Journal
CHEMSUSCHEM
Volume 9, Issue 20, Pages 2922-2927Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201601081
Keywords
electrochemical dealloying; hydrogen absorption; hydrogen evolution reaction; nanoparticles; platinum-free catalyst
Funding
- Department of Science and Technology (DST) [SB/FT/CS-07/2011]
- Sheikh Saqr Laboratory
- Jawaharlal Nehru Centre for Advanced Scientific Research (JNCASR)
- Council of Scientific and Industrial Research
- JNCASR
- DST
- DST [SR/S2/RJN-24/2010]
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Manipulating the d-band center of the metal surface and hence optimizing the free energy of hydrogen adsorption (G(H)) close to the optimal adsorption energy (G(H)=0) for hydrogen evolution reaction (HER), is an efficient strategy to enhance the activity for HER. Herein, we report a oleylamine-mediated (acting as the solvent, stabilizer, and reducing agent) strategy to synthesize intermetallic PdCu3 nanoparticles (NPs) without using any external reducing agent. Upon electrochemical cycling, PdCu3 transforms into Pd-rich PdCu (G(H)=0.05eV), exhibiting remarkably enhanced activity (with a current density of 25mAcm(-2) at approximate to 69mV overpotential) as an alternative to Pt for HER. The first-principle calculation suggests that formation of low coordination number Pd active sites alters the d-band center and hence optimal adsorption of hydrogen, leading to enhanced activity. This finding may provide guidelines towards the design and development of Pt-free highly active and robust electrocatalysts.
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