Surface Iron Species in Palladium–Iron Intermetallic Nanocrystals that Promote and Stabilize CO2 Methanation

  • 影响因子:15.336
  • DOI码:10.1002/anie.201916032
  • 发表刊物:Angew.Chem.Int.Ed
  • 关键字:CO2 hydrogenation, intermetallic nanocrystals, iron, palladium, Binary alloys, Carbon dioxide, Hydrogenation, Intermetallics, Methanation, Nanocrystals, Direct conversion, Efficient catalysts, Intrinsic mechanisms, Iron intermetallics, Mechanistic studies, Reduction process, Reversible oxidation
  • 摘要:It is of pivotal importance to develop efficient catalysts and investigate the intrinsic mechanism for CO2 methanation. Now, it is reported that PdFe intermetallic nanocrystals afforded high activity and stability for CO2 methanation. The mass activity of fct-PdFe nanocrystals reached 5.3 mmol g−1 h−1, under 1 bar (CO2:H2=1:4) at 180 °C, being 6.6, 1.6, 3.3, and 5.3 times as high as that of fcc-PdFe nanocrystals, Ru/C, Ni/C, and Pd/C, respectively. After 20 rounds of successive reaction, 98 % of the original activity was retained for PdFe intermetallic nanocrystals. Further mechanistic studies revealed that PdFe intermetallic nanocrystals enabled the maintenance of metallic Fe species via a reversible oxidation–reduction process in CO2 methanation. The metallic Fe in PdFe intermetallic nanocrystals induced the direct conversion of CO2 into CO* as the intermediate, contributing to the enhanced activity.
  • 合写作者:Yi Cui, Ziyuan Chen, Jiaxin Wu, Yulu Cao, Jie Luo, Yizhou Dai, Wei-Xue Li
  • 第一作者:Laihao Luo, Menglin Wang
  • 通讯作者:Jun Bao, Jie Zeng
  • 卷号:59
  • 期号:34
  • 页面范围:14434-14442
  • 是否译文:
  • 发表时间:2020/04/07
  • 发布期刊链接:https://onlinelibrary.wiley.com/doi/10.1002/anie.201916032