Method for preparing liquid hydrocarbon by directly hydrogenating through carbon dioxide
A technology for carbon dioxide and liquid hydrocarbons, applied in chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, preparation of liquid hydrocarbon mixtures, etc., to achieve important commercial value, excellent recycling performance, and solve environmental and resource problems problem effect
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Embodiment 1
[0053] Preparation and characterization of embodiment 1, cobalt-based bimetallic catalyst
[0054] co 6 MnO x Catalyst preparation: Co(NO 3 ) 2 ·6H 2 O(0.873g,3.0mmol) and Mn(NO 3 ) 2 4H 2 O (0.125g, 0.5mmol) was dissolved in 40mL deionized water, and stirred for 1 hour to obtain a solution of the bimetallic salt. Gradually drop the above solution into 100mL Na under stirring within 1 hour 2 CO 3 solution (0.5 mol / L), continued to stir for 3 hours, and then centrifuged to obtain a solid powder. The powder was washed with 500 mL of deionized water, dried at 110°C for 10 hours, then calcined at 400°C for 3 hours, then reduced in a hydrogen stream at 400°C for 1 hour, and finally inerted at room temperature for 30 hours in nitrogen containing 1% oxygen. Minutes to avoid the failure of the prepared catalyst to burn in the air. After the above steps, Co 6 MnO x catalyst. The catalysts with Co / Mn molar ratios of 2, 10 and 14 were obtained by adjusting the Co(NO 3 ) 2...
Embodiment 2
[0058] Embodiment 2, catalytic system screening
[0059] The preparation steps of liquid hydrocarbons are as follows: the carbon dioxide hydrogenation reaction is carried out in a 16 ml stainless steel reactor with a tetrafluoro liner. Add 20 mg of catalyst and 1 mL of solvent (20 g / L) into the reactor, close the reactor, and replace it with 1 MPa of carbon dioxide three times. Before the reaction, fill in 4 MPa of carbon dioxide and 4 MPa of hydrogen at room temperature, heat the reactor to 200 ° C, and start After reacting for 15 hours, stop the reaction, and the preparation of liquid hydrocarbons is completed. Put the reactor into an ice-water bath to cool down, release the gas slowly and collect it in an air bag, and analyze it in a gas chromatograph. The reaction mother liquor was also analyzed by gas chromatography with toluene as internal standard. The gas-liquid samples are also supplemented by GC-MS for qualitative analysis.
[0060] Based on the above preparation ...
Embodiment 3
[0064] Embodiment 3, reaction condition optimization
[0065] Based on preferred Co 6 MnO x Catalyst and squalane solvent, optimized reaction condition, other conditions except variable are identical with the experiment of serial number 1 in table 2. Figure 8 A shows the effect of temperature on reactivity and selectivity. The reaction can be carried out at 140 °C, which is much lower than the reaction temperature reported in the current literature. As the temperature gradually increased up to 200 °C, the reactivity and liquid product selectivity also increased significantly. Further increasing the reaction temperature, the improvement of catalytic performance becomes less obvious. Therefore, 200°C is a more suitable reaction temperature, and this temperature is also the lowest temperature reported so far for the synthesis of liquid fuels by hydrogenation of carbon dioxide. At 200°C, the influence of the partial pressure ratio of carbon dioxide and hydrogen was observed,...
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