Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 10, Issue 44, Pages 38015-38023Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b11764
Keywords
oxygen reduction reaction; intermetallic; atomic ordering; Pt skin; oxygen adsorption energy
Funding
- National Natural Science Foundation of China [21776092, 91534202, 91534122]
- Social Development Program of Shanghai [17DZ1200900]
- Innovation Program of Shanghai Municipal Education Commission
- Fundamental Research Funds for the Central Universities [222201718002]
- Shanghai Scientific and Technological Innovation Project [18JC1410600]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
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Constructing Pt skin on intermetallics has been confirmed as an efficient strategy to boost oxygen reduction reaction (ORR) kinetics. However, there still lacks a systematic study on revealing the influence of low-Pt-content intermetallic substrates (L1(2)-PtM3). In this paper, Pt skin encapsulated low-Pt-mole-fraction L1(2) Cu3Pt has been constructed (denoted as Pt-o-Cu3Pt/C) and compared with its disordered analogue (denoted as Pt-d-Cu3Pt/C). The L1(2) substrate shows a contracted lattice structure and provides Pt-o-Cu3Pt/C with an excellent specific activity of 1.73 mA cm(-2), which is 1.4- and 8.4-fold higher than that of Pt-d-Cu3Pt/C and commercial Pt/C, respectively. Density functional theory calculations reveal that this superior performance is attributed to the more favorable oxygen adsorption energy of surface Pt atoms. Furthermore, the lower formation energy of L1(2) Cu3Pt combined with the enhanced antioxygenation of Pt provide Pt-o-Cu3Pt/C with a superior durability, showing only a 12.5% loss in mass activity after 5000 potential cycles. Therefore, it is suggested that L1(2) atomic ordered structure with a low Pt fraction is a promising substrate for building high-performance Pt-skin catalysts for ORR.
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