Aerobic Oxidations of Light Alkanes over Solid Metal Oxide Catalysts

Grant, Joseph T.; Venegas, Juan M.; McDermott, William P.; Hermans, Ive

doi:10.1021/acs.chemrev.7b00236

Cited by 278 publications

(195 citation statements)

References 285 publications

(764 reference statements)

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“…Propylene is an important building block in the chemical industry, mostly obtained by steam cracking of naphtha and fluid catalytic cracking as a byproduct. [ 1 ] However, large amounts of shale gas were discovered worldwide in recent years, making the source of steam cracking lighter. This may lead to a shortage of propylene in the near future.…”

Section: Introductionmentioning

confidence: 99%

Chemical Insight into the Structure and Formation of Coke on PtSn Alloy during Propane Dehydrogenation

Wang

Chen

Mao

et al. 2020

Advanced Sustainable Systems

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Propane dehydrogenation (PDH) catalyzed by PtSn/Al2O3 is a vital industrial process for producing propylene, a significant building block in the chemical industry. However, coke produced in the process deactivates the catalyst and the energy‐intensive regeneration procedures can produce considerable CO2 emission. In this work, coke on the spent catalysts is analyzed by thermogravimetric‐mass spectra, Raman spectra, 1H solid NMR spectra, and infrared spectra. Several C3 species, including propyl, propylidene and propylidyne are found on the surface of the PtSn alloy. Several reaction pathways are investigated by density functional theory (DFT) calculations. It is also found that this coke can be hydrogenated to propylene in the PDH process. These results could provide theoretical guidance for optimizing process parameters in industry.

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Section: Introductionmentioning

confidence: 99%

Chemical Insight into the Structure and Formation of Coke on PtSn Alloy during Propane Dehydrogenation

Wang

Chen

Mao

et al. 2020

Advanced Sustainable Systems

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“…Ethylene (C 2 H 4 ) is one of the most fundamental building blocks in chemical industry for the synthesis of various chemical products 1,2 . The industrial manufacture of ethylene is mainly by steam cracking of naphtha and ethane, which is operated at high temperature (> 800 °C) due to the thermodynamic constraint of this process.…”

Section: Read Full License Introductionmentioning

confidence: 99%

Defect-rich TiO2 in situ evolved from MXene for efficiently oxidative dehydrogenation of ethane

Zhou¹,

Li²,

Chai³

et al. 2020

Preprint

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It remains a challenge to make metal oxides with limited reducibility as active component rather than support or modifier for the oxidative dehydrogenation (ODH) of light alkanes. Here, we report a special TiO2 (M-TiO2) evolved from Ti3C2Tx MXene material to be a new kind of efficient catalyst in the ODH of ethane. The reactivity on this M-TiO2 is four times higher than that on P25 TiO2, endowing an excellent ethylene productivity of 15.4 gC2H4 gcat-1 h-1 that outperforms the previously reported catalysts. Experimental characterizations and theoretical calculations reveal the existence of both Ti and oxygen vacancy defects on M-TiO2. The Ti defect can increase the reducibility of M-TiO2 to reduce the activation barrier of ethane while the oxygen vacancy facilitates the adsorption of O2 to recover lattice oxygen, accounting for the high performance. This work enlightens the defect engineering of traditional metal oxide as a promising catalyst in the oxidation catalysis.

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“…[1][2][3][4][5][6] Several metal-oxides that are used as a catalyst for the aerobic oxidation of organic molecules are semiconductors (e. g. TiO 2 , ZnO, Fe 2 O 3 ) and also act as chemiresistors for the detection of vapor phase organic analytes. catalyzed aerobic oxidations of organic molecules are attractive as a cost-effective and greener route for the synthesis of fine chemicals as compared to the traditional liquid phase reactions.…”

mentioning

confidence: 99%

Discrimination of 1‐ and 2‐Propanol by Using the Transient Current Change of a Semiconducting ZnFe₂O₄ Chemiresistor

