Formation of monometallic Au and Pd and bimetallic Au–Pd nanoparticles confined in mesopores via Ar glow-discharge plasma reduction and their catalytic applications in aerobic oxidation of benzyl alcohol

Au–Pd bimetallic nanoparticles confined in SBA-15 are superior to Au and Pd monometallic catalysts for selective benzyl alcohol oxidation. The plasma reduction outperforms the H2 thermal reduction, showing modified morphology and surface chemistry of metal nanoparticles, as well as enhanced catalyti...

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Veröffentlicht in:Journal of catalysis 2012-05, Vol.289, p.105-117
Hauptverfasser: Chen, Yuanting, Wang, Houpeng, Liu, Chang-Jun, Zeng, Zhiyuan, Zhang, Hua, Zhou, Chunmei, Jia, Xinli, Yang, Yanhui
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container_end_page 117
container_issue
container_start_page 105
container_title Journal of catalysis
container_volume 289
creator Chen, Yuanting
Wang, Houpeng
Liu, Chang-Jun
Zeng, Zhiyuan
Zhang, Hua
Zhou, Chunmei
Jia, Xinli
Yang, Yanhui
description Au–Pd bimetallic nanoparticles confined in SBA-15 are superior to Au and Pd monometallic catalysts for selective benzyl alcohol oxidation. The plasma reduction outperforms the H2 thermal reduction, showing modified morphology and surface chemistry of metal nanoparticles, as well as enhanced catalytic performance. Successfully prepared via Ar glow-discharge plasma reduction, Au–Pd bimetallic nanoparticles were highly active in the selective oxidation of benzyl alcohol, showing a rate constant of 0.50h−1, which was 12.5 and 2× that of Au and Pd monometallic catalysts, respectively. Characterization analyses attributed the enhancement in both activity and selectivity to a Pd-rich shell/Au-rich core structure with abundant surface-coordination-unsaturated Pd atoms of those effectively confined and well-dispersed Au–Pd nanoparticles. As a green, efficient, and safe protocol, plasma reduction outperformed conventional H2 thermal reduction due to the different particle nucleation and growth mechanism, which afforded modified morphology and surface chemistry of metal nanoparticles. Further oxidation and re-reduction of plasma-reduced Au–Pd catalyst resulted in the atomic rearrangement of nanoparticles, leading to inferior catalytic performance.
doi_str_mv 10.1016/j.jcat.2012.01.020
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The plasma reduction outperforms the H2 thermal reduction, showing modified morphology and surface chemistry of metal nanoparticles, as well as enhanced catalytic performance. Successfully prepared via Ar glow-discharge plasma reduction, Au–Pd bimetallic nanoparticles were highly active in the selective oxidation of benzyl alcohol, showing a rate constant of 0.50h−1, which was 12.5 and 2× that of Au and Pd monometallic catalysts, respectively. Characterization analyses attributed the enhancement in both activity and selectivity to a Pd-rich shell/Au-rich core structure with abundant surface-coordination-unsaturated Pd atoms of those effectively confined and well-dispersed Au–Pd nanoparticles. As a green, efficient, and safe protocol, plasma reduction outperformed conventional H2 thermal reduction due to the different particle nucleation and growth mechanism, which afforded modified morphology and surface chemistry of metal nanoparticles. Further oxidation and re-reduction of plasma-reduced Au–Pd catalyst resulted in the atomic rearrangement of nanoparticles, leading to inferior catalytic performance.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2012.01.020</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>benzyl alcohol ; Benzyl alcohol oxidation ; Bimetallic nanoparticles ; Catalysis ; Catalysts ; catalytic activity ; Catalytic oxidation ; Chemical reactions ; Chemistry ; Colloidal state and disperse state ; Exact sciences and technology ; General and physical chemistry ; Gold ; hydrogen ; Mesoporous molecular sieve ; Metals ; Nanoparticles ; oxidation ; Palladium ; Physical and chemical studies. Granulometry. Electrokinetic phenomena ; Plasma ; Porous materials ; Theory of reactions, general kinetics. Catalysis. 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The plasma reduction outperforms the H2 thermal reduction, showing modified morphology and surface chemistry of metal nanoparticles, as well as enhanced catalytic performance. Successfully prepared via Ar glow-discharge plasma reduction, Au–Pd bimetallic nanoparticles were highly active in the selective oxidation of benzyl alcohol, showing a rate constant of 0.50h−1, which was 12.5 and 2× that of Au and Pd monometallic catalysts, respectively. Characterization analyses attributed the enhancement in both activity and selectivity to a Pd-rich shell/Au-rich core structure with abundant surface-coordination-unsaturated Pd atoms of those effectively confined and well-dispersed Au–Pd nanoparticles. As a green, efficient, and safe protocol, plasma reduction outperformed conventional H2 thermal reduction due to the different particle nucleation and growth mechanism, which afforded modified morphology and surface chemistry of metal nanoparticles. Further oxidation and re-reduction of plasma-reduced Au–Pd catalyst resulted in the atomic rearrangement of nanoparticles, leading to inferior catalytic performance.</description><subject>benzyl alcohol</subject><subject>Benzyl alcohol oxidation</subject><subject>Bimetallic nanoparticles</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>catalytic activity</subject><subject>Catalytic oxidation</subject><subject>Chemical reactions</subject><subject>Chemistry</subject><subject>Colloidal state and disperse state</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Gold</subject><subject>hydrogen</subject><subject>Mesoporous molecular sieve</subject><subject>Metals</subject><subject>Nanoparticles</subject><subject>oxidation</subject><subject>Palladium</subject><subject>Physical and chemical studies. Granulometry. 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subjects benzyl alcohol
Benzyl alcohol oxidation
Bimetallic nanoparticles
Catalysis
Catalysts
catalytic activity
Catalytic oxidation
Chemical reactions
Chemistry
Colloidal state and disperse state
Exact sciences and technology
General and physical chemistry
Gold
hydrogen
Mesoporous molecular sieve
Metals
Nanoparticles
oxidation
Palladium
Physical and chemical studies. Granulometry. Electrokinetic phenomena
Plasma
Porous materials
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
title Formation of monometallic Au and Pd and bimetallic Au–Pd nanoparticles confined in mesopores via Ar glow-discharge plasma reduction and their catalytic applications in aerobic oxidation of benzyl alcohol
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