A kind of method for synthesizing higher alcohol by catalytic conversion of ethanol

A technology for catalytic conversion and higher alcohols, applied in chemical instruments and methods, preparation of organic compounds, carbon-based compounds, etc., can solve the problems of complex catalyst preparation, high price, unfavorable preparation and application, etc., and achieve excellent stability, Effects of low cost, increased selectivity and ethanol conversion

Active Publication Date: 2022-07-22
ZHEJIANG UNIV OF TECH +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

Recently, the research group of the present invention also applied the metal-organic framework-confined nano-Pd catalyst (Pd@UiO-66) to the reaction of ethanol dehydrogenation condensation to n-butanol, and achieved up to 38.7% C4 under the conditions of 250 ° C and 2 MPa -C8 alcohol yield, but the preparation of the catalyst is complicated, expensive, and 13.9% cracked products are produced, so it is also unfavorable for its large-scale preparation and application [CN108636453 B; ACS Catal., 2018, 8, 11973-11978 ]

Method used

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  • A kind of method for synthesizing higher alcohol by catalytic conversion of ethanol
  • A kind of method for synthesizing higher alcohol by catalytic conversion of ethanol
  • A kind of method for synthesizing higher alcohol by catalytic conversion of ethanol

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0069] 0.7603g copper nitrate (Cu(NO 3 ) 2 ·3H 2 O) and 0.4555g cerium nitrate (Ce(NO) 3 ) 3 ·6H 2 O) was added to 10ml of absolute ethanol, after it was dissolved and mixed uniformly, 2g of alumina carrier (specific surface was 291m 2 / g, the average pore size is 10.1 nm, and the pore volume is 0.74 mL / g). The above mixture was dried on a rotary evaporator at 50 °C and 0.09 MPa for 3 h, and then dried at 80 °C and 0.09 MPa for 2 h. The dried solid matter was calcined in a muffle furnace at 450 °C for 3 h in an air atmosphere, and then calcined in a tube furnace or fixed bed reactor with 10% H 2 / N 2 Mixed gas at 500 ℃, gas air velocity 1800h -1 The catalyst I-a is obtained by reducing under the condition for 6h. The weight content of its metal Cu is 8.4wt%, CeO 2 The loading amount is 7.6wt%, and the rest is alumina carrier. The surface element composition and valence state of the catalyst were analyzed by X-ray fluorescence spectroscopy (XPS) characterization tech...

Embodiment 2

[0072] The preparation method of catalyst I-b is the same as in Example 1, but copper nitrate (Cu(NO) 3 ) 2 ·3H 2 O) and cerium nitrate (Ce(NO) 3 ) 3 ·6H 2 The masses of O) were 0.6083 g and 0.4555 g, respectively. The weight content of its metal Cu is 6.8 wt%, CeO 2 The weight content is 7.7wt%, and the rest is alumina carrier. The surface element composition and valence state of the catalyst were analyzed by XPS characterization technology, and it was proved that in the reduced catalyst, cerium was replaced by CeO. 2 form, while the copper active component exists in the form of +1-valent Cu and zero-valent Cu, and Cu 0 / Cu + The ratio (molar ratio) was 1:6.9.

[0073] Continuous catalytic conversion of ethanol to synthesize higher alcohol fixed bed reactor such as Figure 5 As shown, 1 g of catalyst I-b was weighed and loaded into Figure 5 In the isothermal zone of the reaction tube of the fixed bed reactor shown. Under the set reaction conditions, with N 2 The...

Embodiment 3

[0075] 0.7603g copper nitrate (Cu(NO 3 ) 2 ·3H 2 O) and 0.4542g lanthanum nitrate (La(NO) 3 ) 3 ·6H 2 O) was added to 10 ml of absolute ethanol, and after it was dissolved and mixed uniformly, 2 g of alumina carrier was added to it for immersion for 4 hours. The above mixture was dried on a rotary evaporator at 50°C and 0.09MPa for 3h, and then dried at 80°C and 0.09MPa for 2h. The dried solid matter was calcined in a muffle furnace at 450 °C for 3 h in an air atmosphere, and then calcined in a tube furnace or fixed bed reactor with 10% H 2 / N 2 Mixed gas at 500 ℃, gas air velocity 1800h-1 The catalyst I-c was obtained by reduction under conditions for 6 h. The weight content of its metal Cu is 8.4wt%, La 2 O 3 The weight content is 7.7wt%, and the rest is alumina carrier. The surface element composition and valence state of the catalyst were analyzed by XPS characterization technology, and it was proved that in the reduced catalyst, lanthanum was replaced by La. 2 ...

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Abstract

The invention discloses a method for synthesizing higher alcohol by catalytic conversion of ethanol. The method takes ethanol as a raw material, and reacts under the action of a catalyst to generate higher alcohol. It is characterized in that: the catalyst has a mass ratio of 1:10~ The uniform mixture of catalyst I and catalyst II of 10:1, the catalyst I is a solid catalyst for ethanol dehydrogenation and condensation to generate higher alcohols, and the catalyst II is a catalyzed aldehyde or ketone containing α-H to generate a hydroxyl group. The solid catalyst with aldehyde condensation reaction function introduces more aldol condensation active centers on the basis of catalyst I, and the two synergistically catalyze the conversion of ethanol to form higher alcohols. The invention simultaneously improves the higher alcohol selectivity and the ethanol conversion rate, and finally realizes the efficient conversion of ethanol to higher alcohol under relatively mild reaction conditions, and no small molecule cracking products are produced; and the catalyst has excellent stability.

Description

(1) Technical field [0001] The invention relates to a method for synthesizing higher alcohols (mainly including C4-C8 alcohols) by catalytic conversion of ethanol. (2) Background technology [0002] Using bioethanol as a gasoline additive can increase gasoline octane while reducing greenhouse gas emissions, so it is generally accepted in the United States, China, Brazil and some European countries. However, ethanol has problems such as strong hygroscopicity and low energy density, so it is not an ideal gasoline blending component. Bio-butanol produced by upgrading bio-ethanol has higher calorific value and low corrosiveness, and can be used directly without modification of the engine, thus becoming a more ideal bio-fuel than bio-ethanol. In addition, butanol is also an important chemical raw material for synthesizing dibutyl phthalate, butyl acrylate and other plastic / rubber plasticizers or coating / adhesive monomers. Industrial butanol mainly uses petroleum-based propylene...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C07C31/12C07C29/32C07C29/17B01J23/83B01J23/10B01J35/10
CPCC07C29/32C07C29/175C07C45/74C07C45/002B01J23/83B01J23/10B01J23/002B01J35/0006B01J35/1019B01J35/1061B01J35/1042C07C31/12C07C47/21C07C47/06Y02P20/52
Inventor 江大好沈昕悦胡晓利张继生侯圣国孟华胡皓森许孝良张群峰李小年
Owner ZHEJIANG UNIV OF TECH
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