CN102400169A - Method for producing hydrogen by alkalescent microbe electrolysis - Google Patents
Method for producing hydrogen by alkalescent microbe electrolysis Download PDFInfo
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- CN102400169A CN102400169A CN2011103399221A CN201110339922A CN102400169A CN 102400169 A CN102400169 A CN 102400169A CN 2011103399221 A CN2011103399221 A CN 2011103399221A CN 201110339922 A CN201110339922 A CN 201110339922A CN 102400169 A CN102400169 A CN 102400169A
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Abstract
The invention belongs to the technical field of microbe electrochemistry and aims to provide a method for producing hydrogen by alkalescent microbe electrolysis. The method comprises steps of: (1) starting an electrolytic bath under a microbiological fuel cell mode: accessing a resistor in a closed-loop of a system and replacing a solution in the electrolytic bath when a voltage is low; continuing to replace until voltages at two ends of the resistor are higher than 500mV to finish anode starting; (2) producing hydrogen under a microbe electrolytic bath mode: replacing a cathode in the started electrolytic bath with stainless steel net or foamed nickel, keeping solution in the whole electrolytic bath in a anaerobic state and applying 0.4-0.8 V voltage at two ends of the cathode and the anode by using direct-current power supply and realizing hydrogen production of the electrolytic bath at 20-35 DEG C. The invention can effectively inhibit generation of methane, realize long time continuous operation or multiple batch operation and generate gas with low methane content; the method has a low cost and can obtain high hydrogen generation rate; utilization rate of organic matter under an alkalescent environment is increased, and hydrogen generation stability of the system is increased.
Description
Technical field
The invention belongs to the microorganism electrochemical technical field, what be specifically related to is a kind of alkaline mikrobe electrolytic hydrogen production method.
Background technology
Hydrogen Energy is a kind of clean energy.The development of Hydrogen Energy has very important meaning to future source of energy and environment.The production of hydrogen at present is mainly derived from non-renewable material such as oil, Sweet natural gas etc., prepares hydrogen through chemical means such as catalytic pyrolysis, gasifications.Yet following hydrogen must obtain from reproducible resource.Water electrolysis hydrogen production, solar photolysis water hydrogen and fermentative hydrogen production are continuable hydrogen manufacturing approach.Consume energy big cost of water electrolysis method is high.There is the low and stability problem of efficient in sun power photodissociation water law.Biological fermentation process have cleaning, energy consumption low, can administer advantage such as pollution simultaneously, be considered to following important hydrogen production process and approach, but also there is the low problem of biomass material utilization ratio in this method.Utilize the production by biological electrical characteristic; Gone out the microorganism electrolysis cell hydrogen generating system in conjunction with the brine electrolysis technological development, reached any biodegradable material capable of using and produced hydrogen, energy efficiency is high; And organic waste water capable of using is realized environment and energy doulbe-sides' victory effect that recovered energy is purified waste water again simultaneously.
The microorganism electrolysis cell hydrogen generating system is to utilize mikrobe to produce electronics and proton at the anodic oxidation organism, and electronics and proton combine to produce hydrogen at negative electrode by means of small impressed voltage.It can be designed to two chambers and single chamber.The double-chamber microbiological electrolyzer adopts ion-exchange membrane that battery is divided into cathode compartment and anolyte compartment, " is used to produce the bio-electrochemical process " (publication number CN1856706A) of hydrogen like Chinese patent.Twin cell complex structure, manufacturing and running cost are high, and hydrogen-producing speed is low, and there is the problem that anode pH value reduces and negative electrode pH value increases in long-time running.In contrast, the single-chamber microbial electrolyzer removes ion-exchange membrane, makes battery structure compact simple, and manufacturing cost reduces, and internal resistance of cell reduction, and hydrogen-producing speed is multiplied, and is the optimum structure of practical application.But the single-chamber microbial electrolyzer has only obtained high hydrogen-producing speed in short-term operation at present; And the long-time running hydrogen-producing speed reduces gradually; Its reason is methanogen growth fast in neutral reaction solution; Utilize hydrogen to become methane to make hydrogen yield reduce [Rader, G.K.and B.E.Logan..Int.J.Hydrogen Energy.2010 carbon dioxide reduction; 35 (17): 8848-8854).Methanogen also can directly receive electronics from negative electrode carbon dioxide reduction is become methane, thereby the electrical efficiency that makes system produce hydrogen reduces [Cheng, S., et al., Environ.Sci.Technol.2009; 43 (10): 3953-3958].The growth that suppresses methanogen is the essential key issue that solves of single-chamber microbial electrolytic hydrogen production technology.
