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Method for synthesizing methanol at low temperatures

A technology for synthesizing methanol at low temperature, which is applied in chemical instruments and methods, preparation of organic compounds, preparation of hydroxyl compounds, etc. It can solve the problems of reaction temperature limitation, achieve good stability, avoid sintering phenomenon, and be easy to prepare.

Active Publication Date: 2018-11-13
XIAMEN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] Some recent reports employ non-Cu catalysts for CO 2 Hydrogenation reaction results, such as In 2 o 3 (Martin et al., Angew. Chem. Int. Ed. 2016, 55, 1–6), ZnO-ZrO 2 (Wangetal, Science Advances2017, 3:e1701290), etc., have improved to a certain extent in terms of catalytic performance, especially catalyst stability, but the high methanol selectivity of these catalysts is only obtained at high space velocity
In addition, the reaction temperature is limited, and it is only catalytically active at high temperatures (above 300 degrees)

Method used

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  • Method for synthesizing methanol at low temperatures

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Experimental program
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Effect test

Embodiment 1

[0016] Weigh 0.5g of In with a particle size of 30-60 mesh 2 S 3 The catalyst was loaded into a fixed-bed reactor, and 10% H 2 -90% Ar mixed gas flow, at a pressure of 2bar and a space velocity of 3000mLh -1 g -1 Under certain conditions, the temperature was raised to 300°C for pretreatment of the catalyst for 1 hour, and then the temperature was lowered to 30°C. switch to CO 2 and H 2 The mixed gas atmosphere, where H 2 with CO 2 The volume ratio is 3:1, pressurized to 50bar, and the reaction space velocity is 10000mLh -1 g -1 , heated to 180°C for CO 2 Hydrogenation to methanol reaction. The reaction products were analyzed online by gas chromatography, and qualitative and quantitative analysis were performed by TCD and FID detectors, respectively. The specific reaction properties are listed in Table 1.

Embodiment 2

[0018] Weigh 0.5g of CoS catalyst with a particle size of 30-60 mesh and put it into a fixed-bed reactor, and feed 10%CO-90%N 2 Mixed air flow, at a pressure of 2bar and a space velocity of 2000mLh -1 g -1 Under certain conditions, the temperature was raised to 350°C for pretreatment of the catalyst for 1 hour, and then the temperature was lowered to 30°C. switch to CO 2 and H 2 The mixed gas atmosphere, where H 2 with CO 2 The volume ratio is 3:1, pressurized to 50bar, and the reaction space velocity is 5000mLh -1 g -1 , heated to 180°C for CO 2 Hydrogenation to methanol reaction. The reaction products were analyzed online by gas chromatography, and qualitative and quantitative analysis were performed by TCD and FID detectors, respectively. The specific reaction properties are listed in Table 1.

Embodiment 3

[0020] Weigh 0.5g of MoS with a particle size of 30-60 mesh 2 The catalyst was loaded into a fixed-bed reactor, and 10% H 2 -90%N 2 Mixed air flow, at a pressure of 1bar and a space velocity of 3000mLh -1 g -1 Under certain conditions, the temperature was raised to 300°C for pretreatment of the catalyst for 1 hour, and then the temperature was lowered to 30°C. switch to CO 2 and H 2 The mixed gas atmosphere, where H 2 with CO 2 The volume ratio is 3:1, pressurized to 50bar, and the reaction space velocity is 3000mLh -1 g -1 , heated to 180°C for CO 2 Hydrogenation to methanol reaction. The reaction products were analyzed online by gas chromatography, and qualitative and quantitative analysis were performed by TCD and FID detectors, respectively. The specific reaction properties are listed in Table 1.

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Abstract

The invention discloses a method for synthesizing methanol at the low temperatures, and relates to methanol synthesis. The method includes carrying out heating pretreatment on catalysts in reducing gas atmosphere; cooling the catalysts until the temperatures of the catalysts reach the room temperature, then switching the catalysts into carbon dioxide and hydrogen mixed atmosphere and carrying outreaction for preparing the methanol by means of carbon dioxide hydrogenation. The method has the advantages that the excellent catalytic performance for preparing the methanol by means of carbon dioxide hydrogenation is displayed, conditions are mild, and products are high in selectivity; the CO2 conversion rate can reach 15% under low-temperature reaction conditions, and the selectivity of the methanol can reach 90% at least under the low-temperature reaction conditions; the catalysts are sulfide or metal oxide or supported catalysts with the sulfide or the metal oxide, sintering phenomena can be prevented in reaction procedures, and the stability of the catalysts can be improved; the catalysts are pretreated in the reducing atmosphere, active sites of the catalysts can be positioned in unsaturated coordination environments to a certain extent, accordingly, the catalysts are high in carbon dioxide activation ability, and selective generation of the methanol can be promoted; proceduresfor preparing the catalysts are simple and controllable, and expanded preparation can be facilitated.

Description

technical field [0001] The invention relates to the synthesis of methanol, in particular to a method for synthesizing methanol at low temperature by using a catalyst treated in a reducing atmosphere to carry out hydrogenation of carbon dioxide to produce methanol. Background technique [0002] CO 2 It is one of the culprits of global warming. As an extremely chemically inert substance, it is difficult to be activated at low temperatures. Methanol is considered CO 2 The ideal product of hydrogenation can be used as hydrogen storage material or chemical raw material. However, via CO 2 Hydrogenation of methanol is limited by many factors: at high temperature, CO 2 The reaction of hydrogenation to methanol is thermodynamically unfavorable and accompanied by severe reverse water gas shift (RWGS) side reactions, resulting in the production of large CO by-products; at low temperatures, CO 2 difficult to be activated. For a long time, Cu-based catalysts have been considered as...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C07C29/153C07C29/156C07C31/04
CPCC07C29/153C07C29/156C07C31/04Y02P20/52
Inventor 康金灿胡景庭成康邓浇张庆红邓德会王野
Owner XIAMEN UNIV
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