Facet effect of Pt nanocrystals on catalytical properties toward glycerol oxidation reaction

Zhou, Jian; Hu, Junhui; Zhang, Xueqiong; Li, Jiefei; Jiang, Kunhong; Liu, Yajun; Zhao, Guohui; Wang, Xiaojing; Chu, Haibin

doi:10.1016/j.jcat.2019.11.019

Cited by 32 publications

(22 citation statements)

References 49 publications

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“…Hence, the almost same reaction orders of both GLY and O 2 and the nearly unchanged activation energies of these catalysts for either Route I or II indicate that the reaction proceeds in the same kinetics regime under the experimental conditions, and furthermore the same reaction mechanism within Pt particle size range of 1.5–2.5 nm. Moreover, the Pt dispersion was determined to be 50.4%, 47.1%, and 37.3%, and the corresponding TOF GLYD&GLYA (395.9, 655.3, and 917.7 h −1 ) and TOF DHA (74.8, 100.2, and 169.5 h −1 ) at 60°C were calculated and following the trend of the number of Pt(100) site in Figure 1(D), consistent with previous study of Pt(100) site as the main active site for this reaction 8 …”

Section: Resultssupporting

confidence: 89%

“…Glycerol (GLY) has been regarded as a versatile biomass‐derived “platform” feedstock for the production of commodity chemicals 1–3 . So far, various transformations have been envisaged for glycerol conversion, including hydrogenolysis, oxidation, dehydration, cyclization, halogenation, and pyrolysis, among which the selective oxidation of glycerol has aroused wide interests to produce the high value‐added products 4–8 . Although the two terminal (primary) hydroxyl groups within glycerol are more reactive to produce glyceraldehyde (GLYD) and glyceric acid (GLYA), the secondary hydroxyl is more preferred to be oxidized to produce dihydroxyacetone (DHA) as shown in Figure 1(A), serving as important roles in cosmetics and fine chemical industries 9,10 .…”

Section: Introductionmentioning

confidence: 99%

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Kinetics decoupling activity and selectivity of Pt nanocatalyst for enhanced glycerol oxidation performance

et al. 2021

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Herein, we demonstrate a kinetics and a mechanistic strategy to disentangle the origins of the significantly improved activity and selectivity of Pt‐catalyzed glycerol oxidation. The unchanged reactant reaction orders and activation energies suggest the same kinetics despite variable Pt particle sizes, based on which a Michaelis–Menten kinetics treatment is conducted to individually quantify the number and activity of Pt active site. Together with multiple characterization results, the volcano‐shaped activity is mainly arising from the quantity change of Pt active site. Moreover, the atomic structure of bimetallic Pt─Sb catalyst is well elucidated by the formation of Pt─SbO interface along with partial Sb incorporation into Pt lattice, chelating with glycerol to poison Pt active sites for primary hydroxyl activation while creating interfacial site for second hydroxyl activation, further evidenced by kinetics shift. The kinetics strategy could be extended to other metal catalysts with simultaneously high activity and selectivity.

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Section: Resultssupporting

confidence: 89%

Section: Introductionmentioning

confidence: 99%

Kinetics decoupling activity and selectivity of Pt nanocatalyst for enhanced glycerol oxidation performance

et al. 2021

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“…The concentrations of the glucose and the oxidation products were analyzed by the external calibration method. 29…”

Section: Methodsmentioning

confidence: 99%

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

Yao

et al. 2022

Catal. Sci. Technol.

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“…Compared with the Mn 2 O 3 -O and Mn 2 O 3 -T catalysts, the Mn 2 O 3 -C catalyst displays the lowest activation energy for the oxidation of these three substrates (E a 1 : 103. 6 the substrate can be oxidized. This suggests that although the oxidation of glycerol over the Mn 2 O 3 -C catalyst could easily occur (E a 1 ), the as-formed GLYA could be further rapidly oxidized to GLYOA (E a 2 ), and even the GLYOA product could also be easily oxidized into other C1 products (E a 3 ).…”

Section: Introductionmentioning

confidence: 99%

Tailoring Facets of α-Mn₂O₃ Microcrystalline Catalysts for Enhanced Selective Oxidation of Glycerol to Glycolic Acid

et al. 2021

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Understanding and tuning the crystal-facet-dependent catalytic properties of catalysts are of great importance for the selective oxidation of polyols. Herein, a series of α-Mn2O3 catalysts with various morphologies (octahedron, truncated octahedron, and cube) are successfully synthesized for the enhanced selective oxidation of glycerol to glycolic acid. Our results show that the different catalytic performances of Mn2O3 catalysts with various morphologies originated from the chemical nature of the (001) and (111) facets. Multicharacterizations and density functional theory calculations revealed that the surface oxygen vacancies on the (001) facets are well correlated with the catalytic activity, and the C–H bond in oxygen-containing intermediates could be easily activated on the surface oxygen vacancies of the (001) facets, thus improving the catalytic activity. Moreover, the main role of (111) facets is to prevent the over-oxidation of glycolic acid products, leading to the improvement of glycolic acid selectivity. Consequently, the Mn2O3-truncated octahedron catalyst with both (001) and (111) facets shows high catalytic activity (0.87 mmol/(h m2)) and glycolic acid selectivity (52.6%) simultaneously. We anticipate that this work could give some suggestions for the design of highly efficient inexpensive catalysts in the glycerol oxidation system.

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Facet effect of Pt nanocrystals on catalytical properties toward glycerol oxidation reaction

Cited by 32 publications

References 49 publications

Kinetics decoupling activity and selectivity of Pt nanocatalyst for enhanced glycerol oxidation performance

Kinetics decoupling activity and selectivity of Pt nanocatalyst for enhanced glycerol oxidation performance

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

Tailoring Facets of α-Mn₂O₃ Microcrystalline Catalysts for Enhanced Selective Oxidation of Glycerol to Glycolic Acid

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Facet effect of Pt nanocrystals on catalytical properties toward glycerol oxidation reaction

Cited by 32 publications

References 49 publications

Kinetics decoupling activity and selectivity of Pt nanocatalyst for enhanced glycerol oxidation performance

Kinetics decoupling activity and selectivity of Pt nanocatalyst for enhanced glycerol oxidation performance

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

Tailoring Facets of α-Mn2O3 Microcrystalline Catalysts for Enhanced Selective Oxidation of Glycerol to Glycolic Acid

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Product

Resources

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

Tailoring Facets of α-Mn₂O₃ Microcrystalline Catalysts for Enhanced Selective Oxidation of Glycerol to Glycolic Acid