Summary of the invention
The technical problem that the present invention will solve is, overcomes that the single-chamber microbial electrolytic hydrogen production produces methane and the problem that causes hydrogen generation efficiency to reduce, a kind of effective inhibition methanogen growth is provided and does not influence the alkaline mikrobe electrolytic hydrogen production method of hydrogen generation efficiency.What be applied in this method is microbe-derived in city domestic sewage, anaerobic activated sludge, beer waste water etc., through alkaline medium and organic substrate acclimation shaking culture, and directly domestication on anode, growth film forming under the closed circuit condition of battery.
Be the technical solution problem, alkaline microorganism electrolysis cell provided by the invention produces hydrogen methods, comprises step:
(1) under the microbiological fuel cell pattern, start electrolyzer:
The volume ratio of pressing 1: 1 earlier is with organic waste water and nutritive medium A uniform mixing, and using basic soln adjustment pH of mixed value then is 9～12, and adds organism matrix in the ratio of 1 grams per liter, obtains mixed liquid B; Mixed liquid B is added in the electrolyzer, in the loop line of system, insert 1000 ohmic resistances, when the resistance voltage is lower than 20mV, change the solution in the electrolyzer with new mixed liquid B; Greater than 500mV, anode starts and finishes lasting replacing reactor solution up to the resistance voltage;
(2) hydrogen manufacturing under the microorganism electrolysis cell pattern:
Started the negative electrode in the electrolyzer with stainless (steel) wire or nickel foam replacing, with electrolyzer and air insulated, made whole electrolytic solution cell be in anaerobic state with cover plate; Using the pH value of basic soln adjustment nutritive medium A is 9～12, and adds organism matrix in the ratio of 0.5～8 grams per liter, then mixing solutions is joined in the electrolyzer as electrolytic solution; Utilize direct supply to add 0.4～0.8V voltage, make electrolyzer 20～35 ℃ of operation realization hydrogen manufacturing down at electrolyzer anode and cathode two ends;
Said nutritive medium A consists of: comprise 8.4g NaHCO in every liter of nutritive medium
3, 0.31g NH
4Cl, 0.13gKCl, 2ml trace element solution, surplus are zero(ppm) water;
Said trace element solution is solvent with water, comprises following solute in every liter of solution: 2mg vitamin H, 2mg vitamins B, 10mg Y factor, 5mg vitamin G, 5mg thiamines, 5mg nicotinic acid, 5mg vitamin B3,0.1mg B-12,5mg para-amino benzoic acid, 5mg Thioctic Acid, 1.5g NTA, 3.0g MgSO
4, 0.5g MnSO
4H
2O, 1.0g NaCl, 0.1g FeSO
47H
2O, 0.1g CaCl
22H
2O, 0.1g CoCl
26H
2O, 0.13g ZnCl
2, 0.01g CuSO
45H
2O, 0.01g AlK (SO
4)
212H
2O, 0.01g H
3BO
3, 0.025g Na
2MoO
4, 0.024g NiCl
26H
2O, 0.025gNa
2WO
42H
2O;
Employed electrolyzer is the single compartment electrolytic cell that is made up of battery container, anode and air cathode; Its anode is the active carbon brush of being processed by titanium silk and NACF; Air cathode is the carbon cloth that the two sides applies diffusion layer and granulated active carbon Catalytic Layer respectively, and with diffusion layer towards air, activated carbon catalysis layer towards electrolytic solution.
Among the present invention, described organism matrix is any one in sodium acetate, acetate, glucose, ethanol or the formic acid.
