CN113663623B - Synthetic method of liquid fuel by solar bionic catalysis - Google Patents
Synthetic method of liquid fuel by solar bionic catalysis Download PDFInfo
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- CN113663623B CN113663623B CN202010404233.3A CN202010404233A CN113663623B CN 113663623 B CN113663623 B CN 113663623B CN 202010404233 A CN202010404233 A CN 202010404233A CN 113663623 B CN113663623 B CN 113663623B
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J19/12—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electromagnetic waves
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
- C10L1/00—Liquid carbonaceous fuels
- C10L1/02—Liquid carbonaceous fuels essentially based on components consisting of carbon, hydrogen, and oxygen only
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
- C12P39/00—Processes involving microorganisms of different genera in the same process, simultaneously
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
- C12P5/00—Preparation of hydrocarbons or halogenated hydrocarbons
- C12P5/02—Preparation of hydrocarbons or halogenated hydrocarbons acyclic
- C12P5/023—Methane
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- C—CHEMISTRY; METALLURGY
- C12—BIOCHEMISTRY; BEER; SPIRITS; WINE; VINEGAR; MICROBIOLOGY; ENZYMOLOGY; MUTATION OR GENETIC ENGINEERING
- C12P—FERMENTATION OR ENZYME-USING PROCESSES TO SYNTHESISE A DESIRED CHEMICAL COMPOUND OR COMPOSITION OR TO SEPARATE OPTICAL ISOMERS FROM A RACEMIC MIXTURE
- C12P7/00—Preparation of oxygen-containing organic compounds
- C12P7/40—Preparation of oxygen-containing organic compounds containing a carboxyl group including Peroxycarboxylic acids
- C12P7/54—Acetic acid
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/10—Process efficiency
- Y02P20/133—Renewable energy sources, e.g. sunlight
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/59—Biological synthesis; Biological purification
Abstract
The invention discloses a synthetic method of bionic solar liquid fuel, which utilizes a combined technology that solar energy is utilized to efficiently convert carbon dioxide and water into liquid fuel under the synergistic effect of a photocatalyst and a biocatalyst; the method comprises the steps of performing advantage complementation on two reaction systems of chemical reaction and microbial electrosynthesis, realizing efficient conversion of carbon dioxide into liquid fuel by using a solar device, and finally converting the liquid fuel into electric energy and CO by using a fuel cell 2 The method realizes the effective circulation of carbon, is expected to solve the environmental problems of energy crisis, greenhouse effect and the like, and realizes the sustainable development of clean energy.
Description
Technical Field
The invention relates to the technical field of renewable clean energy utilization, in particular to a combined technology for efficiently converting carbon dioxide and water into liquid fuel under the synergistic effect of a photocatalyst and a biocatalyst by utilizing solar energy.
Background
With the gradual aggravation of problems such as global environmental pollution and energy shortage, the search for efficient clean energy to replace the existing fossil energy is the current research focus. The consumption of a large amount of traditional fossil energy sources such as coal, petroleum, natural gas and the like not only brings about the rapid reduction of energy reserves, but also causes serious environmental pollution problems, in particular to CO 2 The emission of the iso-greenhouse gases seriously threatens the ecological balance of the world. How to reduce the content in the atmosphere, alleviate the greenhouse effect and convert it into clean energy, and realizing the efficient utilization of renewable energy has attracted a great deal of attention. In recent years, CO has been produced by methods such as homogeneous and heterogeneous catalytic hydrogenation, inorganic photoelectrocatalysis, and pyrolysis 2 The technology of carbon capture and utilization for activation has made great progress to achieveCO (carbon monoxide) 2 Will convert methane, methanol and longer carbon chain alcohols and fatty acid ester polymers and other organic matters. CO 2 The biological fixation method can realize CO under mild conditions 2 Conversion utilization has more advantages than an inorganic catalytic method, wherein a microbial electrosynthesis method is the current research focus, and the production of organic matters such as methane, formic acid, acetic acid, butyric acid and the like by utilizing microbial electrosynthesis is realized at present. However, the current synthesis efficiency is far from high enough for the microbial electrosynthesis method to be widely popularized and applied in industrial production, and the main difficulty is the low metabolic rate of the microbial carbon fixation pathway and the low microbial extracellular electrode transfer. In order to promote the development and practical application of the microorganism electrosynthesis carbon fixation way and meet the industrial production requirement, the optimization of the reactor design and the combined utilization of various energy production means to improve the conversion efficiency are more effective means besides the transformation of the genetic way of microorganisms and the design of efficient electrode materials.
