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This content will become publicly available on February 1, 2019

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

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.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [3] ;  [4] ;  [1] ;  [3] ;  [2] ;  [1]
  1. Soochow Univ., Jiangsu (China)
  2. Peking Univ., Beijing (China)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Hong Kong Polytechnic Univ. (China)
Publication Date:
Report Number(s):
BNL-200056-2018-JAAM
Journal ID: ISSN 2451-9294
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Chem
Additional Journal Information:
Journal Volume: 4; Journal Issue: 2; Journal ID: ISSN 2451-9294
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; Pd3Pb Tripods; ORR; Coupled s-p-d Exchange
OSTI Identifier:
1425055