Among the present invention, said organic waste water is any one in city domestic sewage, beer waste water, food processing wastewater or the livestock industry waste water.
Among the present invention, said basic soln is NaOH or KOH solution, and its concentration is 1M.
Compared with prior art, beneficial effect of the present invention is:
(1) can effectively suppress methane and produce, long-time continuous operation or multiple batches of operation, the methane content of output gas is less than 1%, and hydrogen-producing speed is 0.1～2.5m
3H
2/ m
3My god.
(2) adopt nickel foam, stainless (steel) wire to make cathod catalyst and substitute precious metals pt, though reduce cost, but still can obtain higher hydrogen-producing speed.
(3) under alkaline environment, organic utilization ratio improves, and the stability that system produces hydrogen improves.
Description of drawings
Fig. 1 is the structural representation (electrolyzer startup) of the embodiment of the invention 1 said microbiological fuel cell.
Fig. 2 is the structural representation (electrolyzer hydrogen manufacturing) of the embodiment of the invention 1 said microbiological fuel cell.
Label among the figure, 2: 1 battery container, 2 thomels brush anode, 3 air cathodes, 4 collection and confinement of gases pipes, 5 resistance, 6 direct supplys, 7 cathode of electrolytic tank.
6 batches hydrogen output and electric current were over time when Fig. 3 was 0.6V for embodiment 1 impressed voltage.
Fig. 4 for embodiment 6 impressed voltages be 0.6V, the hydrogen output when substrate concn is 4 grams per liters and electric current over time.
Embodiment
Through specific embodiment, implementation of the present invention is described in detail below.
Alkaline microorganism electrolysis cell among the present invention produces hydrogen methods, comprises step:
(1) under the microbiological fuel cell pattern, start electrolyzer:
The volume ratio of pressing 1: 1 earlier is with organic waste water and nutritive medium A uniform mixing, and using basic soln adjustment pH of mixed value then is 9～12, and adds organism matrix in the ratio of 1 grams per liter, obtains mixed liquid B; Mixed liquid B is added in the electrolyzer, in the loop line of system, insert 1000 ohmic resistances, when the resistance voltage is lower than 20mV, change the solution in the electrolyzer with new mixed liquid B; Greater than 500mV, anode starts and finishes lasting replacing reactor solution up to the resistance voltage;
(2) hydrogen manufacturing under the microorganism electrolysis cell pattern:
Started the negative electrode in the electrolyzer with stainless (steel) wire or nickel foam replacing, with electrolyzer and air insulated, made whole electrolytic solution cell be in anaerobic state with cover plate; Using the pH value of basic soln adjustment nutritive medium A is 9～12, and adds organism matrix in the ratio of 0.5～8 grams per liter, then mixing solutions is joined in the electrolyzer as electrolytic solution; Utilize direct supply to add 0.4～0.8V voltage, make electrolyzer 20～35 ℃ of operation realization hydrogen manufacturing down at electrolyzer anode and cathode two ends.
Said nutritive medium A consists of: comprise 8.4g NaHCO in every liter of nutritive medium
3, 0.31g NH
4Cl, 0.13gKCl, 2ml trace element solution, surplus are zero(ppm) water; Said trace element solution is solvent with water, comprises following solute in every liter of solution: 2mg vitamin H, 2mg vitamins B, 10mg Y factor, 5mg vitamin G, 5mg thiamines, 5mg nicotinic acid, 5mg vitamin B3,0.1mg B-12,5mg para-amino benzoic acid, 5mg Thioctic Acid, 1.5g NTA, 3.0g MgSO
4, 0.5g MnSO
4H
2O, 1.0g NaCl, 0.1g FeSO
47H
2O, 0.1g CaCl
22H
2O, 0.1g CoCl
26H
2O, 0.13g ZnCl
2, 0.01g CuSO
45H
2O, 0.01g AlK (SO
4)
212H
2O, 0.01g H
3BO
3, 0.025g Na
2MoO
4, 0.024g NiCl
26H
2O, 0.025g Na
2WO
42H
2O;
Employed electrolyzer is the single compartment electrolytic cell that is made up of battery container, anode and air cathode; Its anode is the active carbon brush of being processed by titanium silk and NACF; Air cathode is the carbon cloth that the two sides applies diffusion layer and granulated active carbon Catalytic Layer respectively, and with diffusion layer towards air, activated carbon catalysis layer towards electrolytic solution.
