Au-Pd nanoparticles immobilized on TiO2 nanosheet as an active and durable catalyst for solvent-free selective oxidation of benzyl alcohol

Wang, Zhe; Feng, Jiling; Li, Xiaoliang; Oh, Rena; Shi, Daxin; Akdim, Ouardia; Xia, Ming; Zhao, Liang; Huang, Xiaoyang; Zhang, Guojie

doi:10.1016/j.jcis.2020.11.112

Cited by 39 publications

(18 citation statements)

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“…For better comparison, the specific rate per gram of active gold per second was compared with the most reported results ( Table S2 ). The specific rates are 185 and 208 μmol/g/s for AuNi 8 /CNT and AuNi 12 /CNT, which is among the efficient catalysts reported by literature [ 40 , 41 , 42 ]. No matter how, the balance exists between the exposure of Au sites and construction of Au-Ni-O x hybrid structure.…”

Section: Resultsmentioning

confidence: 70%

Nano-Sized NiO Immobilized on Au/CNT for Benzyl Alcohol Oxidation: Influences of Hybrid Structure and Interface

Zhou¹,

Shan²,

Yang³

et al. 2021

Molecules

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Tiny gold nanoparticles were successfully anchored on carbon nanotubes (CNT) with NiO decoration by a two-step synthesis. Characterizations suggested that Ni species in an oxidative state preferred to be highly dispersed on CNT. During the synthesis, in situ reduction by NaBH4 and thermal treatment in oxidation atmosphere were consequently carried out, causing the formation of Au-Ni-Ox interfaces and bimetal hybrid structure depending on the Ni/Au atomic ratios. With an appropriate Ni/Au atomic ratio of 8:1, Ni atoms migrated into the sub-layers of Au particles and induced the lattice contraction of Au particles, whilst a higher Ni/Au atomic ratio led to the accumulation of NiO fractions surrounding Au particles. Both contributed to the well-defined Au-Ni-Ox interface and accelerated reaction rates. Nickel species acted as structure promoters with essential Au-Ni-Ox hybrid structure as well as the active oxygen supplier, accounting for the enhanced activity for benzyl alcohol oxidation. However, the over-layer of unsaturated gold sites easily occured under a high Ni/Au ratio, resulting in a lower reaction rate. With an Au/Ni atomic ratio of 8:1, the specific rate of AuNi8/CNT reached 185 μmol/g/s at only 50 °C in O2 at ordinary pressure.

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Section: Resultsmentioning

confidence: 70%

Nano-Sized NiO Immobilized on Au/CNT for Benzyl Alcohol Oxidation: Influences of Hybrid Structure and Interface

Zhou¹,

Shan²,

Yang³

et al. 2021

Molecules

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“…The comparison of kinetic parameters of BzOH oxidation with PdAu@APTES@SiO 2 microspheres with the similar studies are given in Table 3. Note that, BzOH consumption rate and BzH formation yield obtained with PdAu@APTES@SiO 2 microspheres were considerably higher than those obtained with most of these catalysts [1a,8,14–16] . Only, a slightly better catalytic performance was obtained with the graphene supported AuPd catalyst at 25 °C [7] .…”

Section: Resultsmentioning

confidence: 78%

“…In recent years, the heterogeneous bimetallic catalysts containing Au and Pd nanoparticles as the active sites were synthesized and successfuly used for catalytic oxidation of BzOH [1a,7–8,14–16] . The comparison of kinetic parameters of BzOH oxidation with PdAu@APTES@SiO 2 microspheres with the similar studies are given in Table 3.…”

Section: Resultsmentioning

confidence: 95%

Bimetallic Pd‐Au Nanoparticles Supported Monodisperse Porous Silica Microspheres as an Efficient Heterogenous Catalyst for Fast Oxidation of Benzyl Alcohol

2022

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A bimetallic heterogeneous catalyst in the form of PdAu nanoparticle supported monodisperse‐porous SiO2 microspheres (PdAu@APTES@SiO2) was prepared for fast oxidation of benzyl alcohol (BzOH). The mesoporous support obtained by an originally developed staged‐shape templated hydrolysis‐condensation protocol provided large surface area and high pore volume for parking of noble metal nanoparticles. PdAu@APTES@SiO2 provided higher BzOH conversion, benzaldehyde (BzH) selectivity and BzH formation yield with respect to monometallic catalysts containing Pd or Au nanoparticles supported with SiO2 microspheres. BzOH conversions and BzH formation yields higher than 95 % were obtained in 30 min at 80 °C. The maximum TON and TOF values were determined as 300 and 600 h−1, respectively. BzOH conversions and TOF were also higher with respect to similar catalysts prepared using different supports also carrying PdAu nanoparticles. PdAu@APTES@SiO2 exhibited good stability with a decrease of BzOH conversion less than 2.5 % over five consecutive runs.

