Ultrasound-assisted decoration of CuOx nanoclusters on TiO2 nanoparticles for additives free photocatalytic hydrogen production and biomass valorization by selective oxidation

Dimitrios A. Giannakoudakis; Abdul Qayyum; Vaishakh Nair; Ayesha Khan; Swaraj R. Pradhan; Jovana Prekodravac; Kyriazis Rekos; Alec P. LaGrow; Oleksandr Bondarchuk; Dariusz Łomot; Konstantinos S. Triantafyllidis; Juan Carlos Colmenares

doi:10.1016/j.mcat.2021.111664

Ultrasound-assisted decoration of CuO_x nanoclusters on TiO₂ nanoparticles for additives free photocatalytic hydrogen production and biomass valorization by selective oxidation

Dimitrios A. Giannakoudakis^*
, Abdul Qayyum
, Vaishakh Nair
, Ayesha Khan
, Swaraj R. Pradhan
, Jovana Prekodravac
, Kyriazis Rekos
, Alec P. LaGrow
, Oleksandr Bondarchuk
, Dariusz Łomot
, Konstantinos S. Triantafyllidis
, Juan Carlos Colmenares

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

24 Scopus citations

Abstract

The herein presented ultrasound-assisted ultra-wet (US-UWet) impregnation synthetic approach was followed in order to avoid the drawbacks of the conventional wet impregnation synthesis. The goal was to homogeneously decorate the surface of the TiO₂ nanoparticles with nanometric sized (< 4 nm) clusters of mixed cupric and cuprous oxides. The physicochemical features of the nanocomposite (TiO_2[sbnd]CuO_x) were determined by high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM), high-resolution transmission electron microscopy (HR-TEM), energy dispersive X-ray (EDX), X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction (XRD), and Diffuse reflectance (DR) spectroscopy. TiO_2[sbnd]CuO_x showed an enhanced and continuous capability to generate molecular hydrogen upon low power ultraviolet irradiation. The benchmark commercial TiO₂ P25 did not reveal any H₂ formation under these conditions. TiO_2[sbnd]CuO_x presented also a high efficiency for the additives-free selective partial oxidation of two well established biomass derived model platform chemicals/building blocks, 5-hydroxymethylfurfural (HMF) and benzyl alcohol (BnOH) to the value-added chemicals 2,5-diformylfuran (DFF) and benzyl aldehyde (PhCHO), respectively. The nanocomposite showed higher DFF and PhCHO yield compared to P25.

Original language	English
Article number	111664
Journal	Molecular Catalysis
Volume	514
DOIs	https://doi.org/10.1016/j.mcat.2021.111664
State	Published - Sep 2021
Externally published	Yes

Bibliographical note

Publisher Copyright:
© 2021

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Keywords

Benzyl alcohol
Biomass photocatalytic valorization
HMF selective photo-oxidation
Hydrogen generation
Nano-engineered titanium dioxide
Ultrasound assisted synthesis

ASJC Scopus subject areas

Catalysis
Process Chemistry and Technology
Physical and Theoretical Chemistry

Access to Document

10.1016/j.mcat.2021.111664

Cite this

Giannakoudakis, D. A., Qayyum, A., Nair, V., Khan, A., Pradhan, S. R., Prekodravac, J., Rekos, K., LaGrow, A. P., Bondarchuk, O., Łomot, D., Triantafyllidis, K. S., & Colmenares, J. C. (2021). Ultrasound-assisted decoration of CuO_x nanoclusters on TiO₂ nanoparticles for additives free photocatalytic hydrogen production and biomass valorization by selective oxidation. Molecular Catalysis, 514, Article 111664. https://doi.org/10.1016/j.mcat.2021.111664

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title = "Ultrasound-assisted decoration of CuOx nanoclusters on TiO2 nanoparticles for additives free photocatalytic hydrogen production and biomass valorization by selective oxidation",

abstract = "The herein presented ultrasound-assisted ultra-wet (US-UWet) impregnation synthetic approach was followed in order to avoid the drawbacks of the conventional wet impregnation synthesis. The goal was to homogeneously decorate the surface of the TiO2 nanoparticles with nanometric sized (< 4 nm) clusters of mixed cupric and cuprous oxides. The physicochemical features of the nanocomposite (TiO2[sbnd]CuOx) were determined by high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM), high-resolution transmission electron microscopy (HR-TEM), energy dispersive X-ray (EDX), X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction (XRD), and Diffuse reflectance (DR) spectroscopy. TiO2[sbnd]CuOx showed an enhanced and continuous capability to generate molecular hydrogen upon low power ultraviolet irradiation. The benchmark commercial TiO2 P25 did not reveal any H2 formation under these conditions. TiO2[sbnd]CuOx presented also a high efficiency for the additives-free selective partial oxidation of two well established biomass derived model platform chemicals/building blocks, 5-hydroxymethylfurfural (HMF) and benzyl alcohol (BnOH) to the value-added chemicals 2,5-diformylfuran (DFF) and benzyl aldehyde (PhCHO), respectively. The nanocomposite showed higher DFF and PhCHO yield compared to P25.",

