Directed self-assembly pathways of three-dimensional Pt/Pd nanocrystal superlattice electrocatalysts for enhanced methanol oxidation reaction

Directed self-assembly pathways of three-dimensional Pt/Pd nanocrystal superlattice electrocatalysts for enhanced methanol oxidation reaction
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三维Pt/Pd纳米晶超晶格电催化剂的定向自组装途径增强甲醇氧化反应

DOI:
10.1039/c8ta03196g
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发表时间:
2018-07
影响因子:
11.9
通讯作者:
Zhang Jun
Zhang Jun
中科院分区:
材料科学2区
文献类型:
--
作者:
Xu Guangran;Si Rui;Liu Jiayin;Zhang Luyao;Gong Xia;Gao Rui;Liu Baocang;Zhang Jun

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Although considerable interest has been devoted to revealing the formation of vigorous particles, very little is known about the regulating mechanism of these particles being self-assembled into higher-order supercrystals. Herein, we present a robust one-step approach to create three-dimensional (3D) Pt/Pd nanocrystal superlattices (NSLs) via self-assembly of Pt/Pd seeds anchored on polyvinylpyrrolidone chains into 3D networks with the assistance of Pt2+/Pd2+ coordinated N,N-dimethylformamide (DMF) as a bridging backbone linker. The 3D Pt/Pd NSLs are composed of well-defined interior Pt/Pd nanocrystals in a 3D face-centered cubic (fcc) superlattice oriented along the (111), (200) and (220) planes. EXAFS and XPS measurements confirm the strong synergy effect of Pt/Pd in 3D Pt/Pd NSLs due to the rich Pt0 species on the surface, predicting the enhanced electrocatalytic performance. The DFT calculations further reveal that the electrocatalytic enhancement of 3D Pt/Pd NSLs arises from the improved capability of methanol adsorption on metallic Pt active sites enriched by appropriate Pd alloying and surface nitrogen doping during the synthesis. The 3D Pt/Pd NSLs show a high current density of 952 mA mg−1, 4.7 times higher than that of the commercial Pt/C catalyst. The self-assembly pathways may be extended to synthesize other 3D noble metal NSLs with enhanced electrocatalytic performance for direct methanol fuel cells.
原位还原绿色合成石墨烯上Pt-on-Pd双金属纳米枝晶及其增强的甲醇氧化电催化活性
DOI: 10.1016/j.electacta.2014.02.055
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