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Synthesis and Performance Characterizations of Transition Metal Single Atom Catalyst for Electrochemical CO2 Reduction

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L1₂ Atomic Ordered Substrate Enhanced Pt-Skin Cu₃Pt Catalyst for Efficient Oxygen Reduction Reaction.

Na Cheng¹, Ling Zhang¹, Shuying Mi¹

¹Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering , East China University of Science & Technology , Shanghai 200237 , China.

ACS Applied Materials & Interfaces

|October 27, 2018

Summary

Constructing platinum (Pt) skin on ordered L1₂ Cu₃Pt intermetallics significantly enhances oxygen reduction reaction (ORR) kinetics. This Pt-skin catalyst exhibits superior activity and durability compared to disordered analogues and commercial Pt/C.

Keywords:

Pt skin atomic ordering intermetallic oxygen adsorption energy oxygen reduction reaction

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Area of Science:

Electrochemistry
Materials Science
Catalysis

Background:

Platinum skin on intermetallics is effective for boosting oxygen reduction reaction (ORR) kinetics.
Systematic studies on low-platinum-content intermetallic substrates (L1₂-PtM₃) are lacking.

Purpose of the Study:

To construct and evaluate Pt skin-encapsulated L1₂ Cu₃Pt (Pt-o-Cu₃Pt/C) and compare it with its disordered counterpart (Pt-d-Cu₃Pt/C).
To elucidate the influence of the ordered L1₂ structure on ORR performance.

Main Methods:

Synthesis of Pt skin-encapsulated L1₂ Cu₃Pt and its disordered analogue.
Electrochemical evaluation of ORR activity and durability.
Density functional theory (DFT) calculations to understand performance origins.

Main Results:

Pt-o-Cu₃Pt/C demonstrated a specific activity 1.4-fold higher than Pt-d-Cu₃Pt/C and 8.4-fold higher than commercial Pt/C.
DFT calculations indicated more favorable oxygen adsorption energy on surface Pt atoms in Pt-o-Cu₃Pt/C.
Pt-o-Cu₃Pt/C exhibited superior durability with only a 12.5% mass activity loss after 5000 potential cycles.

Conclusions:

The ordered L1₂ atomic structure of Cu₃Pt provides a contracted lattice and enhances ORR performance.
Low-Pt-content L1₂ intermetallics serve as promising substrates for high-performance Pt-skin catalysts.
The combination of favorable electronic structure and enhanced antioxidation contributes to the catalyst's stability.