Construction of Cu-Ce interface for boosting toluene oxidation: Study of Cu-Ce interaction and intermediates identified by in situ DRIFTS

Different Cu contents (x wt%) were supported on the cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) (xCu/OMS-2; x = 1, 5, 15, and 20) via a pre-incorporation method. Physicochemical properties of the OMS-2 and xCu/OMS-2 samples were characterized by means of the XRD, FT-IR, SEM, TG/DTG, ICP-OES, XPS, O2-TPD, H2-TPR, and in situ DRIFTS techniques, and their catalytic activities were measured for the oxidation of CO, ethyl acetate, and toluene. The results show that the Cu species were homogeneously dispersed in the tunnel and framework structure of OMS-2. Among all of the samples, 15Cu/OMS-2 sample exhibited the best activities with the T50% of 65, 165, and 240 °C as well as the T90% of 85, 215, and 290 °C for CO, ethyl acetate and toluene oxidation, respectively, which was due to the existence of the Cu species and Mn3+/Mn4+ redox couples, rich oxygen vacancies, good oxygen mobility, low-temperature reducibility, and strong interaction between the Cu species and the OMS-2 support. The reaction mechanisms were also deduced by analyzing the in situ DRIFTS spectra of the 15Cu/OMS-2 sample. The excellent oxygen mobility associated with the electron transfer between Cu species and Mn3+/Mn4+ redox couples might be conducive to the continuous replenishment of active oxygen species and the constantly generated reactant intermediates, thereby increasing the reactant reaction rate.

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Toluene oxidation process and proper mechanism over Co3O4 nanotubes: Investigation through in-situ DRIFTS combined with PTR-TOF-MS and quasi in-situ XPS

Chemical Engineering Journal ◽

10.1016/j.cej.2020.125375 ◽

2020 ◽

Vol 397 ◽

pp. 125375 ◽

Cited By ~ 3

Author(s):

Jinping Zhong ◽

Yikui Zeng ◽

Mingyuan Zhang ◽

Weihua Feng ◽

Diran Xiao ◽

...

Keyword(s):

Oxidation Process ◽

Toluene Oxidation ◽

In Situ Drifts ◽

In Situ Xps ◽

Tof Ms

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Insight into the Promoting Role of Er Modification on SO2 Resistance for NH3-SCR at Low Temperature over FeMn/TiO2 Catalysts

Catalysts ◽

10.3390/catal11050618 ◽

2021 ◽

Vol 11 (5) ◽

pp. 618

Author(s):

Huan Du ◽

Zhitao Han ◽

Xitian Wu ◽

Chenglong Li ◽

Yu Gao ◽

...

Keyword(s):

Low Temperature ◽

Catalyst Surface ◽

Impregnation Method ◽

In Situ Drifts ◽

Tio2 Catalyst ◽

Nh3 Scr ◽

Nh3 Adsorption ◽

So2 Resistance ◽

Fast Scr

Er-modified FeMn/TiO2 catalysts were prepared through the wet impregnation method, and their NH3-SCR activities were tested. The results showed that Er modification could obviously promote SO2 resistance of FeMn/TiO2 catalysts at a low temperature. The promoting effect and mechanism were explored in detail using various techniques, such as BET, XRD, H2-TPR, XPS, TG, and in-situ DRIFTS. The characterization results indicated that Er modification on FeMn/TiO2 catalysts could increase the Mn4+ concentration and surface chemisorbed labile oxygen ratio, which was favorable for NO oxidation to NO2, further accelerating low-temperature SCR activity through the “fast SCR” reaction. As fast SCR reaction could accelerate the consumption of adsorbed NH3 species, it would benefit to restrain the competitive adsorption of SO2 and limit the reaction between adsorbed SO2 and NH3 species. XPS results indicated that ammonium sulfates and Mn sulfates formed were found on Er-modified FeMn/TiO2 catalyst surface seemed much less than those on FeMn/TiO2 catalyst surface, suggested that Er modification was helpful for reducing the generation or deposition of sulfate salts on the catalyst surface. According to in-situ DRIFTS the results of, the presence of SO2 in feeding gas imposed a stronger impact on the NO adsorption than NH3 adsorption on Lewis acid sites of Er-modified FeMn/TiO2 catalysts, gradually making NH3-SCR reaction to proceed in E–R mechanism rather than L–H mechanism. DRIFTS.

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Experimental and Theoretical Studies of Sonically Prepared Cu–Y, Cu–USY and Cu–ZSM-5 Catalysts for SCR deNOx

Catalysts ◽

10.3390/catal11070824 ◽

2021 ◽

Vol 11 (7) ◽

pp. 824

Author(s):

Przemysław J. Jodłowski ◽

Izabela Czekaj ◽

Patrycja Stachurska ◽

Łukasz Kuterasiński ◽

Lucjan Chmielarz ◽

...

Keyword(s):

Ion Exchange ◽

Ultrasonic Irradiation ◽

Active Phase ◽

Spectroscopic Studies ◽

In Situ Drifts ◽

Ft Ir ◽

Diffuse Reflectance Infrared ◽

Experimental And Theoretical Studies

The objective of our study was to prepare Y-, USY- and ZSM-5-based catalysts by hydrothermal synthesis, followed by copper active-phase deposition by either conventional ion-exchange or ultrasonic irradiation. The resulting materials were characterized by XRD, BET, SEM, TEM, Raman, UV-Vis, monitoring ammonia and nitrogen oxide sorption by FT-IR and Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). XRD data confirmed the purity and structure of the Y/USY or ZSM-5 zeolites. The nitrogen and ammonia sorption results indicated that the materials were highly porous and acidic. The metallic active phase was found in the form of cations in ion-exchanged zeolites and in the form of nanoparticle metal oxides in sonochemically prepared catalysts. The latter showed full activity and high stability in the SCR deNOx reaction. The faujasite-based catalysts were fully active at 200–400 °C, whereas the ZSM-5-based catalysts reached 100% activity at 400–500 °C. Our in situ DRIFTS experiments revealed that Cu–O(NO) and Cu–NH3 were intermediates, also indicating the role of Brønsted sites in the formation of NH4NO3. Furthermore, the results from our experimental in situ spectroscopic studies were compared with DFT models. Overall, our findings suggest two possible mechanisms for the deNOx reaction, depending on the method of catalyst preparation (i.e., conventional ion-exchange vs. ultrasonic irradiation).

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Diffuse Reflectance FT-IR Characterization of Active Sites under Reaction Conditions: The Production of Oxygenates in the CO/H2 Reaction

Applied Spectroscopy ◽

10.1366/0003702944027345 ◽

1994 ◽

Vol 48 (10) ◽

pp. 1208-1212 ◽

Cited By ~ 7

Author(s):

J. J. Benítez ◽

I. Carrizosa ◽

J. A. Odriozola

Keyword(s):

Infrared Spectra ◽

Active Sites ◽

Diffuse Reflectance ◽

Reaction Conditions ◽

In Situ Drifts ◽

Ft Ir

The reactivity of a Lu2O3-promoted Rh/Al2O3 catalyst in the CO/H2 reaction is reported. Methane, heavier hydrocarbons, methanol, and ethanol are obtained. In situ DRIFTS has been employed to record the infrared spectra under the actual reaction conditions. The structure of the observed COads DRIFTS bands has been resolved into its components. The production of oxygenates (methanol and ethanol) has been correlated with the results of the deconvolution calculation. Specific sites for the production of methanol and ethanol in the CO/H2 reaction over a Rh,Lu2O3/Al2O3 catalyst are proposed.

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