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.

doi:10.1039/c9nr09759g

Title: Intermetallic Pd₃Pb nanocubes with high selectivity for the 4-electron oxygen reduction reaction pathway

Journal Article · Tue Jan 14 00:00:00 EST 2020 · Nanoscale

DOI:https://doi.org/10.1039/c9nr09759g· OSTI ID:1659426

Gamler, Jocelyn T. L. ^[1];

^[2]; Ashberry, Hannah M. ^[1];

^[3]; Bueno, Sandra L. A. ^[1];

^[4];

^[2];

^[1]

Indiana Univ., Bloomington, IN (United States)
Univ. of Texas, Austin, TX (United States)
Indiana Univ., Bloomington, IN (United States); Nanjing Normal Univ. (China)
Nanjing Normal Univ. (China)

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 mg_Pd^–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.

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Research Organization:: Indiana Univ., Bloomington, IN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Welch Foundation; Texas Advanced Computing Center; National Natural Science Foundation of China (NSFC); China Scholarship Council (CSC)

Grant/Contract Number:: SC0018961; 201806860028

OSTI ID:: 1659426

Alternate ID(s):: OSTI ID: 1582679

Journal Information:: Nanoscale, Vol. 12, Issue 4; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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Title: Intermetallic Pd₃Pb nanocubes with high selectivity for the 4-electron oxygen reduction reaction pathway