Flower-like Pt/Fe2O3–CeO2 Catalysts for Highly Efficient Low-Temperature Catalytic Oxidation of Toluene

Zhou, Yuanbo; He, Jiaqin; Chen, Dongyun; Li, Xunxun; Wang, Yaru; Xiao, Jun; Li, Najun; Xu, Qingfeng; Li, Hua; He, Jinghui; Lu, Jianmei

doi:10.1021/acs.iecr.1c00108

Cited by 23 publications

(11 citation statements)

References 51 publications

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“…The XRD of these samples reveals that the α-Fe 2 O 3 structure of the catalysts is not changed by the low concentration of doped Ce, but the peak in Ce-doped samples gradually broadened compared to that of pure Fe 2 O 3 -350 °C. The slight decrease in the iron content and the sintering inhibition of dopant cerium resulted in poor crystallinity. , The structure and composition of the as-prepared catalysts were analyzed by Raman spectroscopy (Figure S1). The sharp peak at 460 cm –1 attributed to the F 2g vibration mode of a fluorite-type structure could only be observed in CeO 2 -350 °C .…”

Section: Resultsmentioning

confidence: 99%

“…The slight decrease in the iron content and the sintering inhibition of dopant cerium resulted in poor crystallinity. 41,42 The structure and composition of the as-prepared catalysts were analyzed by Raman spectroscopy (Figure S1). The sharp peak at 460 cm −1 attributed to the F 2g vibration mode of a fluorite-type structure could only be observed in CeO 2 -350 °C.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

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Modulating the Electronic Structure of α-Fe₂O₃ by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Zhao

Wang

Gao

et al. 2023

ACS Sustainable Chem. Eng.

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The metal-oxide-catalyzed transfer hydrogenation of nitroarenes to anilines by hydrazine hydrate has been widely reported; however, the risk of explosion resulting from excess hydrazine hydrate and high temperatures and complex preparations of these catalysts immensely hinder their industrial application. Herein, we use a simple co-precipitation method to synthesize atomically dispersed Ce-doped α-Fe 2 O 3 (Ce 0.025 -Fe 2 O 3 -350 °C), which can completely reduce nitroarenes using stoichiometric hydrazine hydrate at room temperature, where the parent α-Fe 2 O 3 is inactive. A thorough characterization indicates that the incorporation of Ce into the crystal lattice of α-Fe 2 O 3 reorganizes the electronic structure of the surrounding Fe, such that the Lewis acidity of Fe 2 O 3 is enhanced, which is the key for the room-temperature decomposition of N 2 H 4 •H 2 O. The structure is also beneficial for the adsorption of nitroarene, leading to the weakening of the N−O bonds. Mechanistic experiments and DFT calculations demonstrate that the reduction proceeds through Ph-NO 2 → Ph-NHOH → Ph-NH 2 without the widely recognized Ph-NO intermediate. Moreover, Ce 0.025 -Fe 2 O 3 -350 °C exhibits good stability in a continuous-flow reaction.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 99%

Modulating the Electronic Structure of α-Fe₂O₃ by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Zhao

Wang

Gao

et al. 2023

ACS Sustainable Chem. Eng.

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“…In addition, Zhou et al (2021) reported the preparation of Pt nanoparticle-loaded Fe 2 O 3 –CeO 2 catalysts for efficient catalytic oxidation of toluene, showing the superior catalytic activity of this catalyst for toluene oxidation compared with unmodified Fe 2 O 3 –CeO 2 . It was found that the high concentration of active surface lattice oxygen, whose formation is promoted by both the addition of Pt and the synergism between Fe 2 O 3 and CeO 2 , plays a vital role in efficient toluene combustion . These studies demonstrated that active surface lattice oxygen of a catalyst is a key factor for effective VOC combustion.…”

Section: Introductionmentioning

confidence: 97%

“…These studies demonstrated that active surface lattice oxygen of a catalyst is a key factor for effective VOC combustion. Various transitional metal oxides such as Fe 2 O 3 , MnO 2 , Co 3 O 4 , Cr 2 O 3 , and CeO 2 have frequently been utilized as supports for noble metal nanoparticles (Pd, Au, Rh, and Pt) due to their excellent oxygen storage capacity and good redox properties for oxygen activation . Most previous studies have focused on the catalytic combustion of aromatics and heteroatom-containing organic compounds, such as benzene, toluene, o -xylene, and trichloroethylene. − In contrast, few studies have focused on the catalytic combustion of cyclohexane due to its chemically inactive molecular structure and stability, resulting in most catalysts being unsuitable for its catalytic decomposition under low-temperature conditions. , In addition, little is known about the interfacial VOC transformation process and oxidation mechanisms associated with noble metals and surface oxygen vacancices in VOC combustion.…”

Section: Introductionmentioning

confidence: 99%

Efficient Catalytic Combustion of Cyclohexane over PdAg/Fe₂O₃ Catalysts under Low-Temperature Conditions: Establishing the Degradation Mechanism Using PTR-TOF-MS and in Situ DRIFTS

Wen

Guo

et al. 2022

ACS Appl. Mater. Interfaces

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Cyclohexane, a typical volatile organic compound (VOC), poses high risks to the environment and humans. Herein, synthesized PdAg/Fe2O3 catalysts exhibited exceptional catalytic performance for cyclohexane combustion at lower temperatures (50% mineralization temperature (T 50) of 199 °C, 90% mineralization temperature (T 90) of 315 °C) than Pd/Fe2O3 (T 50 of 262 °C, T 90 of 335 °C) and Fe2O3 (T 50 of 305 °C, T 90 of 360 °C). In addition, PdAg/Fe2O3 displayed enhanced stability by alloying Ag with Pd. The redox and acidity of the PdAg/Fe2O3 were studied by XPS, H2-TPR, and NH3-TPD. In situ diffuse reflectance infrared Fourier transform spectroscopy and proton-transfer-reaction time-of-flight mass spectrometry were applied to identify the intermediates formed on the catalyst surface and in the tail gas during oxidation, respectively. Results suggested that loading PdAg onto Fe2O3 significantly enhanced the adsorption and activation of oxygen and cyclohexane, oxidative dehydrogenation of cyclohexane to benzene, and catalytic cracking of cyclohexane to olefins at low temperatures. This in-depth study will benefit the design and application of efficient catalysts for the effective combustion of VOCs at low temperatures.

