Gold Nanoparticles Supported on Silica & Titania Hybrid Mesoporous Spheres and Their Catalytic Performance Regulation

doi:10.15541/jim20210261

Abstract

Abstract:

In order to exploit energy sources (like photocatalytic water splitting for hydrogen production) and protect environment (like organics degradation), supported noble metal catalysts have made considerable progress in terms of design, fabrication, and theory. Herein, based on the specific morphology and structure of dendritic mesoporous silica nanospheres (DMSNs), TiO₂ nanoparticles (NPs) were introduced into the channels via Sol-Gel method, developing dendritic mesoporous silica&titania nanospheres (DMSTNs). Then, amino groups (-NH₂) were grafted onto DMSTNs surfaces by organic modification technology. Finally, ultrasmall gold (Au) NPs were anchored onto the as-prepared DMSTNs-NH₂ through impregnation method and sodium borohydride (NaBH₄) reduction. DMSTNs supported Au NPs catalysts could be successfully constructed, as verified by different methods. Under simulated sunlight for splitting water, the amount of produced H₂ by the brand-new catalysts and the corresponding rate are 69.08 µmol·g^-1 and 13.82 µmol·g^-1·h^-1, respectively, roughly. seven times of that of the contrast sample (DMSNs supported Au NPs). Without light irradiation, the apparent kinetic constant of p-nitrophenol reduction by the as-prepared catalysts is 6.540×10^-3s^-1, about 17 times higher than that of the reference (0.372×10^-3 s^-1). ln conclusion, DMSTNs supported Au NPs exhibit good multifunctional catalytic activity.

Key words: dendritic nanospheres, silica&titania hybrid, gold nanoparticles, photocatalytic water splitting for hydrogen production, p-nitrophenol reduction

CLC Number:

TQ127

MA Hui, TAO Jianghui, WANG Yanni, HAN Yu, WANG Yabin, DING Xiuping. Gold Nanoparticles Supported on Silica & Titania Hybrid Mesoporous Spheres and Their Catalytic Performance Regulation[J]. Journal of Inorganic Materials, 2022, 37(4): 404-412.

Figures/Tables 9

Fig. 1 Schematic diagram of constructing DMSNs- and DMSTNs-based supported Au NPs catalysts

Fig. 2 SEM images of DMSNs (a), DMSTNs (b), DMSNs-NH2 (c), DMSTNs-NH2 (d), DMSNs-NH2-Au (e), and DMSTNs-NH2-Au (f)

Fig. 3 FT-IR spectra of DMSNs, DMSTNs, DMSNs-NH2, and DMSTNs-NH2

Fig. 4 XPS survey scan of DMSTNs, DMSNs-NH2, and DMSNs-NH2

Fig.5 TEM images of DMSNs (a), DMSTNs (b), DMSNs-NH2 (c), DMSTNs-NH2 (d), DMSNs-NH2-Au (e), and DMSTNs-NH2-Au (f), and TEM-mapping images of DMSNs-NH2-Au (g) and DMSTNs-NH2-Au (h)

Fig. 6 XRD patterns (a), UV-Vis-DRS spectra (b) and PL spectra (c) of DMSNs, DMSTNs, DMSNs-NH2-Au, and DMSTNs-NH2-Au

Fig. 7 H2 production amount as a function of irradiation time (a) and the corresponding production rates (b) of DMSNs, DMSTNs, DMSNs-NH2-Au, and DMSTNs-NH2-Au, cycling tests of DMSTNs-NH2-Au for H2 production (c), and TEM image of DMSTNs-NH2-Au sample experienced five cycles, with inset showing the high-angle annular dark-field imaging (d)

Fig. 8 Characteristic ultraviolet absorption peaks of p-nitrophenol, p-nitrophenolate, and p-aminophenol (a), Ultraviolet absorption spectra of different samples, including p-nitrophenol+NaBH4 as the blank sample (b), with the addition of DMSNs (c), DMSTNs (d), DMSNs-NH2-Au (e), and DMSTNs-NH2-Au (f), the conversion (g) and pseudo first-order linear equation (h) of DMSNs-NH2-Au, and DMSTNs-NH2-Au, and cycling tests of DMSTNs-NH2-Au for p-nitrophenol reduction (i), SEM images (j) and energy dispersive spectroscopy (EDS) mappings (k) of DMSTNs-NH2-Au sample experienced ten cycles. EDS measurement of random four DMSTNs-NH2-Au individuals (l)

Fig. 9 Schematic illustration of possible photocatalytic mechanisms for DMSTNs-NH2-Au to split water under simulated sunlight (a) and ordinary catalytic reduction of p-nitrophenol without light irritation (b)

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