Low Temperature Oxidation of Trace Ethylene over Pt Nanoparticles Supported on Hydrophobic Mesoporous Silica

Satter, Shazia Sharmin; Hirayama, Jun; Nakajima, Kiyotaka; Fukuoka, Atsushi

doi:10.1246/cl.180364

Cited by 12 publications

(29 citation statements)

References 12 publications

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“…17,18 TEM measurement of Pt/A380(800) in this study shows that Pt nanoparticles in size of 5.5 nm are highly dispersed on A380(800) surface (FiguresS1(C) and (D)). Structural parameters and catalytic activity for silica-supported Pt catalysts.…”

mentioning

confidence: 53%

“…They showed similar time courses of ethylene oxidation to that of Pt/SBA-15(800) as shown in Figures S2 and S3. 18 Ethylene conversion and CO2 yield became constant apparently in all cases at 300 min. Table 1 summarizes structural parameters and catalytic activities of all catalysts examined.…”

Section: Structure and Catalysis Ofmentioning

confidence: 86%

“…On the other hand, calcination at 800 °C makes SBA-15 hydrophobic, which improves the activity (Pt/SBA-15(800)). 18 It should be noted that the order of these activities (Pt/SBA-15(800) >> Pt/SBA-15 = Pt/A380(800) = Pt/A380) cannot be simply explained with hydrophobic nature of silica supports (Pt/SBA-15(800) = Pt/A380(800) = Pt/A380 >> Pt/SBA-15).…”

Section: Structure and Catalysis Ofmentioning

confidence: 99%

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Water-Resistant Pt Sites in Hydrophobic Mesopores Effective for Low-Temperature Ethylene Oxidation

et al. 2020

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Structure-activity relationship of silica-supported Pt catalysts in aerobic oxidation of 50 ppm ethylene was studied at 0 °C with a fixed-bed flow reactor and in-situ characterization techniques using FTIR (Fourier-transform infrared) spectroscopy. The activity of all Pt catalysts examined here decreased by water molecules formed during stoichiometric oxidation of ethylene and became stable steadily. Mesoporous silica-supported Pt catalyst improved its steady-state activity after calcination of the support in air at 800 °C, whereas no such effect was observed for nonporous silica support. CO-pulse titration, H2O adsorption measurements, 29 Si MAS NMR, and in-situ FTIR along with catalytic activity studies revealed that the activity of mesoporous silica-supported Pt catalyst is higher than that of nonporous silica-supported ones, despite similar hydrophobicity and low Pt dispersion. In-situ characterization using CO as a molecular probe indicates that a part of Pt surface inside hydrophobic mesopores is not involved in hydrogen-bonding network among physisorbed water molecules and surface SiOH groups even after full hydration of catalyst surface, and bare Pt sites are expected to work more effectively for ethylene oxidation. Such "hydrophobic Pt surface" can only be formed on hydrophobic mesoporous silica support, which is probably due to Pt nanoparticles surrounded with hydrophobic siloxane network entirely. Unique environment derived from condensed siloxane network and restricted mesopores contributes largely to high activity of Pt nanoparticles for low temperature oxidation of trace ethylene.

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confidence: 53%

Section: Structure and Catalysis Ofmentioning

confidence: 86%

Section: Structure and Catalysis Ofmentioning

confidence: 99%

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Water-Resistant Pt Sites in Hydrophobic Mesopores Effective for Low-Temperature Ethylene Oxidation

et al. 2020

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“…Although improvements have been made to lower the working temperature, − the removal of trace amounts of ethylene at 0 °C did not progress until the development of a mesoporous silica-supported Pt catalyst (Pt/MCM-41) . This catalyst, as well as the recently developed Pt/SBA-15, , can completely oxidize 50 ppm of ethylene to CO 2 and H 2 O at around 0 °C. Public implementation is ongoing, and these catalysts have already been installed in commercially available refrigerators.…”

Section: Introductionmentioning

confidence: 99%

DFT Mechanistic Study on the Complete Oxidation of Ethylene by the Silica-Supported Pt Catalyst: C═C Activation via the Ethylene Dioxide Intermediate

et al. 2019

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Low-temperature complete oxidation of ethylene by the mesoporous silica-supported Pt catalyst is a forefront technology for food preservation. Public implementations of the Pt catalyst have already begun, and spectroscopy analyses on the catalytic mechanism have been reported. In this study, density functional theory calculations were conducted to clarify the potential energy profile and electronic mechanism of the catalytic reaction. Based on the experimental findings, a reaction pathway was proposed for ethylene oxidation up to CO2 formation via the HCHO intermediate. Among several possibilities, a reaction pathway via ethylene dioxide species is energetically plausible for the C–C bond cleavage to generate HCHO. Particular focus was given to the electronic effect of the silica support in the ethylene dioxide route. The reservoir effect, in which the siloxide groups take electrons from the Pt moiety, reduces the activation energy of the C–C bond cleavage step by taking electrons from the σ(C–C) orbital.

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“…For example, the coke deposited on the surface of the catalyst blocks the active sites, resulting in a rapid deactivation. The formation of formic acid generated as a byproduct in the oxidation of ethylene is considered as the reason for the deactivation of some Pt catalysts. − ,, (III) As shown in Figure , the adsorption of water vapor on ethylene adsorption sites suppresses ethylene adsorption and, thus, decreases the oxidation activity of catalysts with poor water resistance. , …”

Section: Low-temperature Catalytic Oxidationmentioning

confidence: 99%

Elimination or Removal of Ethylene for Fruit and Vegetable Storage via Low-Temperature Catalytic Oxidation

et al. 2021

J. Agric. Food Chem.

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Ethylene acts as an important hormone to trigger the ripening and senescence of fruits and vegetables (F&V). Thus, it is essential to eliminate trace ethylene and prevent F&V losses effectively. There are several technologies currently applying to control the ethylene concentration in the storage and transportation environment, including adsorption, gene modification, oxidation, etc. These protocols will be compared, and special attention will be paid to the low-temperature catalytic oxidation that has already been applied to practical production in this review. The active sites, supports, and reaction and deactivation mechanism of the catalysts for the low-temperature ethylene oxidation will be discussed and evaluated systematically to provide new insights for the development of effective catalysts, along with the suggestion of some perspectives for future research on this important catalytic system for F&V preservation.

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Low Temperature Oxidation of Trace Ethylene over Pt Nanoparticles Supported on Hydrophobic Mesoporous Silica

Cited by 12 publications

References 12 publications

Water-Resistant Pt Sites in Hydrophobic Mesopores Effective for Low-Temperature Ethylene Oxidation

Water-Resistant Pt Sites in Hydrophobic Mesopores Effective for Low-Temperature Ethylene Oxidation

DFT Mechanistic Study on the Complete Oxidation of Ethylene by the Silica-Supported Pt Catalyst: C═C Activation via the Ethylene Dioxide Intermediate

Elimination or Removal of Ethylene for Fruit and Vegetable Storage via Low-Temperature Catalytic Oxidation

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