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Title: Ternary Palladium–Boron–Phosphorus Alloy Mesoporous Nanospheres for Highly Efficient Electrocatalysis

Abstract

Alloying palladium (Pd) catalysts with various metalloid and nonmetal elements can improve their catalytic performance in different chemical reactions. However, current nanosynthesis methods can only generate Pd alloys containing one metalloid or nonmetal, which limits the types of element combinations that may be used to improve Pd-based nanocatalysts. Here, we report a simple soft-templating synthetic strategy to co-alloy Pd with the metalloid boron (B) and the nonmetal phosphorus (P) to generate ternary PdBP mesoporous nanospheres (MSs) with three-dimensional dendritic frameworks. We use a one-step aqueous synthesis method where dimethylamine borane and sodium hypophosphite serve as the B and P sources, respectively, as well as the co-reducing agents to drive the nucleation and growth of ternary PdBP alloy on a sacrificial dioctadecyldimethylammonium chloride template. The concentration of metalloid to nonmetal and the diameters of dendritic MSs can be tailored. The synthetic protocol is also extended to other multicomponent PdMBP alloy MSs to generate different types of dendritic mesoporous frameworks. Boron and phosphorus are known to accelerate the kinetics of the electrochemical oxygen reduction reaction (ORR) and alcohol oxidation reactions (AORs), because their alloys promote the decomposition of oxygen-containing intermediates on Pd surfaces. The dendritic mesoporous morphology of the ternary PdBP MSsmore » also accelerates electron/mass transfer and exposes numerous active sites, enabling better performance in the ORR and AORs. Extending the surfactant-templating synthetic route to multiple types of elements will enable the generation of libraries of multicomponent metal–metalloid-nonmetal alloy nanostructures with functions that are suitable for various targeted applications.« less

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]
  1. Nanjing Normal Univ. (China)
  2. Qingdao Univ. of Science and Technology (China); National Inst. for Materials Science (NIMS), Ibaraki (Japan)
  3. Univ. of Connecticut, Storrs, CT (United States)
  4. Qingdao Univ. of Science and Technology (China); Univ. of Queensland, Brisbane, QLD (Australia); Kyung Hee Univ., Gyeonggi-do (South Korea)
Publication Date:
Research Org.:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division; Natural Science Foundation of Jiangsu Province
OSTI Identifier:
1598220
Grant/Contract Number:  
FG02-86ER13622; BK20180723
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 10; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; metal-metalloid-nonmetal; alloys; mesoporous chemistry; catalytic kinetics; electrocatalysis

Citation Formats

Lv, Hao, Xu, Dongdong, Sun, Lizhi, Henzie, Joel, Suib, Steven L., Yamauchi, Yusuke, and Liu, Ben. Ternary Palladium–Boron–Phosphorus Alloy Mesoporous Nanospheres for Highly Efficient Electrocatalysis. United States: N. p., 2019. Web. doi:10.1021/acsnano.9b06339.
Lv, Hao, Xu, Dongdong, Sun, Lizhi, Henzie, Joel, Suib, Steven L., Yamauchi, Yusuke, & Liu, Ben. Ternary Palladium–Boron–Phosphorus Alloy Mesoporous Nanospheres for Highly Efficient Electrocatalysis. United States. https://doi.org/10.1021/acsnano.9b06339
Lv, Hao, Xu, Dongdong, Sun, Lizhi, Henzie, Joel, Suib, Steven L., Yamauchi, Yusuke, and Liu, Ben. Thu . "Ternary Palladium–Boron–Phosphorus Alloy Mesoporous Nanospheres for Highly Efficient Electrocatalysis". United States. https://doi.org/10.1021/acsnano.9b06339. https://www.osti.gov/servlets/purl/1598220.
@article{osti_1598220,
title = {Ternary Palladium–Boron–Phosphorus Alloy Mesoporous Nanospheres for Highly Efficient Electrocatalysis},
author = {Lv, Hao and Xu, Dongdong and Sun, Lizhi and Henzie, Joel and Suib, Steven L. and Yamauchi, Yusuke and Liu, Ben},
abstractNote = {Alloying palladium (Pd) catalysts with various metalloid and nonmetal elements can improve their catalytic performance in different chemical reactions. However, current nanosynthesis methods can only generate Pd alloys containing one metalloid or nonmetal, which limits the types of element combinations that may be used to improve Pd-based nanocatalysts. Here, we report a simple soft-templating synthetic strategy to co-alloy Pd with the metalloid boron (B) and the nonmetal phosphorus (P) to generate ternary PdBP mesoporous nanospheres (MSs) with three-dimensional dendritic frameworks. We use a one-step aqueous synthesis method where dimethylamine borane and sodium hypophosphite serve as the B and P sources, respectively, as well as the co-reducing agents to drive the nucleation and growth of ternary PdBP alloy on a sacrificial dioctadecyldimethylammonium chloride template. The concentration of metalloid to nonmetal and the diameters of dendritic MSs can be tailored. The synthetic protocol is also extended to other multicomponent PdMBP alloy MSs to generate different types of dendritic mesoporous frameworks. Boron and phosphorus are known to accelerate the kinetics of the electrochemical oxygen reduction reaction (ORR) and alcohol oxidation reactions (AORs), because their alloys promote the decomposition of oxygen-containing intermediates on Pd surfaces. The dendritic mesoporous morphology of the ternary PdBP MSs also accelerates electron/mass transfer and exposes numerous active sites, enabling better performance in the ORR and AORs. Extending the surfactant-templating synthetic route to multiple types of elements will enable the generation of libraries of multicomponent metal–metalloid-nonmetal alloy nanostructures with functions that are suitable for various targeted applications.},
doi = {10.1021/acsnano.9b06339},
url = {https://www.osti.gov/biblio/1598220}, journal = {ACS Nano},
issn = {1936-0851},
number = 10,
volume = 13,
place = {United States},
year = {2019},
month = {9}
}

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