Novel route of synthesis of ultra-small Au nanoparticles on SiO2 supports

Y. Kotolevich, O. Martynyuk, S. Martínez-González, H. Tiznado, A. Pestryakov, M. Avalos Borja, V. Cortés Corberán, N. Bogdanchikova

Research output: Contribution to journalArticle

Abstract

A novel route to prepare monodispersed 1–2 nm gold nanoparticles (NPs), based on the use of extremely small SiO2 NPs (2–4 nm) as a support and increasing their metal-support interaction with surface modifier oxides is presented. The influence of modifier (La, Ce and Fe oxides) and modification method (impregnation (i) or direct synthesis (s)) on the formation of ultra-small Au NPs and their structural and electronic properties was studied. The samples were characterized by N2 adsorption (BET), FTIR of adsorbed CO, XRD and HR-TEM methods, and tested for the catalytic selective oxidation of 1-octanol. Preparation of monodispersed Au NPs with 1 nm diameter was successfully achieved for all the modified samples studied, with exception of Au/Ce/SiO2-i, where CeO2 was not homogeneously distributed. The Au NPs have high degree of monodispersity and are stable when treated in H2 up to 300 °C. Formation of these Au NPs depended on the strong interactions between the cationic gold complex precursor and the surface of modified SiO2 NPs. Modifiers changed electronic properties of supported gold; favoring the formation and stabilization of Auδ+ states, which are probable gold active sites of selective liquid-phase oxidation of alcohols in redox catalytic processes. 1-octanol oxidation was used as a model reaction for oxidation of fatty alcohols obtained during biomass transformation. The best performance for 1-octanol oxidation was found for gold nanoparticles supported on the ultra-small SiO2 modified cerium oxide by impregnation method. The relative order of activity was: AuCeSiO2-i > AuFeSiO2-i ≫ AuLaSiO2-i ≈ AuLaSiO2-s > AuSiO2 > AuFeSiO2-s≫ AuCeSiO2-s. The obtained results open the possibility of further development of high-performance catalysts for conversion of secondary products of biomass processing into valuable chemicals.

LanguageEnglish
Pages589-597
Number of pages9
JournalFuel
Volume236
DOIs
Publication statusPublished - 15 Jan 2019

Fingerprint

Nanoparticles
Gold
1-Octanol
Oxidation
Impregnation
Electronic properties
Oxides
Biomass
Fatty Alcohols
Cerium
Carbon Monoxide
Structural properties
Alcohols
Stabilization
Metals
Transmission electron microscopy
Adsorption
Catalysts
Liquids
Processing

Keywords

  • 1-Octanol oxidation
  • 1 nm gold nanoparticles
  • Gold electronic states
  • Metal nanoparticles synthesis
  • Ultra-small silica

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Fuel Technology
  • Energy Engineering and Power Technology
  • Organic Chemistry

Cite this

Kotolevich, Y., Martynyuk, O., Martínez-González, S., Tiznado, H., Pestryakov, A., Avalos Borja, M., ... Bogdanchikova, N. (2019). Novel route of synthesis of ultra-small Au nanoparticles on SiO2 supports. Fuel, 236, 589-597. https://doi.org/10.1016/j.fuel.2018.09.050

Novel route of synthesis of ultra-small Au nanoparticles on SiO2 supports. / Kotolevich, Y.; Martynyuk, O.; Martínez-González, S.; Tiznado, H.; Pestryakov, A.; Avalos Borja, M.; Cortés Corberán, V.; Bogdanchikova, N.

In: Fuel, Vol. 236, 15.01.2019, p. 589-597.

