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Title: Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties

Abstract

Delicately engineering well-defined noble metal aerogels with favorable structural and compositional features is of vital importance for wide applications. Here, we reported a one-pot and facile method for synthesizing core–shell PdPb@Pd hydrogels/aerogels with multiply-twinned grains and an ordered intermetallic phase using sodium hypophosphite as a multifunctional reducing agent. Due to the accelerated gelation kinetics induced by increased reaction temperature and the specific function of sodium hypophosphite, the formation of hydrogels can be completed within 4 h. As a result, owing to their unique porous structure and favorable geometric and electronic effects, the optimized PdPb@Pd aerogels exhibit enhanced electrochemical performance towards ethylene glycol oxidation with a mass activity of 5.8 times higher than Pd black.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2];  [2];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [2]
  1. Washington State Univ., Pullman, WA (United States); Central China Normal Univ., Wuhan (People's Republic of China)
  2. Washington State Univ., Pullman, WA (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1433968
Alternate Identifier(s):
OSTI ID: 1434119
Report Number(s):
BNL-203501-2018-JAAM
Journal ID: ISSN 2050-7488; JMCAET; TRN: US1802396
Grant/Contract Number:  
SC0012704; AC05-76RL01830.
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Materials Chemistry. A
Additional Journal Information:
Journal Volume: 6; Journal Issue: 17; Journal ID: ISSN 2050-7488
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Electrocatalysis; Aerogel; Nanostructure; PdPb@Pd

Citation Formats

Zhu, Chengzhou, Shi, Qiurong, Fu, Shaofang, Song, Junhua, Du, Dan, Su, Dong, Engelhard, Mark H., and Lin, Yuehe. Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties. United States: N. p., 2018. Web. doi:10.1039/C7TA11233E.
Zhu, Chengzhou, Shi, Qiurong, Fu, Shaofang, Song, Junhua, Du, Dan, Su, Dong, Engelhard, Mark H., & Lin, Yuehe. Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties. United States. https://doi.org/10.1039/C7TA11233E
Zhu, Chengzhou, Shi, Qiurong, Fu, Shaofang, Song, Junhua, Du, Dan, Su, Dong, Engelhard, Mark H., and Lin, Yuehe. Wed . "Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties". United States. https://doi.org/10.1039/C7TA11233E. https://www.osti.gov/servlets/purl/1433968.
@article{osti_1433968,
title = {Core–shell PdPb@Pd aerogels with multiply-twinned intermetallic nanostructures: facile synthesis with accelerated gelation kinetics and their enhanced electrocatalytic properties},
author = {Zhu, Chengzhou and Shi, Qiurong and Fu, Shaofang and Song, Junhua and Du, Dan and Su, Dong and Engelhard, Mark H. and Lin, Yuehe},
abstractNote = {Delicately engineering well-defined noble metal aerogels with favorable structural and compositional features is of vital importance for wide applications. Here, we reported a one-pot and facile method for synthesizing core–shell PdPb@Pd hydrogels/aerogels with multiply-twinned grains and an ordered intermetallic phase using sodium hypophosphite as a multifunctional reducing agent. Due to the accelerated gelation kinetics induced by increased reaction temperature and the specific function of sodium hypophosphite, the formation of hydrogels can be completed within 4 h. As a result, owing to their unique porous structure and favorable geometric and electronic effects, the optimized PdPb@Pd aerogels exhibit enhanced electrochemical performance towards ethylene glycol oxidation with a mass activity of 5.8 times higher than Pd black.},
doi = {10.1039/C7TA11233E},
journal = {Journal of Materials Chemistry. A},
number = 17,
volume = 6,
place = {United States},
year = {Wed Apr 04 00:00:00 EDT 2018},
month = {Wed Apr 04 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
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Citation Metrics:
Cited by: 49 works
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Figures / Tables:

Fig. 1 Fig. 1: (a) Schematic illustration of the synthesis of multiply-twinned PdPb@Pd aerogels. Digital pictures of the multiply-twinned Pd3Pb1@Pd hydrogels (b) and the resultant aerogels (Inset in (c)). SEM (c) and TEM (d, e) images of multiply-twinned Pd3Pb1@Pd aerogels. Inset in (d) shows a SAED pattern.

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Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.