CN108118358A - Photosynthesis and (light) electro-catalysis combined system separate type hydrogen production by water decomposition method - Google Patents
Photosynthesis and (light) electro-catalysis combined system separate type hydrogen production by water decomposition method Download PDFInfo
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- CN108118358A CN108118358A CN201611070004.2A CN201611070004A CN108118358A CN 108118358 A CN108118358 A CN 108118358A CN 201611070004 A CN201611070004 A CN 201611070004A CN 108118358 A CN108118358 A CN 108118358A
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- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
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- C25B1/00—Electrolytic production of inorganic compounds or non-metals
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
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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
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Abstract
The present invention provides a kind of methods using separate type hydrogen production by water decomposition associated with natural biology source photosynthesis and artificial (light) electro-catalysis.This method releases oxygen with the Photosystem I I enzymes of microalgae using solar energy photosynthesis oxidation water, and additional chemical electron carrier is reduced, the electrolyte solution of the carrier of stored electrons and proton is stored and transports (light) electro-catalysis system for producing hydrogen.In (light) electrolytic cell, in anode oxidation reaction release electronics occurs for electron carrier, and cathode combination proton generates hydrogen, will be recycled after collecting hydrogen in electrolyte solution return photosynthesis system.The water oxidation reaction of the biology system into relatively independent with electrochemistry proton reduction reaction designing is spatially separated from production hydrogen and oxygen by this method, solves H2And O2Gas separation problem reaches the comprehensive utilization of solar energy and electric energy with reference to biological photosynthesis and artificial photoelectrochemical process.
Description
Technical field
The invention belongs to solar energy chemical conversion production sun fuel technology fields, and in particular to and a kind of photosynthesis-
The method of (light) electro-catalysis combined system separate type hydrogen production by water decomposition.
Background technology
Growing with human society, energy crisis and environmental problem are tight caused by traditional Fossil fuel consumption
The sustainable development of the mankind is threatened again, and it is extremely urgent to develop clean regenerative resource.Among many clean energy resource forms,
Solar energy has many advantages, such as that inexhaustible, cleaning is pollution-free, widely distributed, is translated into the clean fuel that can be stored and transport
It will be one of approach of Solar use.And Hydrogen Energy has heats of combustion value and zero-emission as another clean energy resource form
Advantage.Therefore, it is a kind of regenerative resource of most prospect to produce clean hydrogen fuel by photochemical catalyzing using solar energy
Technology.
And in nature, higher plant, algae and cyanobacteria carry out photosynthesis using solar energy, in mild condition
The lower oxidation for realizing water and carbon dioxide reduction, convert solar energy into chemical energy and are stored in biomass.At present, microalgae energy
Source and separated part photosynthetic enzyme hydridization device is extracted from plant there is potential application value.
Microalgae has photosynthetic efficiency high, and the features such as being easy to cultivate, being converted into solar energy in chemical-biological energy field is
One of hot spot of research.Part cyanobacteria and microalgae can realize decomposing water with solar energy hydrogen manufacturing, and it is photosynthetic which mainly puts oxygen
The electronics and proton that biological oxidation water generates generate hydrogen by hydrogenase or azotase, but the process is in middle biohydrogenation
Enzyme is easy to inactivate under oxygen atmosphere, this difficult point never solves well at present, becomes the bottleneck of microalgae photosynthetic hydrogen production
(Plant Biotechnol.J.,2016,14,1487-1499).However, by microalgae or separated photosynthetical system enzyme using too
Slave biological cell (enzyme) transfer for the method part that the reducing power (electronics and proton) that sun can decompose water generation passes through manual intervention
It is shifted out, is stored in manual energy's carrier, then reduced by the method for manual electrochemical or optical electro-chemistry and generate hydrogen, be structure
Build a desirable route of decomposing water with solar energy production hydrogen.
