Effect of CeO<sub>2</sub> morphology on the catalytic properties of Au/CeO<sub>2</sub> for base-free glucose oxidation

Qi, Xingyue; He, Yalin; Yao, Yadong; Zhang, Lu; Li, Yiran; Geng, Meiyu; Wei, Hang; Chu, Haibin

doi:10.1039/d1cy02078a

Cited by 20 publications

(10 citation statements)

References 43 publications

(61 reference statements)

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“…In comparison, a KIE value between 0.7 and 1.5 suggests a secondary kinetic isotope effect, and the isotopically labeled atom is not involved in the RDS . In brief, a smaller KIE value reflects a higher priority in the reaction. − …”

Section: Resultsmentioning

confidence: 99%

Revealing the Crystal Facet Effect of Ceria in Pd/CeO₂ Catalysts toward the Selective Oxidation of Benzyl Alcohol

Zhang

Chen

et al. 2023

ACS Catal.

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Ceria is an excellent catalyst or support for various oxidation reactions due to its abundant oxygen vacancies and strong metal–support interactions. In this study, ceria nanocrystals were hydrothermally prepared with different morphologies (nanorods, nanocubes, and nano-octahedra) and corresponding exposed crystal facets [(110), (100), and (111)]. The Pd/CeO2 catalysts were synthesized through an impregnation method by applying these ceria nanocrystals as supports. Selective oxidation of benzyl alcohol, involving multiple catalytic steps, was employed as a model reaction to explore the crystal facet effect of ceria on the catalytic activity of various Pd/CeO2 catalysts. The Pd/CeO2 nanorod catalyst delivers superior performance in each individual step, resulting in an improved overall catalytic activity. Specifically, the highest oxygen vacancy concentration and the optimum metal–support synergy observed on the CeO2 (110) surface are feasible to dissociate the benzyl alcohol adsorbent, eliminate α-H, and activate O2. As a consequence, the Pd/CeO2-nanorod catalysts deliver a much higher benzyl alcohol conversion (74%) than Pd/CeO2-nano-octahedra (35%) and Pd/CeO2-nanocubes (28%). This work provides in-depth insight into the crystal facet–performance relationship of CeO2 in the selective oxidation of benzyl alcohol and sheds light on the catalyst support design strategy for other multistep reactions.

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Section: Resultsmentioning

confidence: 99%

Revealing the Crystal Facet Effect of Ceria in Pd/CeO₂ Catalysts toward the Selective Oxidation of Benzyl Alcohol

Zhang

Chen

et al. 2023

ACS Catal.

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“…For CeO 2 ‐supported metal catalysts, the morphology effect of CeO 2 support on the metal‐CeO 2 interaction, structure and catalytic performance has been extensively observed on the Au/ CeO 2 , [ 59,120‐124 ] Ag/CeO 2 , [ 94 ] Pt/CeO 2 , [ 95,125‐126 ] Pd/CeO 2 , [ 60,65,127‐129 ] Ru/CeO 2 , [ 61,130‐132 ] and Ni/CeO 2 [ 133‐134 ] catalysts. Zhang et al .…”

Section: Morphology‐dependent Catalysis Of Ceo2‐based Nc Model Catalystsmentioning

confidence: 99%

Morphology‐Dependent Catalysis of CeO₂‐Based Nanocrystal Model Catalysts

et al. 2022

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Comprehensive Summary Recent progress in colloidal synthesis has realized the preparations of uniform nanocrystal (NC) model catalysts with rich and well‐controlled morphologies that were employed to explore structure‐activity relationships of powder catalysts, similar to single‐crystal‐based model catalysts under ultrahigh vacuum conditions but can work at the same conditions as powder catalysts without the “materials gap” and “pressure gap”. In this perspective, the CeO2‐based NC model catalysts with various morphologies are included and their relevant progresses are critically reviewed. The detailed descriptions of morphology‐controlled synthesis and characterizations of uniform CeO2 NCs, and morphology‐dependent catalysis of CeO2‐based NC model catalysts containing pure CeO2 NCs, CeO2‐supported oxide catalysts, and CeO2‐supported metal catalysts, provide us a comprehensive cognition in CeO2‐involved catalytic reactions and also open up a new approach for the fundamental studies of complex heterogeneous catalysis. Finally, a concept of oxide‐based NC model catalysts and outlook of oxide NCs acting not only as model catalysts for the fundamental study but also as the support in tailoring structures and optimizing performance of oxide‐involved catalysts are discussed.

