Tandem catalyzing the hydrodeoxygenation of 5-hydroxymethylfurfural over a Ni3Fe intermetallic supported Pt single-atom site catalyst

Single-atom site catalysts (SACs) have been used in multitudinous reactions delivering ultrahigh atom utilization and enhanced performance, but it is challenging for one single atom site to catalyze an intricate tandem reaction needing different reactive sites. Herein, we report a robust SAC with du...

Full description

Saved in:
Bibliographic Details
Published in:Chemical science (Cambridge) 2021-03, Vol.12 (11), p.4139-4146
Main Authors: Ge Meng, Ji, Kaiyue, Zhang, Wei, Kang, Yiran, Wang, Yu, Zhang, Ping, Yang-Gang, Wang, Li, Jun, Cui, Tingting, Sun, Xiaohui, Tan, Tianwei, Wang, Dingsheng, Li, Yadong
Format: Article
Language:English
Subjects:
Cascade chemical reactions
Catalysts
Catalytic converters
Chemistry
First principles
Hydroxymethylfurfural
Intermetallic compounds
Iron compounds
Nickel base alloys
Nickel compounds
Performance enhancement
Recyclability
Structural design
Online Access:Get full text
Tags: Add Tag
No Tags, Be the first to tag this record!
Description
Summary:Single-atom site catalysts (SACs) have been used in multitudinous reactions delivering ultrahigh atom utilization and enhanced performance, but it is challenging for one single atom site to catalyze an intricate tandem reaction needing different reactive sites. Herein, we report a robust SAC with dual reactive sites of isolated Pt single atoms and the Ni3Fe intermetallic support (Pt1/Ni3Fe IMC) for tandem catalyzing the hydrodeoxygenation of 5-hydroxymethylfurfural (5-HMF). It delivers a high catalytic performance with 99.0% 5-HMF conversion in 30 min and a 2, 5-dimethylfuran (DMF) yield of 98.1% in 90 min at a low reaction temperature of 160 °C, as well as good recyclability. These results place Pt1/Ni3Fe IMC among the most active catalysts for the 5-HMF hydrodeoxygenation reaction reported to date. Rational control experiments and first-principles calculations confirm that Pt1/Ni3Fe IMC can readily facilitate the hydrodeoxygenation reaction by a tandem mechanism, where the single Pt site accounts for C=O group hydrogenation and the Ni3Fe interface promotes the C–OH bond cleavage. This interfacial tandem catalysis over the Pt single-atom site and Ni3Fe IMC support may develop new opportunities for the rational structural design of SACs applied in other heterogeneous tandem reactions.
ISSN:2041-6520
2041-6539
DOI:10.1039/d0sc05983h