Solar energy is the most well-known alternative source of energy, and the solar energy is mainly utilized in the forms of photovoltaics, photo-thermal, green plants and the like. The photocatalytic organic synthesis can utilize solar energy to realize the conversion of organic matters under normal pressure, has been widely applied to organic synthesis reactions of amine-to-imine organic matters, alcohol-to-aldehyde organic matters and the like, and has good selectivity of products. However, the catalytic conversion of the organic synthesis is low, and it is still a great challenge to achieve efficient organic synthesis. Recently, the application scene of visible sunlight is greatly expanded by the proposal of the concept of 'liquid sunlight', and the purpose of the method is to extract renewable green liquid fuel from sunlight, carbon dioxide and water and convert the renewable green liquid fuel into storable and operable energy, but the 'liquid sunlight' still has a plurality of technical bottlenecks to break through in order to realize large-scale popularization and application in industry. At present, the photocatalytic reaction and the microbial electrosynthesis are reported to realize the conversion and reutilization of carbon dioxide, and the carbon dioxide is hopeful to be converted into usable liquid fuel while the concentration of the carbon dioxide in the atmosphere is reduced, however, the existing conversion efficiency is low and the method is applied to the industry on a large scale. In conclusion, the advantages of the two reaction systems are complemented, the solar device is utilized to realize the efficient conversion of carbon dioxide to liquid fuel, the environmental problems of energy crisis, greenhouse effect and the like are hopeful to be solved, and the sustainable development of clean energy is realized.
Disclosure of Invention
The invention complements advantages of two reaction systems of photocatalyst and bioelectricity synthesis, realizes high-efficiency conversion of carbon dioxide into liquid fuel by utilizing a solar device, and then converts the synthesized liquid fuel into electric energy and CO by using a fuel cell 2 An efficient cycle of carbon is achieved (principle see fig. 1).
To achieve the above objective, the synthesis process of liquid fuel is designed into two routes (see fig. 2):
(1) First route: the carbon dioxide firstly generates CO, formaldehyde and CH under the catalysis of the photocatalyst 4 And the like. In this step, different photocatalysts are selected to obtain different main products, such as BiVO 4 And zinc oxide, etc. to mainly convert CO 2 Reduction to methane, ti-based compounds mainly allows CO to be obtained 2 Catalytic reduction to formic acid, etc.; then, reasonably selecting microorganism/biological enzyme/bionic enzyme catalysts aiming at different intermediate products, and further catalyzing the intermediate products to generate liquid fuel end products such as methanol, ethanol and the like;
(2) The second route: firstly, adopting a bioelectricity synthesis method to selectively convert the catalyst into CO, formaldehyde and CH by utilizing a microorganism/biological enzyme/bionic enzyme catalyst 4 Etc., such as Clostridium (Clostridia) can be used as multifunctional acidogenic bacteria, and acetogenic bacteria (Sporoouma spp. And Moorella thermoacetica) can convert CO 2 Fixing to acetic acid and the like; and then the catalyst is selected to be converted into liquid fuel end products such as ethanol and the like.
The specific scheme is as follows:
method for synthesizing bionic solar liquid fuel, and CO is synthesized by combining photocatalysis reaction and microorganism electricity 2 Converted into liquid fuel.
The invention relates to a specific method for combined utilization, which comprises the steps of utilizing a photocatalyst I to fix carbon dioxide into an intermediate product, and then selecting the biocatalyst I capable of utilizing the intermediate product to convert the intermediate product into liquid fuel through microbial electrosynthesis;
or CO is synthesized by bioelectricity by using a biocatalyst II 2 Is converted into CO, formaldehyde and CH 4 Etc., and then using the photocatalyst II to make CO, formaldehyde and CH 4 Etc. to a liquid fuel.
As a preferable technical scheme of the invention, the intermediate product is CO, formaldehyde and CH 4 One or more of formic acid.
As a preferable technical scheme of the invention, the liquid fuel is methanol, ethanol and the like.
As a preferable technical scheme of the invention, the biocatalyst I can convert CO, formaldehyde and CH 4 One or more of a microorganism, a biological enzyme, or a biomimetic enzyme that converts to methanol and ethanol; the biocatalyst II is capable of converting CO 2 Is converted into CO, formaldehyde and CH 4 One or more of a microorganism, a biological enzyme, or a biomimetic enzyme, etc.
