Selective oxidation of alcohols over Si3N4-supported silver catalysts

Блохина, А. С.; Курзина, И. А.; Соболев, В. И.; Koltunov, Konstantin Yu.; Mamontov, G. V.; Vodyankina, O. V.

doi:10.1134/s0023158412040015

Cited by 20 publications

(7 citation statements)

References 10 publications

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“…It is clear that in the presence of oxygen, catalytic activity, but not selectivity, is much higher. Notably, such catalytic behaviour is very consistent with that for supported gold and other noble metal catalysts [39,[43][44][45], which was mainly due to the direct involvement of atomic or molecular oxygen species in reaction with ethanol [43] or due to shifting the equilibrium in the dehydrogenation of ethanol through the hydrogen oxidation [39]. Likewise, Co@NC materials, largely known as active catalysts in the oxygen reduction reaction (ORR) [23][24][25], induce an efficient generation of reactive oxygen species due to the surface mono-atomic Co active sites in pyridinic and pyrrolic environment [25,46].…”

Section: Gas-phase Catalytic Reactions Of Ethanol In a Flow Reactorsupporting

confidence: 81%

Ethanol Dehydrogenation to Acetaldehyde over Co@N-Doped Carbon

et al. 2021

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Cobalt and nitrogen co-doped carbon materials (Co@CN) have recently attracted significant attention as highly efficient noble-metal-free catalysts exhibiting a large application range. In a similar research interest, and taking into account the ever-increasing importance of bioethanol as a renewable raw material, here, we report the results on ethanol dehydrogenation to acetaldehyde over Co@NC catalysts. The catalyst samples were synthesized by a variety of affordable techniques, ensuring generation of various types of Co species incorporated in carbon, such as subnanosized cobalt sites and nano-sized particles of metallic cobalt and cobalt oxides. The catalytic activity was tested under both oxidative and non-oxidative gas-phase conditions at 200–450 °C using a fixed-bed flow reactor. The non-oxidative conditions proved to be much more preferable for the target reaction, competing, however, with ethanol dehydration to ethylene. Under specified reaction conditions, ethanol conversion achieved a level of 66% with 84% selectivity to acetaldehyde at 400 °C. The presence of molecular oxygen in the feed led mainly to deep oxidation of ethanol to COx, giving acetaldehyde in a comparatively low yield. The potential contribution of carbon itself and supported cobalt forms to the observed reaction pathways is discussed.

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Section: Gas-phase Catalytic Reactions Of Ethanol In a Flow Reactorsupporting

confidence: 81%

Ethanol Dehydrogenation to Acetaldehyde over Co@N-Doped Carbon

et al. 2021

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“…Taking into account that the oxidation processes are exothermal, a heat exchange between the reagent flow and the catalyst surface as well as between the active species (Ag NPs) and the support influences significantly on the state of active surface and the ratio between selective and nonselective stages. Blokhina et al [56] studied the ethanol oxidation over the Si 3 N 4 -supported silver catalyst with a low specific surface area and unique thermal conductivity. The Ag NPs with sizes below 30 nm were uniformly distributed over the surface of Si 3 N 4 after calcination of the catalysts at 500 • C in air.…”

Section: Ethanolmentioning

confidence: 99%

Ag-Based Catalysts in Heterogeneous Selective Oxidation of Alcohols: A Review

et al. 2018

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Alcohols (bioalcohols) is a class of chemicals that are used as a feedstock for the manufacturing of a large number of valuable intermediates in industrially important processes. Currently, sustainable technologies for selective conversion of alcohols utilize “green” oxidants, mainly, ambient air or oxygen. Due to the high affinity of oxygen towards silver, the latter serves as an active component of supported heterogeneous catalysts. In this review, we consider Ag-based catalysts that participate in gas- or liquid-phase oxidation of alcohols. Oxidation of methanol, ethanol, ethylene glycol, propylene glycol, glycerol, benzyl and allyl alcohols is mostly considered. A particular attention is paid to selective photooxidation of alcohols over Ag-based catalysts. We discuss the catalyst composition in terms of (1) the state of the active component, (2) the nature of the substrate, (3) support nature, and (4) the strength of the metal–support interactions.

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“…Due to this attractiveness, different catalyst systems have been studied for ethanol ODH. The main classes of investigated catalysts are supported metal oxides, mainly supported VO x , [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24] mixed metal oxides, [25,26] supported metal catalysts [27][28][29][30] or carbon-based catalysts. [31][32][33] Supported vanadium oxide catalysts show high activity in the ODH of ethanol.…”

Section: Introductionmentioning

confidence: 99%

Activity, Selectivity and Initial Degradation of Iron Molybdate in the Oxidative Dehydrogenation of Ethanol

et al. 2022

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Iron molybdate catalysts are applied in the industrial FormOx process to produce formaldehyde by oxidative dehydrogenation (ODH) of methanol. Only few studies are available about the applicability of iron molybdate catalysts for the ODH of ethanol to produce acetaldehyde. Herein, an iron molybdate synthesized by co-precipitation (p) and an iron molybdate prepared by a ball-milling solid-state synthesis (bm) are applied as ethanol ODH catalysts. Both materials show attractive acetaldehyde selectivites of > 90 % (280 °C: p-Fe 2 (MoO 4 ) 3 : Y AcH = 90.3 %; bm-Fe 2 (MoO 4 ) 3 : Y AcH = 60.4 %) and a stable performance.The bulk composition and crystal structure could be confirmed by various characterization techniques and is maintained during ethanol ODH. XPS reveals an enrichment of Mo on the catalyst surface which is slightly decreasing after the catalytic tests. This observation could be a first sign of long-term deactivation like known from methanol ODH. Comparing the performance of both materials, p-Fe 2 (MoO 4 ) 3 shows higher activity and aldehyde selectivity. We propose the higher Mo/Fe surface ratio and the lower acidity to be the reasons for these differences.

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Selective oxidation of alcohols over Si3N4-supported silver catalysts

Cited by 20 publications

References 10 publications

Ethanol Dehydrogenation to Acetaldehyde over Co@N-Doped Carbon

Ethanol Dehydrogenation to Acetaldehyde over Co@N-Doped Carbon

Ag-Based Catalysts in Heterogeneous Selective Oxidation of Alcohols: A Review

Activity, Selectivity and Initial Degradation of Iron Molybdate in the Oxidative Dehydrogenation of Ethanol

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