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- Publisher
- Wiley
- Copyright
- © 2022 Wiley‐VCH GmbH
- ISSN
- 1614-6832
- eISSN
- 1614-6840
- DOI
- 10.1002/aenm.202103505
- Publisher site
- See Article on Publisher Site
Abstract
Abundant surface structural defects can endow electrocatalysts with extraordinary physical and chemical characteristics. Herein, metastable Pd nanoparticles (NPs) with abundant twin boundaries (TBs) and atomic steps (ASs) anchored on a carbon substrate (TS‐Pd/C) are directly synthesized by a solid‐state thermal shock (TS) strategy. Molecular dynamics simulation indicates that the transient super cooling procedure after the TS synthesis can boost the formation of TBs. Benefitting from the abundant TBs and ASs, these metastable Pd NPs can serve as an advanced electrocatalyst for the ethanol oxidation reaction (EOR) with superior reactivity, stability, and CO tolerance in alkaline solutions, which far exceeds that of commercial Pd/C. The first‐principles calculations suggest that the defect structure dominated by TBs can achieve the spatial separation of the optimal adsorption sites for CO and OH. The CO can concentrate at optimal surface sites to minimize the number of poisoned active sites. The strong adsorption of OH can accelerate the EOR process and jointly promote the improvement of electrocatalytic reactivity.
Journal
Advanced Energy Materials – Wiley
Published: Feb 1, 2022
Keywords: electrocatalysis; ethanol oxidation reaction; metastable; palladium; twin boundary