调控五配位Al^(3+)含量制备高性能低温Sabatier反应催化剂  

The preparation of high performance catalyst for low-temperature Sabatier reaction by regulating the content of pentacoordinated Al^(3+)

作　　者：陈志强 蒋榕培[1,2] 刘梦然 王青 项锴 孙海云[1,2] 方涛[1,2] CHEN Zhiqiang;JIANG Rongpei;LIU Mengran;WANG Qing;XIANG Kai;SUN Haiyun;FANG Tao(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：《高校化学工程学报》2024年第3期483-492,共10页Journal of Chemical Engineering of Chinese Universities

摘　　要：为了制备出高性能低温Sabatier反应Ru基催化剂,通过调控Al_(2)O_(3)载体中五配位Al^(3+)的含量(五配位Al^(3+)占Al物种的比例),实现对Ru基活性位点电子性质的调控。在此过程中,利用~(27)Al固体核磁共振(~(27)Al-NMR)检测Al_(2)O_(3)载体中五配位Al^(3+)的含量,借助X射线光电子能谱仪(XPS)和H_2程序升温还原(H_(2)-TPR)考察Ru基活性位点电子性质的调控效果,利用固定床反应器测试催化剂性能。结果表明,Al_(2)O_(3)载体中的五配位Al^(3+)可有效调控Ru基活性位点的电子性质,进而提升低温Sabatier反应Ru基催化剂性能。其中,以五配位Al^(3+)含量约为28.1%的Al_(2)O_(3)载体制备的Ru基催化剂,在低温区(<300℃)的CO_(2)转化率和CH_4选择性均可达90%以上。而且,在100 h的稳定性测试中,催化性能没有明显降低。In order to prepare the excellent Ru-based catalyst for low-temperature Sabatier reaction,the electronic properties of Ru-based active sites were regulated by adjusting the content of pentacoordinated Al^(3+)species during the preparation of Al_(2)O_(3) supports.The relative content of pentacoordinated Al^(3+)in different Al_(2)O_(3) samples was investigated by ^(27)Al nuclear magnetic resonance(^(27)Al-NMR),the electronic properties of the Ru-based active sites were characterized by X-ray photoelectron spectroscopy(XPS)and H_(2) temperature-programmed reduction(H_(2)-TPR),and the performances of different catalysts were evaluated by a fixed bed reactor.It was found that the pentacoordinated Al^(3+)species in the Al_(2)O_(3) support could effectively regulate the electronic property of the Ru-based active sites,thus improving the catalytic performance for Sabatier reaction.Specially,CO_(2) conversion and CH_(4) selectivity of Sabatier reaction using Ru-based catalyst prepared on Al_(2)O_(3) support with a pentacoordinated Al^(3+)species content of 28.1%could both reach over 90%at the low reaction temperature(<300℃).Moreover,during 100 h stability test,there was no significant decrease in catalytic performance.

关 键 词：低温Sabatier反应 Ru基催化剂 五配位Al^(3+) 电子性质调控 催化性能提升 

分 类 号：O614.31[理学—无机化学]