,载体氧空位可有效调控Al_(2)O_(3)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℃,n CO_(2)∶n H_(2)=1∶4,空速为6000 mL·g^(-1)·h^(-1)的反应条件下,CO_(2)转化率可达61.25%,CH_(4)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。In this paper,the formation of oxygen vacancy in the Al_(2)O_(3)support was induced by urea doping.Through metal-support interaction,the dispersion of Ru-based active species on the surface of the Al_(2)O_(3)support 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 verified by nuclear magnetic resonance spectroscopy(^(27)Al-NMR)that urea doping can effectively induce the formation of oxygen vacancy in the Al_(2)O_(3)support.Transmission electron microscopy(TEM)showed that,the loaded Ru particles could be stabilized at about 3.7 nm on the surface of the Al_(2)O_(3)support rich in oxygen vacancy,and the distribution of particle size was concentrated.By X-ray photoelectron spectroscopy(XPS)and H_(2)programmed temperature reduction(H_(2)-TPR),it was found that the oxygen vacancy from the Al_(2)O_(3)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℃,n CO_(2)∶n H_(2)=1∶4 and 6000 mL/(g·h),the conversion rate of CO_(2)could be reached at 61.25%and the selectivity of CH 4 could be reached at 92.31%.Moreover,the catalytic performance did not decrease within 20 hours of the reaction time.

关 键 词：Sabatier反应 Ru基催化剂 电子性质 氧空位 CO_(2)转化率 

分 类 号：O614.31[理学—无机化学]