16 results about "Oxidative carbonylation" patented technology

The invention provides a ZIF-derived Co-P catalyst and a preparation method thereof. The catalyst can be used for synthesizing dimethyl carbonate through oxidative carbonylation of methanol. The ZIF-derived Co-P catalyst disclosed by the invention is prepared by roasting a precursor P-doped Zn / Co-ZIF intermediate. Compared with a traditional cobalt-based catalyst, the Co-P catalyst prepared through roasting treatment modification can regulate and control the variety and coordination number of heteroatoms, improve the interaction between metal and a carrier and effectively anchor metal atoms, and meanwhile P atoms can serve as second active sites to assist in improving the adsorption and activation capacity of reactants and intermediate species. In addition, the ZIF generates a hierarchical pore structure in the roasting treatment process, so that the mass transfer and diffusion processes of reactants and products are effectively promoted. According to the Co-P catalyst disclosed by the invention, the methanol oxidative carbonylation reaction activity is remarkably improved, and the catalyst has high stability.

The invention discloses a preparation method and application of a high-nitrogen-doped ordered mesoporous carbon supported copper catalyst, and belongs to the technical field of catalyst preparation. The preparation method comprises the following steps: by taking cane sugar and a copper-nitrogen complex as raw materials, SBA-15 as a template agent and sulfuric acid as a catalyst, carrying out equivalent-volume impregnation, low-temperature heat treatment, 800-900 DEG C high-temperature carbonization and nitric acid / hydrofluoric acid demolding to prepare pyrrole nitrogen enriched or pyridine nitrogen enriched high-nitrogen doped ordered mesoporous carbon with a large specific surface area; the preparation method comprises the following steps: loading a copper species on high-nitrogen-doped ordered mesoporous carbon by adopting an equivalent-volume impregnation method, and reducing at 350-400 DEG C to prepare the high-nitrogen-doped ordered mesoporous carbon loaded copper catalyst. The prepared catalyst is high in nitrogen content, large in specific surface area, high in pyridine nitrogen or pyrrole nitrogen enrichment degree and uniform in copper particle dispersion and shows efficient catalytic performance in methanol oxidative carbonylation reaction, and the highest methanol conversion rate is 9.3%.

The invention discloses a method for synthesizing alkyl carbonate through gas-phase carbonylation. Comprising a dechlorination method and a chlorine circulation process in the process of preparing alkyl carbonate through a gas-phase oxidative carbonylation reaction of carbon monoxide and alkyl nitrite. The content of water and alkyl alcohol in circulating gas is controlled through solvent absorption, alkyl chloride is synthesized with a chlorine supplementing agent HCl and alkyl chloroformate under the action of a dechlorinating agent, and the alkyl chloride is separated from a product through gas-liquid separation. When alkyl carbonate is produced by adopting the dechlorination method and the dechlorination process, the problem of equipment corrosion caused by chlorides can be avoided, the dechlorination process is a low-cost and environment-friendly chlorine circulation process, and stable operation of an industrial device is realized.

The present invention relates to a catalyst for methanol liquid phase oxidative carbonylation to synthesize dimethyl carbonate, and its preparation method and application. The catalyst is a MOFs derivative, and the metal oxide is dispersed on a carbon carrier. The metal oxide is CuO X The MOFs derivative is CuO obtained by calcining Cu-MOF. X Dispersed on a carbon support, the MOF derivative is used in an amount of 1.3% to 3.8% of the amount of methanol used. Compared to existing technologies, this invention leverages the advantages of MOFs, such as adjustable metal nodes and ligand structures, large specific surface area, and diverse structures. The resulting derivatives after calcination also have the advantages of high specific surface area and highly dispersed metal oxides on the carbon support.

The invention discloses a chloride-free copper catalyst, a preparation method and application, and belongs to the technical field of catalysts. The invention solves the problem of how to provide a chloride-free copper catalyst with high conversion rate and high space time yield. The invention relates to a nitrogen-containing three-dimensional interconnected layered porous carbon material loaded with a copper active component, which is prepared by the following steps: mixing a nitrogen-containing biomass derivative with an additional nitrogen source, adding a proper amount of a pore-forming agent, carbonizing the formed mixture at 500-900 DEG C for 0.5-4 hours, impregnating the loaded copper active component by a wet method, and reducing at high temperature of 200-500 DEG C to obtain the nitrogen-containing three-dimensional interconnected layered porous carbon material. SEM characterization and N2 adsorption and desorption characterization show that the catalyst has a hierarchical porous structure and a high specific surface area; when the finally obtained catalyst is used for catalyzing liquid-phase methanol oxidative carbonylation to synthesize dimethyl carbonate, the conversion rate of methanol can be up to 18.19%, the selectivity of dimethyl carbonate can be up to 97.94%, and the space time yield can be up to 25.69 g. (g.h) <-1 >.