Research output: Contribution to journalArticle

Kotolevich, Y, Martynyuk, O, Martínez-González, S, Tiznado, H, Pestryakov, A, Avalos Borja, M, Cortés Corberán, V & Bogdanchikova, N 2019, 'Novel route of synthesis of ultra-small Au nanoparticles on SiO2 supports' Fuel, vol. 236, pp. 589-597. https://doi.org/10.1016/j.fuel.2018.09.050
Kotolevich Y, Martynyuk O, Martínez-González S, Tiznado H, Pestryakov A, Avalos Borja M et al. Novel route of synthesis of ultra-small Au nanoparticles on SiO2 supports. Fuel. 2019 Jan 15;236:589-597. https://doi.org/10.1016/j.fuel.2018.09.050
Kotolevich, Y. ; Martynyuk, O. ; Martínez-González, S. ; Tiznado, H. ; Pestryakov, A. ; Avalos Borja, M. ; Cortés Corberán, V. ; Bogdanchikova, N. / Novel route of synthesis of ultra-small Au nanoparticles on SiO2 supports. In: Fuel. 2019 ; Vol. 236. pp. 589-597.
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abstract = "A novel route to prepare monodispersed 1–2 nm gold nanoparticles (NPs), based on the use of extremely small SiO2 NPs (2–4 nm) as a support and increasing their metal-support interaction with surface modifier oxides is presented. The influence of modifier (La, Ce and Fe oxides) and modification method (impregnation (i) or direct synthesis (s)) on the formation of ultra-small Au NPs and their structural and electronic properties was studied. The samples were characterized by N2 adsorption (BET), FTIR of adsorbed CO, XRD and HR-TEM methods, and tested for the catalytic selective oxidation of 1-octanol. Preparation of monodispersed Au NPs with 1 nm diameter was successfully achieved for all the modified samples studied, with exception of Au/Ce/SiO2-i, where CeO2 was not homogeneously distributed. The Au NPs have high degree of monodispersity and are stable when treated in H2 up to 300 °C. Formation of these Au NPs depended on the strong interactions between the cationic gold complex precursor and the surface of modified SiO2 NPs. Modifiers changed electronic properties of supported gold; favoring the formation and stabilization of Auδ+ states, which are probable gold active sites of selective liquid-phase oxidation of alcohols in redox catalytic processes. 1-octanol oxidation was used as a model reaction for oxidation of fatty alcohols obtained during biomass transformation. The best performance for 1-octanol oxidation was found for gold nanoparticles supported on the ultra-small SiO2 modified cerium oxide by impregnation method. The relative order of activity was: AuCeSiO2-i > AuFeSiO2-i ≫ AuLaSiO2-i ≈ AuLaSiO2-s > AuSiO2 > AuFeSiO2-s≫ AuCeSiO2-s. The obtained results open the possibility of further development of high-performance catalysts for conversion of secondary products of biomass processing into valuable chemicals.",
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AU - Pestryakov, A.

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N2 - A novel route to prepare monodispersed 1–2 nm gold nanoparticles (NPs), based on the use of extremely small SiO2 NPs (2–4 nm) as a support and increasing their metal-support interaction with surface modifier oxides is presented. The influence of modifier (La, Ce and Fe oxides) and modification method (impregnation (i) or direct synthesis (s)) on the formation of ultra-small Au NPs and their structural and electronic properties was studied. The samples were characterized by N2 adsorption (BET), FTIR of adsorbed CO, XRD and HR-TEM methods, and tested for the catalytic selective oxidation of 1-octanol. Preparation of monodispersed Au NPs with 1 nm diameter was successfully achieved for all the modified samples studied, with exception of Au/Ce/SiO2-i, where CeO2 was not homogeneously distributed. The Au NPs have high degree of monodispersity and are stable when treated in H2 up to 300 °C. Formation of these Au NPs depended on the strong interactions between the cationic gold complex precursor and the surface of modified SiO2 NPs. Modifiers changed electronic properties of supported gold; favoring the formation and stabilization of Auδ+ states, which are probable gold active sites of selective liquid-phase oxidation of alcohols in redox catalytic processes. 1-octanol oxidation was used as a model reaction for oxidation of fatty alcohols obtained during biomass transformation. The best performance for 1-octanol oxidation was found for gold nanoparticles supported on the ultra-small SiO2 modified cerium oxide by impregnation method. The relative order of activity was: AuCeSiO2-i > AuFeSiO2-i ≫ AuLaSiO2-i ≈ AuLaSiO2-s > AuSiO2 > AuFeSiO2-s≫ AuCeSiO2-s. The obtained results open the possibility of further development of high-performance catalysts for conversion of secondary products of biomass processing into valuable chemicals.

AB - A novel route to prepare monodispersed 1–2 nm gold nanoparticles (NPs), based on the use of extremely small SiO2 NPs (2–4 nm) as a support and increasing their metal-support interaction with surface modifier oxides is presented. The influence of modifier (La, Ce and Fe oxides) and modification method (impregnation (i) or direct synthesis (s)) on the formation of ultra-small Au NPs and their structural and electronic properties was studied. The samples were characterized by N2 adsorption (BET), FTIR of adsorbed CO, XRD and HR-TEM methods, and tested for the catalytic selective oxidation of 1-octanol. Preparation of monodispersed Au NPs with 1 nm diameter was successfully achieved for all the modified samples studied, with exception of Au/Ce/SiO2-i, where CeO2 was not homogeneously distributed. The Au NPs have high degree of monodispersity and are stable when treated in H2 up to 300 °C. Formation of these Au NPs depended on the strong interactions between the cationic gold complex precursor and the surface of modified SiO2 NPs. Modifiers changed electronic properties of supported gold; favoring the formation and stabilization of Auδ+ states, which are probable gold active sites of selective liquid-phase oxidation of alcohols in redox catalytic processes. 1-octanol oxidation was used as a model reaction for oxidation of fatty alcohols obtained during biomass transformation. The best performance for 1-octanol oxidation was found for gold nanoparticles supported on the ultra-small SiO2 modified cerium oxide by impregnation method. The relative order of activity was: AuCeSiO2-i > AuFeSiO2-i ≫ AuLaSiO2-i ≈ AuLaSiO2-s > AuSiO2 > AuFeSiO2-s≫ AuCeSiO2-s. The obtained results open the possibility of further development of high-performance catalysts for conversion of secondary products of biomass processing into valuable chemicals.

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