Synthetically Tuned Atomic Ordering in PdCu Nanoparticles with Enhanced Catalytic Activity toward Solvent-Free Benzylamine Oxidation
Synthesis of ordered compounds with nano size is of particular interest for tuning the surface properties with enhanced activity and selectivity toward various important industrial catalytic processes. In this work, we synthesized ordered PdCu nanoparticles as highly efficient catalyst for the solve...
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| Vydané v: | ACS applied materials & interfaces Ročník 9; číslo 4; s. 3602 - 3615 |
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| Hlavní autori: | , , , , |
| Médium: | Journal Article |
| Jazyk: | English |
| Vydavateľské údaje: |
United States
01.02.2017
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| Predmet: | |
| ISSN: | 1944-8252 |
| On-line prístup: | Zistit podrobnosti o prístupe |
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| Shrnutí: | Synthesis of ordered compounds with nano size is of particular interest for tuning the surface properties with enhanced activity and selectivity toward various important industrial catalytic processes. In this work, we synthesized ordered PdCu nanoparticles as highly efficient catalyst for the solvent-free aerobic oxidation of benzylamine. The Pd
Cu
catalysts with different chemical compositions (x = 0, 0.25, 0.4, 0.5, 0.6, 0.75, 1) were prepared by polyol method using NaBH
as a reducing agent and were well-characterized by X-ray diffraction (XRD), inductively coupled plasma optical emission spectroscopy, X-ray photoelectron spectroscopy, transmission electron microscopy (TEM) energy-dispersive analysis of X-rays, and X-ray absorption fine structure. The effect of different metal concentrations of Pd and Cu on the formation of Pd
Cu
nanoparticles was investigated. The XRD and TEM confirmed the formation of ordered PdCu intermetallic phase with body-centered cubic (BCC) structure for the synthetic composition of Pd/Cu = 1:1. For compositions x = 0, 0.25, 0.75, and 1, Pd
Cu
alloy with face-centered cubic (FCC) structure was observed, whereas mixed phase of BCC and FCC was observed for x = 0.4 and 0.6. The use of strong reducing agent (NaBH
) was essential to synthesize PdCu ordered phase compared to weak reducing agents such as oleylamine and ascorbic acid. The PdCu nanocatalyst with ordered structure (BCC) showed excellent catalytic activity compared to Pd
Cu
alloy nanoparticles with FCC structure. The atomic ordering in the PdCu intermetallic was the driving force for the enhancement in the catalytic activity with high benzylamine conversion of 94.0% and dibenzylimine selectivity of 92.2% compared to its monometallic and alloy counterparts. Moreover, ordered PdCu alloy showed good recyclability and activity toward the oxidation of different amines. |
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| Bibliografia: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ISSN: | 1944-8252 |
| DOI: | 10.1021/acsami.6b12253 |