Each embodiment data during hydrogen manufacturing under the microorganism electrolysis cell pattern see the following form.
| The specific |
1 | 2 | 3 | 4 | 5 | 6 |
| 1M sodium hydroxide | √ | √ | √ | √ | √ | |
| 1M Pottasium Hydroxide | √ | |||||
| |
10 | 10 | 9 | 12 | 10 | 10 |
| Sewage | √ | √ | ||||
| Beer waste water | √ | √ | ||||
| Food processing wastewater | √ | |||||
| Livestock industry waste water | √ | |||||
| |
2 grams per |
8 grams per |
4 grams per liters | |||
| Acetate | 0.5 grams per | |||||
| Glucose | ||||||
| 1 grams per | ||||||
| Ethanol | ||||||
| 1 grams per liter | ||||||
| |
4 grams per liters | |||||
| The 2mL trace element solution | √ | √ | √ | √ | √ | √ |
| Hydrogen manufacturing cathode of electrolytic tank material | Stainless (steel) wire | Stainless (steel) wire | Stainless (steel) wire | Stainless (steel) wire | Stainless (steel) wire | Nickel foam |
| Impressed voltage (volt) | 0.6 | 0.6 | 0.8 | 0.4 | 0.7 | 0.6 |
| Test temperature (℃) | 30 | 30 | 20 | 35 | 30 | 30 |
Claims (4)
1. an alkaline mikrobe electrolytic hydrogen production method is characterized in that, may further comprise the steps:
(1) under the microbiological fuel cell pattern, start electrolyzer:
The volume ratio of pressing 1: 1 earlier is with organic waste water and nutritive medium A uniform mixing, and using basic soln adjustment pH of mixed value then is 9～12, and adds organism matrix in the ratio of 1 grams per liter, obtains mixed liquid B; Mixed liquid B is added in the electrolyzer, in the loop line of system, insert 1000 ohmic resistances, when the resistance voltage is lower than 20mV, change the solution in the electrolyzer with new mixed liquid B; Greater than 500mV, anode starts and finishes lasting replacing reactor solution up to the resistance voltage;
(2) hydrogen manufacturing under the microorganism electrolysis cell pattern:
Started the negative electrode in the electrolyzer with stainless (steel) wire or nickel foam replacing, with electrolyzer and air insulated, made whole electrolytic solution cell be in anaerobic state with cover plate; Using the pH value of basic soln adjustment nutritive medium A is 9～12, and adds organism matrix in the ratio of 0.5～8 grams per liter, then mixing solutions is joined in the electrolyzer as electrolytic solution; Utilize direct supply to add 0.4～0.8V voltage, make electrolyzer 20～35 ℃ of operation realization hydrogen manufacturing down at electrolyzer anode and cathode two ends;
Said nutritive medium A consists of: comprise 8.4g NaHCO in every liter of nutritive medium
3, 0.31g NH
4Cl, 0.13gKCl, 2ml trace element solution, surplus are zero(ppm) water;
Said trace element solution is solvent with water, comprises following solute in every liter of solution: 2mg vitamin H, 2mg vitamins B, 10mg Y factor, 5mg vitamin G, 5mg thiamines, 5mg nicotinic acid, 5mg vitamin B3,0.1mg B-12,5mg para-amino benzoic acid, 5mg Thioctic Acid, 1.5g NTA, 3.0g MgSO
4, 0.5g MnSO
4H
2O, 1.0g NaCl, 0.1g FeSO
47H
2O, 0.1g CaCl
22H
2O, 0.1g CoCl
26H
2O, 0.13g ZnCl
2, 0.01g CuSO
45H
2O, 0.01g AlK (SO
4)
212H
2O, 0.01g H
3BO
3, 0.025g Na
2MoO
4, 0.024g NiCl
26H
2O, 0.025gNa
2WO
42H
2O;
Employed electrolyzer is the single compartment electrolytic cell that is made up of battery container, anode and air cathode; Its anode is the active carbon brush of being processed by titanium silk and NACF; Air cathode is the carbon cloth that the two sides applies diffusion layer and granulated active carbon Catalytic Layer respectively, and with diffusion layer towards air, activated carbon catalysis layer towards electrolytic solution.