As a preferred embodiment of the present invention, the biocatalyst I includes, but is not limited to, methane-oxidizing bacteria, methanol dehydrogenase, aldose reductase, etc.; the biocatalyst II includes but is not limited to methanogen or acetogen; the acetobacter includes, but is not limited to Moorella thermoacetica, and the methanogen includes, but is not limited to, methanococcus equi (Methanococcus), methanosarcina (Methanono-sarcosina), methanobacterium ruminant (Methanobacterium), and the like.
As a preferable technical scheme of the invention, the photocatalyst I can reduce carbon dioxide to generate CO, formaldehyde and CH 4 The catalytic material is a noble metal or non-noble metal modified vanadium compound, a Ti-based compound or graphite phase carbon nitride;
the photocatalyst II can convert CO, formaldehyde and CH under the condition of room temperature 4 Catalytic material for converting into methanol or ethanol, wherein the catalytic material is noble metalOr a non-noble metal modified vanadium-based compound, a Ti-based compound, or a graphite-phase carbon nitride.
As a preferable technical scheme of the invention, the noble metal is one or more of Pt, ag, pd or Au; the non-noble metal is one or more of Cu, mg, co or Ni.
As a preferred embodiment of the present invention, the photocatalyst I includes, but is not limited to, a high temperature method and a deposition method on BiVO 4 Catalytic materials with Cu, mg, co, ni and other non-noble metal atoms doped on the surface of the substrate material; the photocatalyst II comprises, but is not limited to, cu, pt, pb and other doped polymer carbon nitride materials or silicon oxide supported transition metal phosphide and the like.
The invention has the beneficial effects that: the invention discloses a synthetic method of bionic solar liquid fuel, which comprises the technical field of complementary utilization of various renewable clean energy sources, in particular a multiple combination technology for efficiently converting carbon dioxide and water into liquid fuel under the synergistic effect of a photocatalyst and a biological enzyme catalyst by utilizing solar energy. The invention aims to complement advantages of two reaction systems of photocatalysis reaction and microbial electrosynthesis, and realize efficient conversion of carbon dioxide into liquid fuel by utilizing a solar device. Firstly, designing and synthesizing a proper photocatalyst to adapt to the high-energy catalysis of concentrating solar energy to realize the rapid reaction of organic synthesis; secondly, screening microbial catalysts in the microbial electrosynthesis reaction, and selectively converting carbon dioxide into organic matters such as methane, formaldehyde, formic acid and the like with high efficiency, or converting formic acid, formaldehyde and the like into ethanol and ester organic matters; finally, the photocatalyst and the microbial catalyst are effectively combined, the reaction sequence is adjusted according to the photocatalyst and the microbial catalyst, and the rapid fixed conversion of carbon dioxide and the efficient production of liquid fuel are realized under the help of solar energy.
Drawings
In order to make the objects, technical solutions and advantageous effects of the present invention more clear, the present invention provides the following drawings for description:
FIG. 1 is a schematic view of a cycle for effecting a fixed conversion of carbon dioxide to liquid fuel and then to electrical energy via a fuel cell in accordance with the present invention; the carbon dioxide and the water are efficiently converted into liquid fuels such as ethanol under the action of the photocatalyst and the biocatalyst, and the generated liquid fuels can be directly used as clean energy sources by a fuel cell, so that the rapid cycle of solar energy, chemical energy and electric energy is realized.
The synthetic process design roadmap for liquid fuels is shown in fig. 2.
Detailed Description
The present invention will be further described with reference to the accompanying drawings and specific examples, which are not intended to limit the invention, so that those skilled in the art may better understand the invention and practice it.
Example 1
In BiVO 4 The method is characterized in that a high-temperature method and a deposition method are adopted to dope non-noble metal atoms such as Ni, mg, cu and the like on the surface of the material as a photocatalyst, so that the surface electronic structure of the substrate material is adjusted to improve the photoelectrocatalysis performance of the substrate material, and the photocatalyst is further used for converting carbon dioxide into methane under the irradiation of sunlight, so that the fixed conversion of carbon dioxide and the conversion of solar energy into chemical energy at normal temperature are realized; and then, methane oxidizing bacteria are selected to specifically convert the obtained methane into ethanol, so that sustainable production of liquid fuel is realized.
