Non-aqueous synthesis of homogeneous molybdenum silicate microspheres and their application as heterogeneous catalysts in olefin epoxidation and selective aniline oxidation

Škoda, David; Hanulíková, Barbora; Stýskalík, Aleš; Vykoukal, Vít; Macháč, Petr; Urbánek, Pavel; Domincova-Bergerova, Eva; Šimoníková, Lucie; Kuřitka, Ivo

doi:10.1016/j.jiec.2021.12.001

Cited by 7 publications

(3 citation statements)

References 76 publications

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“…Zirconosilicate samples were prepared by NHSG, a technique that is known to produce mixed metal oxides with high homogeneity of metal mixing and good textural properties [32][33][34][35][36][37].…”

Section: Synthesismentioning

confidence: 99%

Catalytic Performance of Micro-Mesoporous Zirconosilicates Prepared by Non-Hydrolytic Sol-Gel in Ethanol-To-Butadiene Transformation and Related Reactions

Hradsky

Macháč

Škoda

et al. 2022

Preprint

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Synthesis of 1,3-butadiene (BD) from ethanol has experienced a true renaissance in recent years due to ecological and economic reasons. The open porosity and number of Lewis acid sites in metal silicates (M = Zr, Ta) have been reported in numerous studies as key factors enabling reaching high BD productivity. However, some microporous zeolites recently displayed very high BD productivity. To gain a deeper insight, we have applied non-hydrolytic sol-gel (NHSG) – a method well-known to produce highly porous and homogeneous metal silicates – in the preparation of zirconosilicates with varying micropore volume. The porosity (N2 adsorption-desorption experiments), structure (IR, XPS, NMR, and DRUV-Vis spectroscopy, XRD, MAS NMR), and acidity (IR spectroscopy combined with pyridine adsorption) of these materials have been described in detail and compared to a benchmark sample prepared by dry impregnation. Above mentioned characterization methods proved that NHSG preparation provided highly homogeneous Zr dispersion in silica leading to almost doubled Lewis acid site numbers and higher activity in ethanol-to-butadiene (ETB) transformation, Meerwein-Ponndorf-Verley (MPV) redox reaction, and aldol condensation, in comparison to the catalyst prepared by dry impregnation. The fraction of micropore volume in micro-mesoporous samples (ranging from 27 % to 69 %) did not play a significant role: The activity in all three catalytic reactions followed the acid site numbers. The selectivity and long-term stability in ETB process were similar for catalysts prepared by NHSG and dry impregnation.

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Section: Synthesismentioning

confidence: 99%

Catalytic Performance of Micro-Mesoporous Zirconosilicates Prepared by Non-Hydrolytic Sol-Gel in Ethanol-To-Butadiene Transformation and Related Reactions

Hradsky

Macháč

Škoda

et al. 2022

Preprint

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“…27−31 We have recently introduced a facile method for preparing homogeneous molybdenum silicate microspheres and shown their application as heterogeneous catalysts for epoxidation reactions. 32 The synthesis based on the NHSG condensation of a hybrid molybdenum biphenyldicarboxylate-based precursor solution (labeled as Mo-Bpdc) with (3-aminopropyl)triethoxysilane allows for a homogeneous distribution of highly dispersed molybdenum species within a silica matrix after calcination. These findings prompted us to investigate the potential of such Mo-based catalysts in the olefin metathesis reaction.…”

Section: Introductionmentioning

confidence: 99%

Propylene Metathesis over Molybdenum Silicate Microspheres with Dispersed Active Sites

Skoda,

Zhu,

Hanulikova

et al. 2023

ACS Catal.

