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Intermetallic Pd3Pb nanocubes with high selectivity for the 4-electron oxygen reduction reaction pathway.
Gamler, Jocelyn T L; Shin, Kihyun; Ashberry, Hannah M; Chen, Yifan; Bueno, Sandra L A; Tang, Yawen; Henkelman, Graeme; Skrabalak, Sara E.
Afiliación
  • Gamler JTL; Department of Chemistry, Indiana University - Bloomington, 800 E. Kirkwood Ave., Bloomington, IN 47405, USA. sskrabal@indiana.edu.
  • Shin K; Department of Chemistry and the Oden Institute for Computational Engineering and Science, The University of Texas at Austin, 105 E. 24th St., Stop A5300, Austin, TX 78712, USA.
  • Ashberry HM; Department of Chemistry, Indiana University - Bloomington, 800 E. Kirkwood Ave., Bloomington, IN 47405, USA. sskrabal@indiana.edu.
  • Chen Y; Department of Chemistry, Indiana University - Bloomington, 800 E. Kirkwood Ave., Bloomington, IN 47405, USA. sskrabal@indiana.edu and Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, School of Chemistry and Materials Science,
  • Bueno SLA; Department of Chemistry, Indiana University - Bloomington, 800 E. Kirkwood Ave., Bloomington, IN 47405, USA. sskrabal@indiana.edu.
  • Tang Y; Jiangsu Key Laboratory of New Power Batteries, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, P. R. China.
  • Henkelman G; Department of Chemistry and the Oden Institute for Computational Engineering and Science, The University of Texas at Austin, 105 E. 24th St., Stop A5300, Austin, TX 78712, USA.
  • Skrabalak SE; Department of Chemistry, Indiana University - Bloomington, 800 E. Kirkwood Ave., Bloomington, IN 47405, USA. sskrabal@indiana.edu.
Nanoscale ; 12(4): 2532-2541, 2020 Jan 28.
Article en En | MEDLINE | ID: mdl-31932821
Pd-Based nanoparticles are excellent alternatives to the typically used Pt-based materials that catalyze fuel cell reactions. Specifically, Pd-based intermetallic nanomaterials have shown great promise as electrocatalysts for the oxygen reduction reaction (ORR) in alkaline media; however, their synthesis remains a challenge and shape-controlled nanoparticles are limited. Here, a low-temperature approach to intermetallic Pd3Pb nanocubes is demonstrated and their electrocatalytic properties evaluated for the ORR. The intermetallic Pd3Pb nanocubes outperformed all reference catalysts, with a mass activity of 154 mA mgPd-1 which is a 130% increase in activity compared to the commercial Pd/C reference and a 230% increase compared to Pd nanocubes. Tafel analysis reveals that the Pd3Pb nanocubes are highly selective for the 4-electron reduction pathway, with minimal HO2- formation. Density functional theory (DFT) calculations show that the increased activity for the intermetallic nanocubes compared to Pd is likely due to the weakening of OH* adsorption, decreasing the required overpotential. These results show that intermetallic Pd3Pb nanocubes are highly efficient for the 4-electron pathway of the ORR and could inspire the study of other shape-controlled intermetallics as catalysts for fuel cell applications.

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nanoscale Año: 2020 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Nanoscale Año: 2020 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Reino Unido