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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

Bu, Lingzheng, Shao, Qi, Pi, Yecan, Yao, Jianlin, Luo, Mingchuan, Lang, Jianping, Hwang, Sooyeon, Xin, Huolin, Huang, Bolong, Guo, Jun, Su, Dong, Guo, Shaojun, and Huang, Xiaoqing. Coupled s-p-d Exchange in Facet-Controlled Pd 3 Pb Tripods Enhances Oxygen Reduction Catalysis. United States: N. p., Web. doi:10.1016/j.chempr.2018.01.002.
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. Coupled s-p-d Exchange in Facet-Controlled Pd 3 Pb Tripods Enhances Oxygen Reduction Catalysis. United States. doi:10.1016/j.chempr.2018.01.002.
Bu, Lingzheng, Shao, Qi, Pi, Yecan, Yao, Jianlin, Luo, Mingchuan, Lang, Jianping, Hwang, Sooyeon, Xin, Huolin, Huang, Bolong, Guo, Jun, Su, Dong, Guo, Shaojun, and Huang, Xiaoqing. 2018. "Coupled s-p-d Exchange in Facet-Controlled Pd 3 Pb Tripods Enhances Oxygen Reduction Catalysis". United States. doi:10.1016/j.chempr.2018.01.002.
@article{osti_1425055,
title = {Coupled s-p-d Exchange in Facet-Controlled Pd 3 Pb Tripods Enhances Oxygen Reduction Catalysis},
author = {Bu, Lingzheng and Shao, Qi and Pi, Yecan and Yao, Jianlin and Luo, Mingchuan and Lang, Jianping and Hwang, Sooyeon and Xin, Huolin and Huang, Bolong and Guo, Jun and Su, Dong and Guo, Shaojun and Huang, Xiaoqing},
abstractNote = {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.},
doi = {10.1016/j.chempr.2018.01.002},
journal = {Chem},
number = 2,
volume = 4,
place = {United States},
year = {2018},
month = {2}
}