At present, microalgae or photosynthetical system II with photoelectrochemistrpool pool are coupled and realizes that decomposing water with solar energy is still seldom, Chen Jun
With the patent (patent No. of Li Can et al. application：201310322416.0), it was recently reported that a kind of Photosystem I I enzymes and semiconductor nano
The method of material hybridization system photocatalytic hydrogen production by water decomposition gas, hybrid systems are realized in aqueous solution using sunlight decomposes aquatic products
Raw hydrogen and oxygen.Kato et al. reports a kind of light anode, using the PSII enzymes of separation and Extraction in cyanobacteria as water oxidation material,
PSII is assembled in porous electro-conductive glass ITO and forms biological light anode, under additional certain bias, red light irradiation water oxygen
Galvanic current is 1.6 ± 0.3 μ A cm-2(J.Am.Chem.Soc.,2012,134,8332-8335).Chen Zhaoan et al. consolidates microalgae
On the perforated substrate of fixed tablet, biological light anode is made, electron mediator is directly added into electrochemical cell, and between the electrodes
Additional certain voltage realizes photo-biological oxidation water, and generates the hydrogen (patent No. in cathode：201110404949.4).
Alistair J.McCormick et al. report a kind of bio-light cell system, and biological anode is by cyanobacteria
Synechocystis sp.PCC 6803 and the potassium ferricyanide are formed, and under the voltage of additional 1V, the maximum hydrogen-producing speed of system is
0.68mmol H2[mol Chl-1]s-1(Energy Environ.Sci.,2013,6,2682-2690)。
But the structure of the photocatalytic system and photoelectrocatalytioxidation oxidation system in above-mentioned report is all based on separation Photosystem I I enzymes
It, can there are following problems with the hybrid material of inorganic material：
(1) separated Photosystem I I enzymes are incorporated in inorganic material and are easy to inactivate enzyme from plant.
(2) microalgae is fixed in electrode basement, and system is more complicated, cause the activity of microalgae compared to it is free under
Drop, reaction efficiency are relatively low.
(3) microalgae and Photosystem I I enzymes are directly combined with electro-chemical systems, the electronics and proton that photosynthetic water oxygenization generates, by
It in that cannot be enriched with, reacts at low concentrations, density of photocurrent is low, and energy consumption increases.
(4) photocatalytic system generate mixing hydrogen and oxygen, be not easy to separate, it is difficult to the high-purity oxygen of centralized collection and
Hydrogen.
Therefore, how the photosynthesis carried out using photosynthetic organism source system builds efficient decomposing water with solar energy system still
Many challenges are so faced, the present invention combines biological photosynthesis and artificial light (electricity) catalysis material from new angle and thinking
The advantage of system constructs a kind of method of separate type hydrogen production by water decomposition, and solving biology cannot be certainly during photosynthetic-hydrogen-production
The problems such as I replicates and growth, centralized collection solar energy fuel.This method is simple and efficient, hydrogen and oxygen separation, easily operated,
With industrial applications prospect.
The content of the invention
It is an object of the invention to provide a kind of photosynthesis-(light) electro-catalysis combined system separate type hydrogen production by water decomposition
Method
The present invention aoxidizes water using sunlight or artificial light source photosynthesis by microalgae and releases oxygen, by the electronics of generation
With proton storage in the electrolyte solution containing electron carrier, then collect and transport electrolyte solution to (light) electro-catalysis body
Hydrogen is produced in system, in anode oxidation reaction occurs for electron carrier, and cathode combination proton generates hydrogen, and oxygen hydrogen is in time and space
On be kept completely separate generation (see Fig. 1), basic process is：
(1) biological photosynthesis：
2H2O→O2+4H++4e-
Mp++ne-→Mq+(p ＞ q)
(2) the chemical hydrogen manufacturing of light (electricity)：
Mq++2H+→Mp++H2(q ＞ p)
Separate type hydrogen production by water decomposition associated with natural biology source provided by the invention photosynthesis and artificial (light) electro-catalysis
Method, the photosynthesis water oxidation material be microalgae, water plant and its Photosystem I I enzymes.
The side of separate type hydrogen production by water decomposition associated with biological source photosynthesis provided by the invention and artificial (light) electro-catalysis
Method, the microalgae is chrysophyceae, micro- plan ball algae, spirulina, one or more of chlorella and cyanobacteria, algae density for 3,000 ten thousand-
200000000 cells/mls.The Photosystem I I is from higher plant, microalgae and water plant etc..
