Selective methane oxidation to formaldehyde using polymorphic T-, M-, and H-forms of niobium(V) oxide as catalysts

Michalkiewicz, Beata; Sreńscek-Nazzal, Joanna; Tabero, P.; Grzmil, Barbara; Narkiewicz, U.

doi:10.2478/s11696-007-0086-4

Cited by 30 publications

(17 citation statements)

References 41 publications

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“…Nano-size Nb 2 O 5 clearly exhibited 100% selectivity towards the dimethyl ether product with a good stability and activity in the temperature range of 453Á573 K without coke formation. Michalkiewicz et al (45) carried out the selective methane oxidation to formaldehyde over T-Nb 2 O 5 , the mixture of M-Nb 2 O 5 and TT-Nb 2 O 5 as well as TT-Nb 2 O 5 . Using TT-Nb 2 O 5 and M-Nb 2 O 5 phases with a block type structure, they obtained higher formaldehyde selectivity (78% at 0.9 sec) than that of T-Nb 2 O 5 (47% at 0.9 sec) the polymorphic form which does not have a block type structure.…”

Section: Potential Catalytic Applicationsmentioning

confidence: 99%

Nanostructured Nb₂O₅catalysts

et al. 2012

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Niobium pentoxide (Nb2O5) has long been known to catalyze unique acid induced reactions, redox reductions and photo-catalytic reactions, etc. Recently, there have been significant advancements in tailoring the oxide materials with controlled structures and morphologies using nano-chemical synthesis by the help of surfactant or stabilizer for optimal catalytic performance. In this short review, we will particularly highlight these synthetic methods for preparation of Nb2O5 nanostructures, their potential applications in catalysis and their structure-activity relationships

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Section: Potential Catalytic Applicationsmentioning

confidence: 99%

Nanostructured Nb₂O₅catalysts

et al. 2012

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“…While CO is adsorbed in its molecular form, H 2 adsorbs dissociatively. 14 In the next step, adsorbed H* attaches to the adsorbed CO forming HCHO which desorbs from the surface of the catalyst and hydrates to form CH 2 (OH) 2 .…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

Hydrogenation of Carbon Monoxide into Formaldehyde in Liquid Media

Bahmanpour

Hoadley

Mushrif

et al. 2016

ACS Sustainable Chem. Eng.

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Formaldehyde is a bulk chemical which is produced in excess of 30 million tons per annum and is growing in demand. However, the current production process requires methanol production, which is oxidized in air to produce formaldehyde, which must then be absorbed into water. Our recent work introduced a novel method to produce formaldehyde through CO hydrogenation in the aqueous phase. However, the aqueous phase has certain limitations which must be overcome to make it commercially viable. By applying a deuterium labeling technique and investigating the potential intermediates, the reaction mechanism was established which showed that solvents play a vital role in determining the yield. Various solvents were used for formaldehyde production, and the highest formaldehyde yield was achieved by using pure methanol followed by methanol−water mixtures. Formaldehyde reacts with methanol and water to produce hemiacetal and methylene glycol, respectively, thereby shifting the equilibrium of CO hydrogenation toward formaldehyde production. Methanol and water stabilize the hemiacetal and methylene glycol molecules, respectively, via hydrogen bonding. The highest yield of formaldehyde in methanol solvent was found to be 15.58 mmol L −1 g cat −1 at 363 K and 100 bar, which is four times higher than our previous report. The liquid phase method shown here has the potential to be greener and more sustainable than the commercial processes because it operates at low temperatures and results in 100% selectivity toward formaldehyde with no CO 2 generation. ■ INTRODUCTIONDue to the increasing global energy demand, many researchers have focused on reduction of energy consumption in the chemical industry. It is essential to search for more efficient, energy saving processes for the production of valuable chemicals. Many aspects can be considered and evaluated during process optimization. Increasing the conversion of reactants and product yield are often considered; however, process alternatives to save energy and capital costs are sometimes overlooked by researchers. Formaldehyde (HCHO) industrial production through methanol (CH 3 OH) partial oxidation dates back to 1882. 1 Since then, other methods of production such as methane (CH 4 ) partial oxidation 2−8 or CO 2 hydrogenation 9,10 were considered, but none were able to compete with the high conversion achieved by the methanol oxidation process. However, despite the high conversion of CH 3 OH and high selectivity toward HCHO, the industrial methods of HCHO production suffer from CO 2 generation as a byproduct 1 and a high energy consumption rate which leads to low exergy efficiency (43.2%). 11 A novel HCHO production method through direct CO hydrogenation in the aqueous phase using Ru−Ni/Al 2 O 3 was recently introduced, which could potentially increase the exergy efficiency with no CO 2 production, 12 as a result of bypassing the production of methanol and also the much lower reaction temperatures. However, it was not clear how the reaction proceeds in the aqueous phase. Although th...

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“…It is difficult to activate the relatively inert methane on the surface of a catalyst to make formaldehyde, considering the weak chemisorption of methane on the catalyst surface (Michalkiewicz et al 2008). Methane oxidation [eq.…”

Section: Formaldehyde Production From Methanementioning

confidence: 99%

Critical review and exergy analysis of formaldehyde production processes

Bahmanpour

Hoadley

Tanksale

2014

Reviews in Chemical Engineering

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AbstractFormaldehyde is one of the most important intermediate chemicals and has been produced industrially since 1889. Formaldehyde is a key feedstock in several industries like resins, polymers, adhesives, and paints, making it one of the most valuable chemicals in the world. However, not many studies have been dedicated to reviewing the production of this economically important product. In this review paper, we study the leading commercial processes for formaldehyde production and compare them with recent advancements in catalysis and novel processes. This paper compares, in extensive detail, the reaction mechanisms and kinetics of water ballast process (or BASF process), methanol ballast process, and Formox process. The thermodynamics of the reactions involved in the formaldehyde production process was investigated using HSC Chemistry™ software (Outotec Oyj, Espoo, Finland). Exergy analysis was carried out for the natural gas to methanol process and the methanol ballast process for formaldehyde production. The former process was simulated using Aspen HYSYS™ and the latter using Aspen Plus™ software (Aspen technology, Burlington, MA, USA). The yield and product specifications from the simulation results closely matched with published experimental data. The exergy efficiencies of the natural gas to synthesis gas

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Selective methane oxidation to formaldehyde using polymorphic T-, M-, and H-forms of niobium(V) oxide as catalysts

Cited by 30 publications

References 41 publications

Nanostructured Nb₂O₅catalysts

Nanostructured Nb₂O₅catalysts

Hydrogenation of Carbon Monoxide into Formaldehyde in Liquid Media

Critical review and exergy analysis of formaldehyde production processes

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Selective methane oxidation to formaldehyde using polymorphic T-, M-, and H-forms of niobium(V) oxide as catalysts

Cited by 30 publications

References 41 publications

Nanostructured Nb2O5catalysts

Nanostructured Nb2O5catalysts

Hydrogenation of Carbon Monoxide into Formaldehyde in Liquid Media

Critical review and exergy analysis of formaldehyde production processes

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Product

Resources

About

Nanostructured Nb₂O₅catalysts

Nanostructured Nb₂O₅catalysts