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“…Compared to the general combustion method, catalytic oxidation is considered a versatile way for completely converting toxic VOCs into CO 2 and H 2 O with hardly any formation of NO x . , Designing highly active catalysts is the key issue for achieving practical applications of this technique. However, supported platinum group metals (PGMs) are still the most efficient catalysts for the catalytic removal of VOCs. − Considering their high cost, low thermal stability, and poisoning tendency, their wide application will be limited. Therefore, it is highly desirable to explore alternative catalysts with low cost and high performance for deep oxidation of VOCs.…”

Section: Introductionmentioning

confidence: 99%

Fabrication of Hierarchical Porous Metal Oxides by the HPMC-Assisted Gel Combustion Strategy: Incorporation of Nanoceria into Cookie-like Mn₂O₃ with Enhanced Oxidation Activity and Excellent Water Resistance

Cao

Zhang

et al. 2023

Ind. Eng. Chem. Res.

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Constructing nonprecious metal oxide catalysts with a hierarchical porous structure by a simple method for the deep catalytic oxidation of toxic volatile organic compounds at low temperatures is of great value and significance. In this work, a porous manganese trioxide catalyst (Mn 2 O 3 -H) was prepared by a hydroxypropyl methylcellulose-assisted combustion synthesis strategy for catalytic complete oxidation of gaseous toluene. Benefiting from the rich porous nanostructure, Mn 2 O 3 -H has much higher specific surface area and active site density, resulting in better low-temperature reducibility and oxygen activation ability than blank Mn 2 O 3 formed by direct calcination. With this sol−gel combustion process, CeO 2 nanoparticles could be successfully introduced to form cookie-like Ce−Mn composite oxide with a hierarchical porous nanostructure, which builds the strong interaction of CeO 2 − Mn 2 O 3 to weaken Mn−O with more active defects. Among Ce-doped catalysts, 5% CeMn-H shows the best catalytic activity in toluene oxidation with 90% conversion temperature at 242 °C under a weight hour space velocity of 60,000 mL•g −1 •h −1 , which is about 30 and 133 °C lower than that of Mn 2 O 3 -H and Mn 2 O 3 -B, respectively. This advantage is also shown in other typical hydrocarbons such as propylene and propane. Moreover, the as-prepared Ce-doped catalyst exhibits excellent stability and water resistance ability. This simple robust sol−gel combustion method will provide valuable enlightenment for designing porous catalysts with high performance for related catalytic reactions.

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Flower-like Pt/Fe₂O₃–CeO₂ Catalysts for Highly Efficient Low-Temperature Catalytic Oxidation of Toluene

Cited by 23 publications

References 51 publications

Modulating the Electronic Structure of α-Fe₂O₃ by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Modulating the Electronic Structure of α-Fe₂O₃ by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Efficient Catalytic Combustion of Cyclohexane over PdAg/Fe₂O₃ Catalysts under Low-Temperature Conditions: Establishing the Degradation Mechanism Using PTR-TOF-MS and in Situ DRIFTS

Fabrication of Hierarchical Porous Metal Oxides by the HPMC-Assisted Gel Combustion Strategy: Incorporation of Nanoceria into Cookie-like Mn₂O₃ with Enhanced Oxidation Activity and Excellent Water Resistance

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Flower-like Pt/Fe2O3–CeO2 Catalysts for Highly Efficient Low-Temperature Catalytic Oxidation of Toluene

Cited by 23 publications

References 51 publications

Modulating the Electronic Structure of α-Fe2O3 by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Modulating the Electronic Structure of α-Fe2O3 by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Efficient Catalytic Combustion of Cyclohexane over PdAg/Fe2O3 Catalysts under Low-Temperature Conditions: Establishing the Degradation Mechanism Using PTR-TOF-MS and in Situ DRIFTS

Fabrication of Hierarchical Porous Metal Oxides by the HPMC-Assisted Gel Combustion Strategy: Incorporation of Nanoceria into Cookie-like Mn2O3 with Enhanced Oxidation Activity and Excellent Water Resistance

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Flower-like Pt/Fe₂O₃–CeO₂ Catalysts for Highly Efficient Low-Temperature Catalytic Oxidation of Toluene

Modulating the Electronic Structure of α-Fe₂O₃ by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Modulating the Electronic Structure of α-Fe₂O₃ by Doping Atomically Dispersed Ce for the Transfer Hydrogenation of Nitroaromatics Using Stoichiometric Hydrazine Hydrate

Efficient Catalytic Combustion of Cyclohexane over PdAg/Fe₂O₃ Catalysts under Low-Temperature Conditions: Establishing the Degradation Mechanism Using PTR-TOF-MS and in Situ DRIFTS

Fabrication of Hierarchical Porous Metal Oxides by the HPMC-Assisted Gel Combustion Strategy: Incorporation of Nanoceria into Cookie-like Mn₂O₃ with Enhanced Oxidation Activity and Excellent Water Resistance