Separate type hydrogen production by water decomposition associated with natural biology source provided by the invention photosynthesis and artificial (light) electro-catalysis
Method, the photosynthesis oxidation water reaction generate electronics and proton storage in the electrolyte solution containing electron carrier
In.
The side of separate type hydrogen production by water decomposition associated with biological source photosynthesis provided by the invention and artificial (light) electro-catalysis
Method, the electron carrier in the electrolyte solution is the potassium ferricyanide (0-100mM), quinones molecular compound (0-50mM), first
One or more of base amethyst (0-50mM), cobalt-based molecular complex (0-100mM).
Separate type hydrogen production by water decomposition associated with natural biology source provided by the invention photosynthesis and artificial (light) electro-catalysis
Method, in described (light) the electro-catalysis system, anode material is platinum electrode, the carbon paper of modification, fluorine (indium) mix tin oxide
In anode oxidation reaction occurs for one kind in the silicon (Si) that (FTO, ITO) glass, surface are modified, electron carrier.
Separate type hydrogen production by water decomposition associated with natural biology source provided by the invention photosynthesis and artificial (light) electro-catalysis
Method, in described (light) the electro-catalysis system, cathode material is platinum electrode, one kind in the carbon paper electrode of modification, and cathode is also
Protoplasm generates hydrogen.
The side of separate type hydrogen production by water decomposition associated with biological source photosynthesis provided by the invention and artificial (light) electro-catalysis
Method, light source is nature sunlight described in the culture of microalgae, the photosynthetic response of microalgae and electron carrier and optical electro-chemistry reaction
Or indoors and in special circumstances in light that xenon lamp, halogen lamp, LED etc., daily fluorescent lamp and solar simulator are sent
Any one is combined.
The side of separate type hydrogen production by water decomposition associated with biological source photosynthesis provided by the invention and artificial (light) electro-catalysis
Method, in (light) electro-catalysis system, anode material is platinum electrode, the carbon paper of modification, fluorine (indium) mix tin oxide (FTO, ITO)
In anode oxidation reaction occurs for one kind in the silicon (Si) that glass, surface are modified, electron carrier.Cathode material is platinum electrode, changes
Property carbon paper electrode, cathodic reduction proton generate hydrogen.Pass through proton exchange membrane, anion exchange between anode slot and cathode can
Film, ceramic membrane, dialysis membrane etc. are selectively separated through membrane material.
The side of separate type hydrogen production by water decomposition associated with biological source photosynthesis provided by the invention and artificial (light) electro-catalysis
Method, the electrolyte solution be containing phosphate (10-100mM), nitrate (10-100mM), sodium chloride (10-500mM),
The seawater or tap water of one or more of iron, cobalt, nickel, molybdenum, magnesium, manganese, copper, zinc, calcium metal salt (0.01-10mM), according to
Different systems, pH can be in 2-12 scopes.The applied voltage of optical electro-chemistry system is the DC voltage of 0-1.23V.
This method exists the water oxidation reaction of the biology system into relatively independent with electrochemistry proton reduction reaction designing
Production hydrogen and oxygen are spatially separated, solves H2And O2Gas separation problem, with reference to biological photosynthesis and manually it is photoelectrochemical
Process reaches the comprehensive utilization of solar energy and electric energy.It is single by reaction of 100L seawater algae solution by the hydrogen production process of the present invention
Member, 1 year (300 days) about generate 3000 kilograms of hydrogen/hectares, and hydrogen output is the 2 of the microalgae production hydrogen technology reported in the world at present
Times or more.The present invention has catalyst material at low cost, without hydrogen and oxygen separation, sustainable production high purity oxygen gas and hydrogen
The features such as, provide a new way for solar energy fuel production.
