Coupled s-p-d Exchange in Facet-Controlled Pd3Pb Tripods Enhances Oxygen Reduction Catalysis

Bu, Lingzheng; Shao, Qi; Pi, Yecan; Yao, Jianlin; Luo, Mingchuan; Lang, Jianping; Hwang, Sooyeon; Xin, Huolin; Huang, Bolong; Guo, Jun; Su, Dong; Guo, Shaojun; Huang, Xiaoqing

doi:10.1016/j.chempr.2018.01.002

Title: Coupled s-p-d Exchange in Facet-Controlled Pd3Pb Tripods Enhances Oxygen Reduction Catalysis

Journal Article · Thu Feb 01 00:00:00 EST 2018 · Chem

DOI:https://doi.org/10.1016/j.chempr.2018.01.002· OSTI ID:1548781

Bu, Lingzheng; Shao, Qi; Pi, Yecan; Yao, Jianlin; Luo, Mingchuan; Lang, Jianping; Hwang, Sooyeon; Xin, Huolin; Huang, Bolong; Guo, Jun; Su, Dong; Guo, Shaojun; Huang, Xiaoqing

Efficient oxygen reduction reaction (ORR) catalysts are the key in developing high-performance fuel cells. Palladium (Pd) is a promising catalyst system for ORR with its potential to replace platinum (Pt), however it usually exhibits lower activity than Pt. Herein, we report a class of ordered Pd3Pb tripods (TPs) with dominated {110} facets that show extremely high ORR performance in alkaline medium. Totally different from the well-known knowledge that excellent ORR activity of Pt catalyst is caused by its partially-filled d-orbital, our first principle calculations suggest that the strong charge exchange between Pd-4d and Pb-(sp) orbitals on Pd3Pb TPs {110} facet results in the Pd-Pb local bonding unit with the orbital configuration similar to Pt. Consequently, the Pd3Pb TPs exhibit much higher ORR activities than commercial Pt/C and commercial Pd/C. The Pd3Pb TPs are rather endurable and sustain over 20,000 potential cycles with negligible structural and compositional changes.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1548781

Alternate ID(s):: OSTI ID: 1425055

Report Number(s):: BNL-200056-2018-JAAM; S245192941830024X; PII: S245192941830024X

Journal Information:: Chem, Journal Name: Chem Vol. 4 Journal Issue: 2; ISSN 2451-9294

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 74 works

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