Highly effective microwave catalytic oxidative dehydrogenation of propane by CO2 over V-La-doped dendritic mesoporous silica-based microwave catalysts

Ma, Zengsheng; Xu, Wentao; Wang, Qige; Zhou, Qibing; Zhou, Jicheng

doi:10.1016/j.cej.2022.135081

Cited by 21 publications

(6 citation statements)

References 70 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In addition, because of the low-temperature synthesis and high purity of the obtained nanopowders, some researchers have reported sol–gel to be a facile method to synthesize CrO x catalysts for the oxidative dehydrogenation process. , However, the annealing temperature during the preparation of the catalyst could affect the ODHP reaction. Besides, some active sites such as the acid/base properties, the electrophilic oxygen species, and the carbonate species also participate in the oxidation reaction mechanism. − Previous studies proved that CrO x is a highly efficient catalyst for the ODHP. − Others also used CrO x to improve the catalytic activity and stability. , However, the deactivation of these catalysts with time-on-stream still poses a problem for industrial application. Despite extensive research demonstrating CrO x ’s ability to convert propane to propene, no systematic work has been conducted to investigate the effect of calcination temperature on improving the catalytic performance of CrO x for the ODHP reaction and its influence on the catalyst’s stability.…”

Section: Introductionmentioning

confidence: 99%

Oxidative Dehydrogenation of Propane into Propene over Chromium Oxides

Monguen

Kasmi

Arshad

et al. 2022

Ind. Eng. Chem. Res.

View full text Add to dashboard Cite

A series of chromium oxides (CrO x ) were prepared using the sol−gel method for the oxidative dehydrogenation of propane into propene (ODHP). After calcination at temperatures ranging from 300 °C to 600 °C, the obtained nanopowders were comprehensively characterized. X-ray diffraction (XRD) results showed an increase in crystallite size with annealing temperature, whereas Brunauer−Emmett−Teller (BET) analysis disclosed a decreasing tendency of specific surface area. Scanning electron microscopy (SEM) results disclosed spherical and smooth shapes with an agglomeration of small fine particles. X-ray photoelectron spectroscopy (XPS) deconvolution revealed a decrement in lattice oxygen, O Lat /O Ads , and Cr 6+ /Cr 3+ with annealing temperature. Raman and ultraviolet−visible light (UV-vis) spectra reported the presence of isolated and polymeric Cr 6+ oxides and the increment of the bandgap energy with the increase of the calcination temperature. Cr-300 exhibited the best catalytic activity due to the smallest crystallite grain size and bandgap energy, the highest O Lat /O Ads , Cr 6+ /Cr 3+ , and O Lat with the largest surface specific area. Furthermore, after a stability test of 100 h, all catalysts maintained >90% propane conversion, and Cr-300 was the most stable. The DFT calculations revealed that the Cr−O site is the leading active site in the promotion of ODHP. The high stability and performance of Cr-300 catalyst regarding ODHP could pave the way for further industrial applications.

show abstract

Section: Introductionmentioning

confidence: 99%

Oxidative Dehydrogenation of Propane into Propene over Chromium Oxides

Monguen

Kasmi

Arshad

et al. 2022

Ind. Eng. Chem. Res.

View full text Add to dashboard Cite

show abstract

“…Specifically, for the Cr 3% Fe 2% -ZSM-5 sample, the reduction peak around 400 • C was related to the reduction of Fe 2 O 3 to Fe 3 O 4 ; the peak around 500 • C was attributed to the reduction of Fe 3 O 4 to FeO; and the peak around 600 • C was ascribed to the reduction of FeO to Fe [32]. As for Cr 3% Zr 2% -Z5 and Cr 3% La 2% -Z5, the additional reduction peaks at T of 300-400 • C and 400-500 • C were related to the reductions of ZrO 2 and La 2 O 3 , respectively [33,34]. As noted above, after the introduction of Zr, the reduction peaks of Cr (CrO 3 → Cr 2 O 3 ) were shifted to lower temperatures (450 → 290 • C), and also developed a larger reduction peak area.…”

Section: Characterization Of Catalystsmentioning

confidence: 94%

CO2 Oxidative Dehydrogenation of Propane to Olefin over Cr-M (M = Zr, La, Fe) Based Zeolite Catalyst

Xing,

Liu,

Dai

et al. 2024

Catalysts

View full text Add to dashboard Cite

CO2 oxidative dehydrogenation of propane (CO2-ODHP), being not only favorable for olefin production but also beneficial for CO2 emission control, has recently attracted great attention. Here, a series of single metal (Cr) and bimetal (Zr, La, Fe) modified ZSM-5 zeolites were prepared via an impregnation method. It was found that the bimetal modified ZSM-5 possessed much higher C3H8 and CO2 conversion than that of monometallic modified Cr3%-ZSM-5 (Cr3%-Z5), especially for Cr3%Zr2%-ZSM-5 (Cr3%Zr2%-Z5), which displayed the highest activity (65.4%) and olefin yield (1.65 × 103 μmol·gcat−1 h−1). Various characterizations were performed, including XRD, N2 adsorption-desorption, H2-TPR, Raman, XPS, HAAD-STEM, and TEM. It was revealed that Zr not only favored an improvement in the redox ability of Cr, but also contributed to the surface dispersion of loaded Cr species, constituting two major reasons explaining the superior activity of Cr3%Zr2%-Z5. To further improve CO2-ODHP catalytic behavior, a series of Cr3%-ZSM-5@SBA-15-n composite zeolite catalysts with diverse (ZSM-5/SBA-15) mass ratios were prepared (Cr3%-ZS-n, n = 0.5, 2, 6, 16), which screened out an optimum mass ratio of six. Based on this, the Cr3%Zr2%-ZS-6 compound was further prepared, and it eventually achieved even higher CO2-ODHP activity (76.9%) and olefin yield (1.72 × 103 μmol·gcat−1 h−1). Finally, the CO2-ODHP reaction mechanism was further investigated using in situ FTIR, and it was found that the reaction followed the Mars–van Krevelen mechanism, wherein CO2 participated in the reaction through generation of polydentate carbonates. The Cr6+ constituted as the active site, which was reduced to Cr3+ after the dihydrogen reaction, and was then further oxidized into Cr6+ by CO2, forming polydentate carbonates, and thus cycling the reactive species Cr6+. Additionally, assisted by a Brönsted acid site (favoring breaking of the C-C bond), C2H4 and CH4 were produced.