Description of the drawings
Fig. 1 is separate type hydrogen production by water decomposition method associated with biological source photosynthesis of the present invention and artificial light (electricity) catalysis
Process flow chart；
Fig. 2 technical solution schematic diagrames
Fig. 3 aoxidizes water for chrysophyceae photosynthesis and reduces potassium ferricyanide activity time graph；
Fig. 4 is photo-reduction potassium ferricyanide activity time graph under the different light intensity of chrysophyceae；
Fig. 5 is photo-reduction potassium ferricyanide activity time graph under chrysophyceae difference cell density；
Fig. 6 aoxidizes water for flat algae photosynthesis and reduces potassium ferricyanide activity time graph；
Fig. 7 is the voltage-time curve figure of carbon electrode and platinum electrode electrochemical oxidation potassium ferrocyanide；
Fig. 8 is that the potassium ferrocyanide of various concentration schemes the activity of electro-catalysis hydrogen manufacturing；
Fig. 9 is the current-time curvel figure figure of silicon substrate light anode photoelectrocatalysioxidization oxidization potassium ferrocyanide hydrogen manufacturing；
Figure 10 is the activity time graph of silicon substrate light anode photoelectrocatalysioxidization oxidization potassium ferrocyanide hydrogen manufacturing
Figure 11 is that the reduction potassium ferricyanide of chrysophyceae recycles time plot；
Figure 12 is that chrysophyceae schemes the activity of the reduction potassium ferricyanide in Various Seasonal and weather.
Specific embodiment
The following examples will be further described the present invention, but not thereby limiting the invention.
Embodiment 1
The activity of the present embodiment evaluation lsochrysis zhanjiangensis photosynthesis oxidation water reduction potassium ferricyanide.
The whips gold baths such as Zhanjiang that 20 milliliters of bath density are 5,000 ten thousand cells/mls is taken to be stirred in reactor, adding in concentration is
The potassium ferricyanide sea water solution of 5mM, at room temperature, with light intensity in 300E/m2s-1Fluorescent lamp shines for light source light, photosynthesis reduction
The potassium ferricyanide generates potassium ferrocyanide, and the illumination electric content to concentration after a certain period of time is analyzed by ultraviolet-visible absorption spectroscopy,
Its reaction result such as Fig. 3.
Embodiment 2
The present embodiment evaluates light intensity of incident light to lsochrysis zhanjiangensis photosynthesis oxidation water reduction potassium ferricyanide activity
It influences.
The whips gold baths such as Zhanjiang that 20 milliliters of bath density are 5,000 ten thousand cells/mls is taken to be stirred in reactor, adding in concentration is
The potassium ferricyanide sea water solution of 5mM at room temperature, controls fluorescent light with different luminous intensity illumination to reaction system, photosynthetic
The effect reduction potassium ferricyanide generates potassium ferrocyanide, and it is electric to concentration after a certain period of time to analyze illumination by ultraviolet-visible absorption spectroscopy
Content, reaction result such as Fig. 4.
Embodiment 3
The present embodiment evaluates influence of the algae density to lsochrysis zhanjiangensis photosynthesis oxidation water reduction potassium ferricyanide activity.
The whips gold bath such as Zhanjiang is cultivated under the same conditions in other conditions to certain algae density, takes 20 milliliters in reactor
Middle stirring adds in the potassium ferricyanide sea water solution that concentration is 5mM, at room temperature, with light intensity in 300 μ E/m2s-1Fluorescent lamp is light
To reaction system, the photosynthesis reduction potassium ferricyanide generates potassium ferrocyanide, is analyzed by ultraviolet-visible absorption spectroscopy for source illumination
Illumination after a certain period of time electricity to the content of concentration, reaction result such as Fig. 5.
Embodiment 4
The activity of the present embodiment evaluation flat algae photosynthesis oxidation water reduction potassium ferricyanide.
The flat algae that 20 milliliters of bath density is taken to be 5,000 ten thousand cells/mls stirs in reactor, adds in the iron that concentration is 5mM
Potassium cyanide sea water solution, at room temperature, with light intensity in 300 μ E/m2s-1Fluorescent lamp shines for light source light, photosynthesis reduced iron cyaniding
Potassium generates potassium ferrocyanide, and analyzing illumination by ultraviolet-visible absorption spectroscopy, electricity to the content of concentration, reacts after a certain period of time
As a result such as Fig. 6.