This invention relates to a (FeIn) / ZSM-5 catalyst, comprising a ZSM-5 molecular sieve support and an active component supported on the ZSM-5 molecular sieve; the active component is a Fe species and an In species, with the Fe loading in the catalyst being 0.1~1.0 wt% and the In loading being 0.25~1.5 wt%. The invention also discloses a method for preparing the catalyst and its applications. This invention employs a "molecular anchoring" strategy, introducing a second metal, indium. Utilizing the stronger electronic interaction between indium and aluminum in the molecular sieve framework, the migration and aggregation of iron during preparation and reaction are effectively suppressed, significantly increasing the proportion of mononuclear iron in the (FeIn) / ZSM-5 catalyst and promoting the yield of the target product, acetic acid, in the methane oxidative carbonylation reaction.

The invention belongs to the field of medicinal chemistry, and discloses a novel method for preparing lisethopran (7-(4, 7-diazaspiro [2.5] octane-7-yl)-2-(2, 8-dimethyl imidazo [1, 2-b] pyridazine-6-yl) pyrido [1, 2-a] pyrimidine-4-ketone). The method comprises the following steps: taking 3-amino-6-pyridazine as an initial raw material, carrying out oxidative carbonylation, bromination, cyclization, Suzuki coupling methylation and Claisen ester condensation reaction in which carbon monoxide is catalyzed by palladium to obtain a key intermediate 3-(2, 8-dimethyl imidazo [1, 2-b] pyridazine-6-yl)-3-oxoethyl propionate, and carrying out reaction on the key intermediate 3-(2, 8-dimethyl imidazo [1, 2-b] pyridazine-6-yl)-3-oxoethyl propionate and 3-(2, 8-dimethyl imidazo [1, 2-b] pyridazine-6-yl)-3-oxoethyl propionate to obtain a target product. The preparation method comprises the following steps: carrying out condensation, Buchwald-Hartwisting reaction and deprotection on 4-(2, 2-b) pyridazine-6-yl)-3-oxoethyl propionate to obtain a final product. The method is high in yield, low in cost, simple and convenient to operate and high in application value.

The invention provides a preparation method of an iron-based catalyst. The catalyst has high activity and high selectivity in a reaction for synthesizing dimethyl carbonate (DMC) through methanol oxidative carbonylation. The catalyst is formed by roasting a ZIF-derived iron-based catalyst precursor, and the valence state, the particle size, the texture property and the like of Fe species can be adjusted by changing the atomic ratio of iron and zinc metal, carbonization conditions and the like in the preparation process, so that the catalytic performance of the catalyst is adjusted and controlled. Compared with a traditional copper-based catalyst, the selectivity of the iron-based catalyst to DMC reaches up to 99% or above, the preparation raw materials are cheap and easy to obtain, and meanwhile the catalyst can be separated and recycled through magnetic separation.

The present invention relates to a method for synthesizing a dehydrorutaecarpine compound using an electrochemical oxidative carbonylation reaction. This method uses aniline and 1-bromo-9H-pyrido[3,4-b]indole as the starting materials to successfully construct the dehydrorutaecarpine compound through a two-step arylation and electrochemical oxidative carbonylation reaction. This method features readily available starting materials, concise synthetic steps, mild reaction conditions, and a simple operating procedure.

This invention discloses a method for the direct oxidative carbonylation of methane to prepare acetic acid. Specifically, this invention provides a catalytic method for the preparation of acetic acid from methane, comprising the following steps: under solvent conditions, in the presence of light, an iron catalyst, chloride ions, and an oxidant, methane and carbon monoxide undergo a methane oxidative carbonylation reaction to obtain acetic acid. This method utilizes readily available methane, carbon monoxide, and air (or oxygen), employs an iron catalyst, and achieves direct, efficient, and highly selective acetic acid production via a one-step photocatalytic reaction, demonstrating promising application prospects. The substrate scope of this invention is broad, applicable to a range of chain and cyclic alkanes.

The invention relates to a preparation method and application of a cellulose-derived porous carbon supported copper catalyst, and belongs to the technical field of catalyst preparation. The preparation method comprises the following steps: taking microcrystalline cellulose as a raw material, dipping and activating the microcrystalline cellulose in a zinc salt solution, carbonizing the microcrystalline cellulose at a high temperature of 900-1000 DEG C and washing the microcrystalline cellulose with nitric acid to prepare cellulose-derived porous carbon as a catalyst carrier, obtaining a micropore-rich carbon material containing mesopores by using zinc nitrate, and obtaining the micropore-rich carbon material by using zinc chloride; and loading a copper species on the catalyst carrier by adopting an equivalent-volume impregnation method, and reducing at 350-400 DEG C to obtain the cellulose-derived porous carbon loaded copper catalyst. The prepared cellulose-derived porous carbon supported copper catalyst has the advantages of large specific surface area, high dispersion of copper particles and the like, and shows excellent catalytic performance in the reaction of catalyzing methanol oxidative carbonylation to synthesize dimethyl carbonate, the highest methanol conversion rate can reach 9.0%, and the selectivity of dimethyl carbonate is 98% or above.