show abstract

“…12−14 Our team increased propane conversion from 2% in conventional reaction mode (CRM) to 13% in MCRM over the V-La-MSNS + SiC microwave catalyst. 15 The catalytic performance of ZnO/S-1(1.0)-based microwave catalysts at 600 °C in MCRM was significantly better than that of CRM (C 3 H 8 conversion: 60 vs 37%; C 3 H 6 selectivity: 92 vs 87%). 16 However, the low-temperature catalytic performance of environmentally friendly microwave catalysts based on nonprecious metals needs further improvement.…”

Section: Introductionmentioning

confidence: 94%

Suppressed Active Site Loss by Y-Doped ZnO/Silicalite-1 for Superior CO₂ Oxidative Propane Dehydrogenation Performance by Microwave Catalysis

Nie,

Liu,

Sun

et al. 2024

Ind. Eng. Chem. Res.

Self Cite

View full text Add to dashboard Cite

Compared to energy-intensive propane direct dehydrogenation, oxidative propane dehydrogenation by CO 2 (CO 2 −ODHP) significantly reduces the energy consumption of the alkane dehydrogenation process and eliminates CO 2 . However, CO 2 −ODHP faces the challenges of low reaction efficiency at low temperatures and poor product selectivity at high temperatures in the conventional reaction mode. Microwave catalysis offers a new approach to achieve efficient reactions at lower temperatures and further reduce energy consumption, but the key is to develop highperformance microwave catalysts. Cheap and nontoxic ZnO-based catalysts have emerged as promising candidates, but the loss of active components is severe due to reduced ZnO to evaporated metal Zn during reaction. Herein, we developed suppressed active site loss by doping Y into ZnO/Silicalite-1 as a novel microwave catalyst for CO 2 −ODHP. The 5Zn−Y/Silicalite-1 + SiC microwave catalyst showed high performance with C 3 H 8 conversion of 76% and C 3 H 6 selectivity of 89% under microwave irradiation at 550 °C. However, propane conversion was only 29% under conventional reactions. Among low-cost base metal catalysts, its activity level is one of the highest. Microwave irradiation can effectively gather microwave energy and improve energy utilization efficiency. The 5Zn−Y/Silicalite-1 + SiC microwave catalyst achieved better CO 2 conversion (27%) than ZnO/Silicalite-1 + SiC (17%). Moreover, the 5Zn−Y/Silicalite-1 + SiC microwave catalyst has good stability and performance, which is attributed to the reduction of 38.79% Zn loss after Y doping. The activation energy of the catalyst for CO 2 −ODHP was significantly reduced from 98.3 to 57.4 kJ/mol by microwave irradiation. Microwave irradiation is a more energy-efficient method compared to conventional reaction for the same propane conversion. This approach highlights the great potential and advantages of multiphase catalytic reactions under microwave irradiation.

show abstract

Highly effective microwave catalytic oxidative dehydrogenation of propane by CO2 over V-La-doped dendritic mesoporous silica-based microwave catalysts

Cited by 21 publications

References 70 publications

Oxidative Dehydrogenation of Propane into Propene over Chromium Oxides

Oxidative Dehydrogenation of Propane into Propene over Chromium Oxides

CO2 Oxidative Dehydrogenation of Propane to Olefin over Cr-M (M = Zr, La, Fe) Based Zeolite Catalyst

Suppressed Active Site Loss by Y-Doped ZnO/Silicalite-1 for Superior CO₂ Oxidative Propane Dehydrogenation Performance by Microwave Catalysis

Contact Info

Product

Resources

About

Highly effective microwave catalytic oxidative dehydrogenation of propane by CO2 over V-La-doped dendritic mesoporous silica-based microwave catalysts

Cited by 21 publications

References 70 publications

Oxidative Dehydrogenation of Propane into Propene over Chromium Oxides

Oxidative Dehydrogenation of Propane into Propene over Chromium Oxides

CO2 Oxidative Dehydrogenation of Propane to Olefin over Cr-M (M = Zr, La, Fe) Based Zeolite Catalyst

Suppressed Active Site Loss by Y-Doped ZnO/Silicalite-1 for Superior CO2 Oxidative Propane Dehydrogenation Performance by Microwave Catalysis

Contact Info

Product

Resources

About

Suppressed Active Site Loss by Y-Doped ZnO/Silicalite-1 for Superior CO₂ Oxidative Propane Dehydrogenation Performance by Microwave Catalysis