Embodiment 5
The present embodiment, which evaluates carbon electrode and platinum electrode electrocatalytic oxidation potassium ferrocyanide hydrogen manufacturing, influences operating voltage.
In two electrode electrolytic pools of 14mL, using carbon electrode or platinum electrode as working electrode, another platinum electrode is to electricity
Pole, centre are separated with proton exchange membrane, in the phosphate buffer solution of 0.1M (pH, 7.0), add in the ferrocyanide of 10mM
Potassium investigates decomposition voltage with the variation of electrolytic process.As a result such as Fig. 7.
Embodiment 6
The present embodiment evaluation ferrocyanide potassium concn changes the influence to electro-catalysis hydrogen production activity.
In two electrode electrolytic pools of 14mL, using carbon electrode as working electrode, platinum electrode is to electrode, and centre is handed over proton
It changes film to separate, in the phosphate buffer solution of 0.1M (pH, 7.0), adds in the potassium ferrocyanide of various concentration, investigate electrolytic cell
The activity of electro-catalysis hydrogen manufacturing.As a result such as Fig. 8.
Embodiment 7
The photoelectrocatalysis reaction tank ferrous oxide potassium cyanide that the present embodiment evaluation silicon substrate light anode is formed is to electrode hydrogen manufacturing
Activity.
In two electrode electrolytic pools of 50mL, the n-type silicon of tin oxide and titanium dioxide surface modification is mixed as light sun using indium
Pole, platinum electrode are to electrode, and centre is separated with proton exchange membrane, and in the potassium chloride electrolyte of 0.5M, addition concentration is 200mM
Potassium ferrocyanide, using 300W xenon lamps as light source, investigate the operating current of photoelectrolytic cell and the activity of hydrogen manufacturing and efficiency.As a result such as
Fig. 9 and Figure 10.
Embodiment 8
The activity that the present embodiment evaluation seaweed reduction potassium ferricyanide recycles.
The iron cyaniding that concentration is about 5mM is added in every time in the chrysophyceae algae solution (50,000,000/milliliter of algae cell density) of 50mL
Potassium solution, the frustule reduction potassium ferricyanide generate potassium ferrocyanide, react the also commercial weight ultravioletvisible absorption light of ferric ferricyanide
Spectrum quantify, cycles 3 this reaction result such as Figure 12 for using.
Embodiment 9
The present embodiment evaluation seaweed outdoors under full-scale condition Various Seasonal and weather to reducing the activity of the potassium ferricyanide.
It is molten that the potassium ferricyanide that concentration is 10mM is added in the chrysophyceae algae solution (50,000,000/milliliter of algae cell density) of 500mL
Liquid, solar irradiation, the frustule reduction potassium ferricyanide generate potassium ferrocyanide, and the ferric ferrocyanide for reacting generation is inhaled with UV, visible light
Receive quantitative spectrometric, reaction result such as Figure 12.
Claims (10)
1. photosynthesis and (light) electro-catalysis combined system separate type hydrogen production by water decomposition method, utilize natural biology source photosynthesis
With artificial photoelectrocatalysis or electro-catalysis associated with separate type hydrogen production by water decomposition, it is characterised in that：Utilize the Photosystem I I of organism
It aoxidizes water function water oxygenization under sunlight and/or artificial light source effect and releases oxygen, while the electronics of generation and proton are stored up
In the presence of in the electrolyte solution containing electron carrier, then collecting and transport electrolyte solution to photoelectrocatalysis or electro-catalysis system
In anode oxidation reaction occurs for middle production hydrogen, electron carrier, and cathode combination proton generates hydrogen, and oxygen Hydrogen Separation generates.
2. according to the method for claim 1, it is characterised in that：Natural biology source photosynthesis water oxidation material be from
Microalgae and/or the Photosystem I I of water plant.
3. according to the method described in claim 1 or 2, it is characterised in that：The microalgae is chrysophyceae, micro- plan ball algae, spirulina,
One or more of chlorella and cyanobacteria, algae density are 0.1 thousand ten thousand -2 hundred million cells/mls；The Photosystem I I is derived from
One or two or more kinds in higher plant spinach, microalgae and water plant etc..