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In this work, we demonstrate that amorphous and porous molybdenum silicate microspheres are highly active catalysts for heterogeneous propylene metathesis. Homogeneous molybdenum silicate microspheres and aluminum-doped molybdenum silicate microspheres were synthesized via a nonaqueous condensation of a hybrid molybdenum biphenyldicarboxylatebased precursor solution with (3-aminopropyl)triethoxysilane. The as-prepared hybrid metallosilicate products were calcined at 500 °C to obtain amorphous and porous molybdenum silicate and aluminum-doped molybdenum silicate microspheres with highly dispersed molybdate species inserted into the silicate matrix. These catalysts contain mainly highly dispersed MoO x species, which possess high catalytic activity in heterogeneous propylene metathesis to ethylene and butene. Compared to conventional silica-supported MoO x catalysts prepared via incipient wetness impregnation (MoIWI), the microspheres with low Mo content (1.5−3.6 wt %) exhibited nearly 2 orders of magnitude higher steady-state propylene metathesis rates at 200 °C, approaching site time yields of 0.11 s −1 .

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“…Transition-metal complexes have received remarkable attention from current researchers in the removal of organic wastewater through Fenton-like chemical reactions. During the process of nonhomogeneous Fenton reactions, the stability and efficient electron migration ability of nonhomogeneous catalysts are utilized to achieve the complete removal of refractory organic compounds without bringing Fe 3+ from the catalyst into the environment to cause secondary pollution [28]. Common nonhomogeneous Fenton reaction catalysts include Fe 3 O 4 , Fe 2 O 3 , FeOCl, and XFe 2 O 4 (X: Cu, Co, Zn, or Mn) [29][30][31][32][33].…”

Section: Introductionmentioning

confidence: 99%

Preparation of FeSe2-Based Fenton Catalysts Loaded on Chloro-Methyl Styrene-Based Resins and Study of Activated Persulfate Degradation of Tetracycline

Wang

Zhang

et al. 2023

Sustainability

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Fenton technology has excellent performance in the treatment of hard-to-degrade organics but tends to cause secondary pollution to the environment. Given its excellent adsorption capacity and the availability of mature adsorption modification studies, poly(chloromethyl styrene)-based resin (PS-Cl) has received much attention for the adsorption of heavy metal ions. However, combining the mature Fenton technology with the highly popular PS-Cl through a stable bridge to exploit the advantages of catalytic degradation performance of Fenton-like technology is the main focus of our work. The PS-NH2@FeSe2 catalyst with a core–shell structure was synthesized. The catalytic degradation of tetracycline solution in the presence of PS-NH2@FeSe2 and persulfate achieved a satisfactory effect. The removal efficiency was as high as 85.94% within 2 h, and the degradation rate constant was 0.02352 min−1. The main advantages of the PS-NH2@FeSe2 catalyst were high stability and recyclability. Thus, the catalyst would not cause secondary pollution to the environment and could still achieve a degradation efficiency of nearly 70% for TC after five times of reuse. The possible catalytic degradation pathways and potential removal mechanisms were investigated through free-radical quenching experiments and HPLC-MS detection of intermediates generated through catalytic degradation. Column experiments were conducted to investigate the effect of the catalyst on the actual removal of wastewater, and a simple flow model was developed using Yellow River water to make the integration of theory and practice possible. In conclusion, the new idea constructed with FeSe2-loaded modified resin offers promising prospects in the removal of refractory organic compounds, such as tetracycline.

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Non-aqueous synthesis of homogeneous molybdenum silicate microspheres and their application as heterogeneous catalysts in olefin epoxidation and selective aniline oxidation

Cited by 7 publications

References 76 publications

Catalytic Performance of Micro-Mesoporous Zirconosilicates Prepared by Non-Hydrolytic Sol-Gel in Ethanol-To-Butadiene Transformation and Related Reactions

Catalytic Performance of Micro-Mesoporous Zirconosilicates Prepared by Non-Hydrolytic Sol-Gel in Ethanol-To-Butadiene Transformation and Related Reactions

Propylene Metathesis over Molybdenum Silicate Microspheres with Dispersed Active Sites

Preparation of FeSe2-Based Fenton Catalysts Loaded on Chloro-Methyl Styrene-Based Resins and Study of Activated Persulfate Degradation of Tetracycline

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