调控五配位Al3+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 Al3+
陈志强 1蒋榕培 1刘梦然 1王青 1项锴 1孙海云 1方涛1
作者信息
- 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;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
- 折叠
摘要
为了制备出高性能低温Sabatier反应Ru基催化剂,通过调控Al2O3载体中五配位Al3+的含量(五配位Al3+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 27Al固体核磁共振(27Al-NMR)检测Al2O3载体中五配位Al3+的含量,借助X射线光电子能谱仪(XPS)和H2程序升温还原(H2-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,Al2O3载体中的五配位Al3+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Al3+含量约为 28.1%的Al2O3载体制备的Ru基催化剂,在低温区(<300)℃的CO2转化率和CH4 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.
Abstract
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 Al3+species during the preparation of Al2O3 supports.The relative content of pentacoordinated Al3+in different Al2O3 samples was investigated by 27Al nuclear magnetic resonance(27Al-NMR),the electronic properties of the Ru-based active sites were characterized by X-ray photoelectron spectroscopy(XPS)and H2 temperature-programmed reduction(H2-TPR),and the performances of different catalysts were evaluated by a fixed bed reactor.It was found that the pentacoordinated Al3+species in the Al2O3 support could effectively regulate the electronic property of the Ru-based active sites,thus improving the catalytic performance for Sabatier reaction.Specially,CO2 conversion and CH4 selectivity of Sabatier reaction using Ru-based catalyst prepared on Al2O3 support with a pentacoordinated Al3+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Al3+/电子性质调控/催化性能提升Key words
low-temperature Sabatier reaction/Ru-based catalyst/pentacoordinated Al3+/regulation of electronic property/catalytic performance enhancement引用本文复制引用
出版年
2024