4. according to the method for claim 1, it is characterised in that：The electronics and proton storage that photosynthesis oxidation water generates exist
In electrolyte solution containing electron carrier；The electron carrier in electrolyte solution is added as the potassium ferricyanide (1-100mM), quinone
Quasi-molecule compound (1-50mM), methyl amethyst (1-50mM), one kind in cobalt-based molecular complex (1-100mM) or two kinds with
On, the total mol concentration of all electron carriers is (1-500mM).
5. according to the method for claim 1, it is characterised in that：The photosynthetic response of the culture of microalgae, microalgae and electron carrier
And light source described in optical electro-chemistry reaction for nature sunlight or indoors and in special circumstances xenon lamp, halogen lamp, LED etc.,
Any one in the light that daily fluorescent lamp and solar simulator are sent or two kinds of combination of the above.
6. according to the method for claim 1, it is characterised in that：In photoelectrocatalysis or electro-catalysis system, anode material is
Platinum electrode, the carbon paper of modification, fluorine and/or indium doping tin oxide (FTO and/or ITO) glass in one kind, electron carrier is in sun
Oxidation reaction occurs for pole；
In photoelectrocatalysis or electro-catalysis system, cathode material is the silicon that platinum electrode, the carbon paper electrode of modification and surface are modified
(Si) one kind in, cathodic reduction proton generate hydrogen；
It is handed between the cathode can where the anode slot and cathode where photoelectrocatalysis or electro-catalysis system Anodic by proton
Film, anion-exchange membrane, ceramic membrane, dialysis membrane etc. is changed selectively to separate through one kind in membrane material.
7. according to the method described in claim 1 or 4, it is characterised in that：The culture medium composition of the microalgae is to contain phosphoric acid
Salt (10-100mM), nitrate (10-100mM), sodium chloride (10-500mM), iron, cobalt, nickel, molybdenum, magnesium, manganese, copper, zinc, calcium metal
One or two or more kinds of seawater and/or water in salt (0.01-10mM), according to different systems, pH can be in 2-12 scopes.
8. according to the method described in claim 1 or 6, it is characterised in that：Electrically or optically the applied voltage of electrochemical system is 0-
1.23V DC voltage.
9. according to the method for claim 1, it is characterised in that：
It is the electrolysis containing electron carrier using the solution in the Photosystem I I and photoelectrocatalysis of organism or electro-catalysis system
Matter solution.
10. according to the method described in claim 1 or 9, it is characterised in that：
Electrolyte solution containing electron carrier is by water pump in the Photosystem I I using organism and photoelectrocatalysis or electro-catalysis
It is circulated between system.
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| CN112046800A (en) * | 2020-08-14 | 2020-12-08 | 中国科学院空间应用工程与技术中心 | Use multiply wood artificial photosynthesis device under microgravity environment |
| CN113952908A (en) * | 2021-10-08 | 2022-01-21 | 浙江高晟光热发电技术研究院有限公司 | Photocatalytic hydrogen production device and hydrogen production system |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN112046800A (en) * | 2020-08-14 | 2020-12-08 | 中国科学院空间应用工程与技术中心 | Use multiply wood artificial photosynthesis device under microgravity environment |
| CN112046800B (en) * | 2020-08-14 | 2022-02-01 | 中国科学院空间应用工程与技术中心 | Use multiply wood artificial photosynthesis device under microgravity environment |
| CN113952908A (en) * | 2021-10-08 | 2022-01-21 | 浙江高晟光热发电技术研究院有限公司 | Photocatalytic hydrogen production device and hydrogen production system |
| CN113952908B (en) * | 2021-10-08 | 2023-12-05 | 浙江高晟光热发电技术研究院有限公司 | Photocatalysis hydrogen production device and hydrogen production system |
| CN114534666A (en) * | 2022-02-23 | 2022-05-27 | 中国能源建设集团广东省电力设计研究院有限公司 | Continuous photocatalytic hydrogen production reaction device and hydrogen production method thereof |
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