Coupled s-p-d Exchange in Facet-Controlled Pd 3 Pb 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 Pd 3 Pb Tripods Enhances Oxygen Reduction Catalysis

Journal Article · 01 February 2018 · Chem

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

Bu, Lingzheng ^[1]; Shao, Qi ^[1]; Pi, Yecan ^[1]; Yao, Jianlin ^[1]; Luo, Mingchuan ^[2]; Lang, Jianping ^[1]; Hwang, Sooyeon ^[3]; Xin, Huolin ^[3]; Huang, Bolong ^[4]; Guo, Jun ^[1]; Su, Dong ^[3]; Guo, Shaojun ^[2]; Huang, Xiaoqing ^[1]

Soochow Univ., Jiangsu (China)
Peking Univ., Beijing (China)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Hong Kong Polytechnic Univ. (China)

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 Laboratory (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

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

Publisher:: Cell Press, ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 88 works

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