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

Impact Factor:

15.336

DOI number:

10.1002/anie.201916032

Journal:

Angew.Chem.Int.Ed

Key Words:

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

Abstract:

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.

Co-author:

Yi Cui, Ziyuan Chen, Jiaxin Wu, Yulu Cao, Jie Luo, Yizhou Dai, Wei-Xue Li

First Author:

Laihao Luo, Menglin Wang

Correspondence Author:

Jun Bao, Jie Zeng

Volume:

59

Issue:

34

Page Number:

14434-14442

Translation or Not:

no

Date of Publication:

2020-04-07

Links to published journals:

https://onlinelibrary.wiley.com/doi/10.1002/anie.201916032