et al. 2019

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A semiconducting metal oxide (SMO) chemiresistor (ZnFe 2 O 4 ) is used for discriminating two isomeric volatile organic compounds (VOCs), namely 1-and 2-propanol. The transient current of the SMO chemiresistor is correlated with the aerobic oxidation of organic vapors on its surface. The changes in transient current of the ZnFe 2 O 4 chemiresistor are measured at different temperatures (260-320°C) for detecting equal concentrations (200 ppm) of the two structural isomers of propanol. The transient current of ZnFe 2 O 4 reflects a faster oxidation of 2propanol than 1-propanol on the surface. First-principles calculations and kinetic studies on the interaction of 1-and 2propanol over ZnFe 2 O 4 provide further insight in support of the experimental evidence. The calculations predict more spontaneous adsorption of 2-propanol on the (111) surface of ZnFe 2 O 4 than 1-propanol. Kinetic parameters for the oxidation of isomeric vapors are estimated by modelling the transient current of ZnFe 2 O 4 using the Langmuir-Hinshelwood reaction mechanism. The faster oxidation of 2-propanol and comparatively lower activation energy for the respective process over ZnFe 2 O 4 is justified in accordance to the chemical structures of vapors. The findings have strong implications in exploring a new technique for discriminating isomeric VOCs, which is significant for environmental monitoring and medical applications.Metal-oxide (e. g.etc.) catalyzed aerobic oxidations of organic molecules are attractive as a cost-effective and greener route for the synthesis of fine chemicals as compared to the traditional liquid phase reactions. [1][2][3][4][5][6] Several metal-oxides that are used as a catalyst for the aerobic oxidation of organic molecules are semiconductors (e. g. TiO 2 , ZnO, Fe 2 O 3 ) and also act as chemiresistors for the detection of vapor phase organic analytes. [7][8][9][10] Unlike physisorption based charge transfer sensors, semiconducting metal oxide (SMO) based chemiresistors are mostly operative at high temperature and their resistance/conductance changes in exposure to reducing gases or vapors. [11][12][13][14] Investigating the operation principle of SMO chemiresistors, it is identified that their transient current in response cycle is basically the reflection of collective interactions (e. g., adsorption, diffusion, and aerobic oxidation) of target analyte on the respective metal-oxide surface. The adsorption, diffusion, and oxidation of two organic vapors over single SMO chemiresistor (kept at fixed experimental condition) are dependent on the molecular weight and chemical structure of the vapors. The transient response for SMOs under the exposure of isomeric vapors (having the same molecular weight) is influenced only by their chemical structures. It is thus possible to discriminate a volatile organic compound (VOC) from its isomeric counterpart by monitoring the transient current of the chemiresistors. As compared to adsorption and diffusion, aerobic oxidation of vapors predominantly modulates the charge carriers i...

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Aerobic Oxidations of Light Alkanes over Solid Metal Oxide Catalysts

Cited by 278 publications

References 285 publications

Chemical Insight into the Structure and Formation of Coke on PtSn Alloy during Propane Dehydrogenation

Chemical Insight into the Structure and Formation of Coke on PtSn Alloy during Propane Dehydrogenation

Defect-rich TiO2 in situ evolved from MXene for efficiently oxidative dehydrogenation of ethane

Discrimination of 1‐ and 2‐Propanol by Using the Transient Current Change of a Semiconducting ZnFe₂O₄ Chemiresistor

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Aerobic Oxidations of Light Alkanes over Solid Metal Oxide Catalysts

Cited by 278 publications

References 285 publications

Chemical Insight into the Structure and Formation of Coke on PtSn Alloy during Propane Dehydrogenation

Chemical Insight into the Structure and Formation of Coke on PtSn Alloy during Propane Dehydrogenation

Defect-rich TiO2 in situ evolved from MXene for efficiently oxidative dehydrogenation of ethane

Discrimination of 1‐ and 2‐Propanol by Using the Transient Current Change of a Semiconducting ZnFe2O4 Chemiresistor

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Product

Resources

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Discrimination of 1‐ and 2‐Propanol by Using the Transient Current Change of a Semiconducting ZnFe₂O₄ Chemiresistor