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

Abstract

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:
; ; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1548781
Alternate Identifier(s):
OSTI ID: 1425055
Report Number(s):
BNL-200056-2018-JAAM
Journal ID: ISSN 2451-9294; S245192941830024X; PII: S245192941830024X
Grant/Contract Number:  
SC0012704
Resource Type:
Published Article
Journal Name:
Chem
Additional Journal Information:
Journal Name: Chem Journal Volume: 4 Journal Issue: 2; Journal ID: ISSN 2451-9294
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
29 ENERGY PLANNING, POLICY AND ECONOMY; Pd3Pb Tripods; ORR; Coupled s-p-d Exchange

Citation Formats

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 Pd3Pb Tripods Enhances Oxygen Reduction Catalysis. United States: N. p., 2018. Web. doi:10.1016/j.chempr.2018.01.002.
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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 Pd3Pb Tripods Enhances Oxygen Reduction Catalysis. United States. https://doi.org/10.1016/j.chempr.2018.01.002
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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. Thu . "Coupled s-p-d Exchange in Facet-Controlled Pd3Pb Tripods Enhances Oxygen Reduction Catalysis". United States. https://doi.org/10.1016/j.chempr.2018.01.002.
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@article{osti_1548781,
title = {Coupled s-p-d Exchange in Facet-Controlled Pd3Pb 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}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.chempr.2018.01.002
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Cited by: 11 works
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Figures / Tables:

Figure 1 Figure 1: Morphological and Structural Characterizations of Pd-Pb TPs. (A) TEM image, (B) PXRD pattern, (C) STEM-EELS elemental mappings, (D) reconstructed 3D tomograms along [110] zone axis, (E) atomic model along [110] zone axis, (F) 3D illustration along <100> zone axis, and cross-sectinoal reconstructed planes and corresponding atomic models ofmore » (G, I) the <100> fork and (H, J) <111> fork of the Pd3Pb TPs. See also Figures S1-S9 and Videos S1-S2.« less
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