Example 2
By H 2 /CO 2 As a substrate, hydrogen-producing methanogens are microbial catalysts for reducing carbon dioxide to methane at normal temperature under anaerobic conditions, or are capable of converting CO using acetogens (Moorella thermoacetica) 2 Conversion to acetic acid, etc.; and then, the Cu doped polymer carbon nitride material or the silicon oxide supported transition metal phosphide is used as a photocatalyst material, methane or acetic acid obtained by the microbial electrosynthesis is converted into liquid fuels such as ethanol, and the efficiency of the bioelectricity synthesis and the photocatalysis reaction in the embodiment is higher along with reasonable selection of the catalyst, so that the rapid conversion of carbon dioxide into the liquid fuels can be effectively realized.
In the embodiment of the invention, through the selection and reaction sequence adjustment of the photocatalyst and the biocatalyst, the parameter adjustment comprises the following steps: (1) intensity of sunlight: according to the tolerance of the photocatalyst to sunlight intensity, the range is from one sunlight to ten sunlight; (2) reactor temperature: the temperature of the reaction system is gradually increased under the influence of illumination factors, and the whole reaction system needs to be controlled within the range of highest activity of the biological enzyme/bionic enzyme catalyst (generally 30-37 ℃) through a cooling device; (3) poisoning of the intermediate product on the catalyst: the increase of the concentrations of the intermediate products and the final products can have a certain influence on the activity of the catalyst, and in order to ensure the continuous catalytic reaction, the final products of the liquid fuel need to be collected in real time through a receiving device.
The activity and the selectivity of the catalyst are high in the process of fixedly converting the carbon dioxide into the liquid fuel, the generation of byproducts can be effectively reduced, and the generated liquid fuel can also be directly utilized by a fuel cell, so that the rapid cyclic conversion from solar energy to chemical energy to electric energy is realized.
The above-described embodiments are merely preferred embodiments for fully explaining the present invention, and the scope of the present invention is not limited thereto. Equivalent substitutions and modifications will occur to those skilled in the art based on the present invention, and are intended to be within the scope of the present invention. The protection scope of the invention is subject to the claims.
Claims (3)
1. The synthesis method of the solar bionic catalytic liquid fuel is characterized by comprising the following steps of: CO synthesis by combination of photocatalytic reaction and microbial electrosynthesis 2 The method comprises the steps of fixing carbon dioxide into an intermediate product by using a photocatalyst I, and then selecting the biocatalyst I capable of using the intermediate product to convert the intermediate product into liquid fuel through microbial electrosynthesis;
or CO is synthesized by bioelectricity by using a biocatalyst II 2 Converting into an intermediate product, and further converting the intermediate product into liquid fuel by utilizing a photocatalyst II;
the intermediate product is CO, formaldehyde and CH 4 One or more of the following; the liquid fuel is methanol, ethanol or esters; the biocatalyst I is capable of converting CO, formaldehyde, CH 4 One or more of a microorganism, a biological enzyme or a biomimetic enzyme that converts to methanol or ethanol, the biocatalyst I comprising methane-oxidizing bacteria, methanol dehydrogenase, aldose reductase;
the biocatalyst II is capable of converting CO 2 Is converted into CO, formaldehyde and CH 4 One or more of a microorganism, a biological enzyme or a bionic enzyme, wherein the biological catalyst II comprises methanogen or acetic acid bacteria; the acetobacter is Mortierella acetobacter (Moorella thermoacetate), and the methanogen comprises Methanococcus equi (Methanonococcus), methanopyccus (Methanano-Sarcina) and Methanobacterium ruminant (Methanofacillus); the photocatalyst I can reduce carbon dioxide to generate CO, formaldehyde and CH 4 The catalytic material is a noble metal or non-noble metal modified vanadium compound, a Ti-based compound or graphite phase carbon nitride; the photocatalyst II can convert CO, formaldehyde and CH under the condition of room temperature 4 The catalytic material is a vanadium compound, a Ti-based compound or graphite phase carbon nitride modified by noble metal or non-noble metal.
2. The method for synthesizing the solar biomimetic catalysis liquid fuel according to claim 1, wherein the method comprises the following steps: the noble metal is one or more of Pt, ag, pd or Au; the non-noble metal is one or more of Cu, mg, co or Ni.
3. The method for synthesizing the solar biomimetic catalysis liquid fuel according to claim 1, wherein the method comprises the following steps: the photocatalyst I is prepared on BiVO by adopting a high-temperature method and a deposition method 4 Catalytic material doped with Cu, mg, co or Ni non-noble metal atoms on the surface of the substrate material; the photocatalyst II is a polymer carbon nitride material doped with Cu, pt and Pb or a silicon oxide loaded transition metal phosphide.
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