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“…As we know, as an important catalyst support, TiO 2 has been widely utilized to immobilize various noble metal single atoms or NPs for a variety of heterogeneous catalytic reactions. − More specifically, surface defective oxygen vacancies on reducible TiO 2 supports can not only tune surface electronic structures , but also stabilize and disperse noble metal NPs or clusters through their anchoring effect. , Previously, Panpranot et al reported a series of selective hydrogenations of acetylene and phenylacetylene over various reducible TiO 2 -supported Pd catalysts. − Especially, they found that calcination and reduction conditions as well as preparation methods could strongly affect the surface defective structures of nano-sized TiO 2 supports, ,,, therefore effectively governing metal–support interactions and the dispersion of Pd NPs. For defective TiO 2 -supported Pd catalysts, however, the real origin of active sites in the selective hydrogenation of phenylacetylene is not still clearly revealed.…”

Section: Introductionmentioning

confidence: 99%

Surface Defect-Induced Site-Specific Dispersion of Pd Nanoclusters on TiO₂ Nanoparticles for Semihydrogenation of Phenyl Acetylene

Liang

Feng

et al. 2021

ACS Appl. Nano Mater.

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Currently, the wide application of heterogeneous noble metal catalysts is greatly limited due to their high cost and scarcity in global reserves. Thus, an effective strategy is to design highly efficient and stable catalysts with low metal loadings. In this work, highly dispersed Pd nanoclusters supported on high-surface-area TiO2 with a large number of defective Ti3+-Ov structures (Ov: oxygen vacancy) were fabricated by our developed hydrogen bubble-assisted approach, which were applied for phenylacetylene semihydrogenation to produce styrene. As-constructed supported Pd catalysts bearing a Pd loading amount of 0.2 wt % afforded a superior catalytic performance to other Pd-based catalysts with higher Pd loading amounts and commercial TiO2-supported counterparts, along with a 99% yield of styrene and a quite high turnover frequency of ∼18,930 h–1 at room temperature and ambient hydrogen pressure. Comprehensive structural characterizations, comparative catalytic experiments, and density functional theory calculations based on a Pd4 cluster model system on a defective TiO2(101) surface emphatically revealed that surface defective structures could greatly facilitate the site-specific dispersion of single Pd atoms or nanoclusters, thereby leading to the formation of electron-rich Pd0 sites favoring the semihydrogenation of phenylacetylene.

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Au-Pd nanoparticles immobilized on TiO2 nanosheet as an active and durable catalyst for solvent-free selective oxidation of benzyl alcohol

Cited by 39 publications

References 50 publications

Nano-Sized NiO Immobilized on Au/CNT for Benzyl Alcohol Oxidation: Influences of Hybrid Structure and Interface

Nano-Sized NiO Immobilized on Au/CNT for Benzyl Alcohol Oxidation: Influences of Hybrid Structure and Interface

Bimetallic Pd‐Au Nanoparticles Supported Monodisperse Porous Silica Microspheres as an Efficient Heterogenous Catalyst for Fast Oxidation of Benzyl Alcohol

Surface Defect-Induced Site-Specific Dispersion of Pd Nanoclusters on TiO₂ Nanoparticles for Semihydrogenation of Phenyl Acetylene

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Au-Pd nanoparticles immobilized on TiO2 nanosheet as an active and durable catalyst for solvent-free selective oxidation of benzyl alcohol

Cited by 39 publications

References 50 publications

Nano-Sized NiO Immobilized on Au/CNT for Benzyl Alcohol Oxidation: Influences of Hybrid Structure and Interface

Nano-Sized NiO Immobilized on Au/CNT for Benzyl Alcohol Oxidation: Influences of Hybrid Structure and Interface

Bimetallic Pd‐Au Nanoparticles Supported Monodisperse Porous Silica Microspheres as an Efficient Heterogenous Catalyst for Fast Oxidation of Benzyl Alcohol

Surface Defect-Induced Site-Specific Dispersion of Pd Nanoclusters on TiO2 Nanoparticles for Semihydrogenation of Phenyl Acetylene

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Surface Defect-Induced Site-Specific Dispersion of Pd Nanoclusters on TiO₂ Nanoparticles for Semihydrogenation of Phenyl Acetylene