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Title: Surface molecular pump enables ultrahigh catalyst activity
The performance of electrocatalysts is critical for renewable energy technologies. While the electrocatalytic activity can be modulated through structural and compositional engineering following the Sabatier principle, the insufficiently explored catalyst-electrolyte interface is promising to promote microkinetic processes such as physisorption and desorption. By combining experimental designs and molecular dynamics simulations with explicit solvent in high accuracy, we demonstrated that dimethylformamide can work as an effective surface molecular pump to facilitate the entrapment of oxygen and outflux of water. Dimethylformamide disrupts the interfacial network of hydrogen bonds, leading to enhanced activity of the oxygen reduction reaction by a factor of 2 to 3. This strategy works generally for platinum-alloy catalysts, and we introduce an optimal model PtCuNi catalyst with an unprecedented specific activity of 21.8 ± 2.1 mA/cm2at 0.9 V versus the reversible hydrogen electrode, nearly double the previous record, and an ultrahigh mass activity of 10.7 ± 1.1 A/mgPt.  more » « less
Award ID(s):
1931587
PAR ID:
10552705
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ;
Publisher / Repository:
AAAS
Date Published:
Journal Name:
Science Advances
Volume:
10
Issue:
36
ISSN:
2375-2548
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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