The invention discloses a catalyst for producing aryl acetic acid through oxidative carbonylation of methyl aromatic hydrocarbon and a preparation method and application of the catalyst, the catalyst is composed of solid acid and metal oxide for modifying the solid acid, the metal oxide is an oxide corresponding to the highest valence of metal, and the metal is one of cobalt, nickel, copper and iron elements; the mass of the catalyst is 100%, the metal oxide accounts for 0.1-20% of the mass of the catalyst, and the balance is the solid acid. The catalyst provided by the invention is simple to synthesize, is beneficial to large-scale preparation, and has good activity and stability; when aryl acetic acid is produced, a fixed bed reactor is adopted, operation is easy, continuous and large-scale production is facilitated, and the reaction process is high in atom economy and environmentally friendly.

The invention discloses a preparation method of a catalyst for preparing dimethyl carbonate through oxidative carbonylation of methanol. The catalyst comprises the following components (in terms of oxide, a carrier is 85.0 to 92.5 wt% of Al2O3, 5.0 to 11.0 wt% of MgO, 0.1 to 1.0 wt% of Na2O, 1.5 to 3.5 wt% of a Cu-containing compound and 0.5 to 1.5 wt% of a Pd-containing compound. Alpha-beta aluminum oxide added during molding reduces the acidity of the carrier and improves the heat-conducting property of the carrier, and a magnesium-containing compound is added before strip extrusion to modify the carrier, so that the structural stability and the mass transfer property of the catalyst are improved. The catalyst prepared by adopting the technology of the patent is weak in acidity, high in active component dispersity and smooth in catalyst pore channel, and has excellent activity and selectivity when being used for preparing a dimethyl carbonate catalyst through methanol oxidative carbonylation.

The invention discloses a preparation method and application of a nitrogen-doped micro-mesoporous carbon supported copper catalyst, and belongs to the technical field of catalyst preparation. The preparation method comprises the following steps: S1, by taking hexamethylenetetramine (HTMA) and a mesoporous molecular sieve SBA-15 as raw materials, mixing and performing high-temperature carbonization (900-1300 DEG C) to prepare a micro-mesoporous high-specific-surface-area high-nitrogen-doped carbon carrier, the total specific surface area reaches 783 m < 2 > / g or above (the mesopore proportion is 71% or above), and the nitrogen content reaches 1.6 wt% during carbonization at 1300 DEG C; and S2, immobilizing a copper species on the nitrogen-doped carbon carrier in the S1 by adopting an impregnation method to prepare the nitrogen-doped carbon supported copper catalyst. The prepared catalyst is high in nitrogen content and shows excellent catalytic performance in methanol oxidative carbonylation reaction, experimental operation is simple, and an experimental basis is provided for research of nitrogen-doped carbon materials.

The invention discloses a cobalt-based catalyst and a preparation method and application thereof, the cobalt-based catalyst is obtained by at least taking a cobalt-based precursor and an organic nitrogen source as raw materials through in-situ carbonization treatment; wherein the raw materials of the cobalt-based precursor at least comprise a cobalt salt, a zinc salt and an imidazole organic ligand. The preparation method comprises the following steps: dissolving cobalt salt and zinc salt in water to obtain a metal salt aqueous solution; the preparation method comprises the following steps: dissolving an imidazole organic ligand in water to obtain an imidazole organic ligand aqueous solution; the preparation method comprises the following steps: mixing a metal salt aqueous solution and an imidazole organic ligand aqueous solution, heating, aging, collecting a solid product, washing and drying to obtain a catalyst precursor; and mixing the catalyst precursor with an organic nitrogen source, and carrying out in-situ carbonization treatment to obtain the catalyst. The cobalt-based catalyst shows excellent catalytic activity and selectivity in the methanol oxidative carbonylation reaction, has good reaction stability, can still keep high methanol conversion rate and DMC selectivity after being recycled for five times, and has good industrial application potential.

A catalyst for oxidative carbonylation of methanol to obtain dimethyl carbonate, a preparation method and applications thereof are disclosed. The catalyst includes a carrier being a porous carbon-nitrogen material, and an active component being Cu, where the weight of Cu accounts for 5-15 wt % of the total weight of the catalyst. The catalyst exhibits good catalytic activity in the reaction of methanol oxidative carbonylation to synthesize dimethyl carbonate, has high space-time yield and selectivity, and the catalyst and the product are easy to separate.