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“…Among the three CeO 2 nanocrystals, CeO 2 NR exhibit the strongest signal, implying that they have the most oxygen defect sites. Notably, the relative amounts of oxygen defect sites for three CeO 2 nanocrystals generally can also be reflected by the ratio of the Raman peak intensity at ∼595 cm –1 (corresponding to the defect-induced (D) mode) to that at ∼461 cm –1 (belonging to the vibration (F 2g ) mode of CeO 2 fluorite phase) Figure F,G shows that the I 595 / I 461 ratios for three CeO 2 nanocrystals rise with the order of CeO 2 NO (0.016), CeO 2 NC (0.021), and CeO 2 NR (0.175), further revealing CeO 2 NR possess more oxygen defect sites than CeO 2 NO and CeO 2 NC.…”

Section: Resultsmentioning

confidence: 99%

Au/CeO₂ NR Restricted Inside Cu-MOFs: A Three-in-One Artificial Enzyme with Synergistically Enhanced Peroxidase-Like Activity for Dual-Mode Sensing of Multiple Biomarkers

Chen

Peng

Lin

et al. 2023

ACS Sustainable Chem. Eng.

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Nanomaterials with inherent enzyme-mimetic properties have been extensively studied in biosensing field, but it is still challenging to overcome their natively weak enzyme-mimetic activity and further promote their stabilities. In this work, a three-in-one artificial enzyme with synergistically enhanced peroxidase-like activity and outstanding stability is constructed by restricting Au-loaded CeO2 nanorods (NR) (1% Au:CeO2 mass ratio) inside Cu-based metal–organic frameworks (Cu(PABA)), termed Au1/CeO2 NR@Cu(PABA). It has been demonstrated that the artificial enzyme possesses significantly improved performance in catalytic decomposition of H2O2, with ∼2.41 and ∼1.49 times higher activity than its individual constituents (Au1/CeO2 NR and Cu(PABA)), benefiting from the synergistic effect and the unique restricted structure; owns strong affinities to substrates, with separately ∼8.21- and ∼3.13-fold lower Michaelis constants toward H2O2 and o-phenylenediamine, respectively, than horseradish peroxidase; and exhibits desirable pH (4–12), thermal (30–80 °C), organic solvent (N,N-dimethylformamide, acetone, methanol, etc.), and long-term storage (30 days) stabilities, advantaging practical applications. Taking aforementioned superior properties of Au1/CeO2 NR@Cu(PABA), a universal colorimetric/fluorometric dual-mode sensing platform is built and utilized for detection of biomarkers (e.g., glucose, galactose, and cholesterol) in biological fluids with satisfactory recoveries (90.2–108%). This work offers new horizons in designing high-efficiency, stable, and credible biomimetic catalysts to accelerate future advanced engineering of nanozymes.

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Effect of CeO₂ morphology on the catalytic properties of Au/CeO₂ for base-free glucose oxidation

Abstract: Catalytic selective oxidation of glucose into value-added gluconic acid is one of the sustainable routes for biomass utilization, for which the supported Au catalysts have been widely explored. Au/CeO2 was...

Cited by 20 publications

References 43 publications

Revealing the Crystal Facet Effect of Ceria in Pd/CeO₂ Catalysts toward the Selective Oxidation of Benzyl Alcohol

Revealing the Crystal Facet Effect of Ceria in Pd/CeO₂ Catalysts toward the Selective Oxidation of Benzyl Alcohol

Morphology‐Dependent Catalysis of CeO₂‐Based Nanocrystal Model Catalysts

Au/CeO₂ NR Restricted Inside Cu-MOFs: A Three-in-One Artificial Enzyme with Synergistically Enhanced Peroxidase-Like Activity for Dual-Mode Sensing of Multiple Biomarkers

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Effect of CeO2 morphology on the catalytic properties of Au/CeO2 for base-free glucose oxidation

Abstract: Catalytic selective oxidation of glucose into value-added gluconic acid is one of the sustainable routes for biomass utilization, for which the supported Au catalysts have been widely explored. Au/CeO2 was...

Cited by 20 publications

References 43 publications

Revealing the Crystal Facet Effect of Ceria in Pd/CeO2 Catalysts toward the Selective Oxidation of Benzyl Alcohol

Revealing the Crystal Facet Effect of Ceria in Pd/CeO2 Catalysts toward the Selective Oxidation of Benzyl Alcohol

Morphology‐Dependent Catalysis of CeO2‐Based Nanocrystal Model Catalysts

Au/CeO2 NR Restricted Inside Cu-MOFs: A Three-in-One Artificial Enzyme with Synergistically Enhanced Peroxidase-Like Activity for Dual-Mode Sensing of Multiple Biomarkers

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Effect of CeO₂ morphology on the catalytic properties of Au/CeO₂ for base-free glucose oxidation

Revealing the Crystal Facet Effect of Ceria in Pd/CeO₂ Catalysts toward the Selective Oxidation of Benzyl Alcohol

Revealing the Crystal Facet Effect of Ceria in Pd/CeO₂ Catalysts toward the Selective Oxidation of Benzyl Alcohol

Morphology‐Dependent Catalysis of CeO₂‐Based Nanocrystal Model Catalysts

Au/CeO₂ NR Restricted Inside Cu-MOFs: A Three-in-One Artificial Enzyme with Synergistically Enhanced Peroxidase-Like Activity for Dual-Mode Sensing of Multiple Biomarkers