keywords = "Benzyl alcohol, Biomass photocatalytic valorization, HMF selective photo-oxidation, Hydrogen generation, Nano-engineered titanium dioxide, Ultrasound assisted synthesis",

author = "Giannakoudakis, \{Dimitrios A.\} and Abdul Qayyum and Vaishakh Nair and Ayesha Khan and Pradhan, \{Swaraj R.\} and Jovana Prekodravac and Kyriazis Rekos and LaGrow, \{Alec P.\} and Oleksandr Bondarchuk and Dariusz {\L}omot and Triantafyllidis, \{Konstantinos S.\} and Colmenares, \{Juan Carlos\}",

note = "Publisher Copyright: {\textcopyright} 2021",

year = "2021",

month = sep,

doi = "10.1016/j.mcat.2021.111664",

language = "English",

volume = "514",

journal = "Molecular Catalysis",

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Giannakoudakis, DA, Qayyum, A, Nair, V, Khan, A, Pradhan, SR, Prekodravac, J, Rekos, K, LaGrow, AP, Bondarchuk, O, Łomot, D, Triantafyllidis, KS & Colmenares, JC 2021, 'Ultrasound-assisted decoration of CuO_x nanoclusters on TiO₂ nanoparticles for additives free photocatalytic hydrogen production and biomass valorization by selective oxidation', Molecular Catalysis, vol. 514, 111664. https://doi.org/10.1016/j.mcat.2021.111664

TY - JOUR

T1 - Ultrasound-assisted decoration of CuOx nanoclusters on TiO2 nanoparticles for additives free photocatalytic hydrogen production and biomass valorization by selective oxidation

AU - Giannakoudakis, Dimitrios A.

AU - Qayyum, Abdul

AU - Nair, Vaishakh

AU - Khan, Ayesha

AU - Pradhan, Swaraj R.

AU - Prekodravac, Jovana

AU - Rekos, Kyriazis

AU - LaGrow, Alec P.

AU - Bondarchuk, Oleksandr

AU - Łomot, Dariusz

AU - Triantafyllidis, Konstantinos S.

AU - Colmenares, Juan Carlos

PY - 2021/9

Y1 - 2021/9

N2 - The herein presented ultrasound-assisted ultra-wet (US-UWet) impregnation synthetic approach was followed in order to avoid the drawbacks of the conventional wet impregnation synthesis. The goal was to homogeneously decorate the surface of the TiO2 nanoparticles with nanometric sized (< 4 nm) clusters of mixed cupric and cuprous oxides. The physicochemical features of the nanocomposite (TiO2[sbnd]CuOx) were determined by high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM), high-resolution transmission electron microscopy (HR-TEM), energy dispersive X-ray (EDX), X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction (XRD), and Diffuse reflectance (DR) spectroscopy. TiO2[sbnd]CuOx showed an enhanced and continuous capability to generate molecular hydrogen upon low power ultraviolet irradiation. The benchmark commercial TiO2 P25 did not reveal any H2 formation under these conditions. TiO2[sbnd]CuOx presented also a high efficiency for the additives-free selective partial oxidation of two well established biomass derived model platform chemicals/building blocks, 5-hydroxymethylfurfural (HMF) and benzyl alcohol (BnOH) to the value-added chemicals 2,5-diformylfuran (DFF) and benzyl aldehyde (PhCHO), respectively. The nanocomposite showed higher DFF and PhCHO yield compared to P25.

AB - The herein presented ultrasound-assisted ultra-wet (US-UWet) impregnation synthetic approach was followed in order to avoid the drawbacks of the conventional wet impregnation synthesis. The goal was to homogeneously decorate the surface of the TiO2 nanoparticles with nanometric sized (< 4 nm) clusters of mixed cupric and cuprous oxides. The physicochemical features of the nanocomposite (TiO2[sbnd]CuOx) were determined by high-angle annular dark-field scanning transmission electron microscope (HAADF-STEM), high-resolution transmission electron microscopy (HR-TEM), energy dispersive X-ray (EDX), X-ray photoelectron spectroscopy (XPS), powder X-ray diffraction (XRD), and Diffuse reflectance (DR) spectroscopy. TiO2[sbnd]CuOx showed an enhanced and continuous capability to generate molecular hydrogen upon low power ultraviolet irradiation. The benchmark commercial TiO2 P25 did not reveal any H2 formation under these conditions. TiO2[sbnd]CuOx presented also a high efficiency for the additives-free selective partial oxidation of two well established biomass derived model platform chemicals/building blocks, 5-hydroxymethylfurfural (HMF) and benzyl alcohol (BnOH) to the value-added chemicals 2,5-diformylfuran (DFF) and benzyl aldehyde (PhCHO), respectively. The nanocomposite showed higher DFF and PhCHO yield compared to P25.

KW - Benzyl alcohol

KW - Biomass photocatalytic valorization

KW - HMF selective photo-oxidation

KW - Hydrogen generation

KW - Nano-engineered titanium dioxide

KW - Ultrasound assisted synthesis

UR - https://www.scopus.com/pages/publications/85107409142

U2 - 10.1016/j.mcat.2021.111664

DO - 10.1016/j.mcat.2021.111664

M3 - Article

AN - SCOPUS:85107409142

SN - 2468-8231

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