2. alkaline mikrobe electrolytic hydrogen production method according to claim 1 is characterized in that described organism matrix is any one in sodium acetate, acetate, glucose, ethanol or the formic acid.
3. alkaline mikrobe electrolytic hydrogen production method according to claim 1 is characterized in that said organic waste water is any one in city domestic sewage, beer waste water, food processing wastewater or the livestock industry waste water.
4. alkaline mikrobe electrolytic hydrogen production method according to claim 1 is characterized in that said basic soln is NaOH or KOH solution, and its concentration is 1M.
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| CN102400169B CN102400169B (en) | 2014-01-22 |
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Cited By (22)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102650063A (en) * | 2012-05-17 | 2012-08-29 | 大连理工大学 | Method for recovering elementary-substance cobalt from lithium cobaltate in one step by utilizing microbial electrolysis cell |
| CN102864463A (en) * | 2012-08-29 | 2013-01-09 | 杭州净洋环保科技有限公司 | H2 collection system for kitchen wastes |
| CN103865957A (en) * | 2012-12-13 | 2014-06-18 | 中国科学院城市环境研究所 | Method utilizing hydrogen-producing acetogens and electricigens to enhance biological hydrogen production efficiency |
| CN104451760A (en) * | 2014-11-27 | 2015-03-25 | 苏州嘉禧萝生物科技有限公司 | Method for MEC (microbial electrolysis cell) hydrogen production liquid |
| CN105463029A (en) * | 2015-12-30 | 2016-04-06 | 中山大学 | Method for enhancing hydrogen production of single-chamber microbial electrolysis cell |
| CN105803001A (en) * | 2016-05-06 | 2016-07-27 | 河海大学 | Method for achieving hydrogen generation from excess sludge by microbial electrolysis cell |
| CN104480493B (en) * | 2014-11-21 | 2017-01-18 | 大连理工大学 | Method for recycling copper and cadmium and preparing cadmium bronze precursor employing compact biological electrochemical reactor |
| CN107245580A (en) * | 2017-05-08 | 2017-10-13 | 大连理工大学 | It is a kind of to clean the effective method that copper, tin and iron are separated and recovered from from spent acidic etching solution |
| CN108390085A (en) * | 2018-04-10 | 2018-08-10 | 中国华能集团清洁能源技术研究院有限公司 | A kind of electrolysis urea hydrogen manufacturing is used for the system and method for fuel cell car |
| CN108569757A (en) * | 2018-05-09 | 2018-09-25 | 南开大学 | A method of handling sulfamido waste water and synchronous hydrogen manufacturing using electrochemical appliance |
| CN109554720A (en) * | 2019-01-03 | 2019-04-02 | 江南大学 | A method of improving microorganism electrolysis cell methane production and purity |
| CN109680290A (en) * | 2018-12-28 | 2019-04-26 | 同济大学 | Manifold type bioelectrochemistry produces hydrogen and collection device, system and produces hydrogen methods |
| CN109680289A (en) * | 2018-12-28 | 2019-04-26 | 同济大学 | Manifold type bioelectrochemistry produces hydrogen and purifying plant, system and produces hydrogen methods |
| CN109680291A (en) * | 2018-12-28 | 2019-04-26 | 同济大学 | Enhance the production hydrogen methods and bioelectrochemistry system for producing hydrogen of bioelectrochemistry |
| CN109680288A (en) * | 2018-12-28 | 2019-04-26 | 同济大学 | Bioelectrochemistry produces hydrogen and collection device and system |
| CN109680292A (en) * | 2018-12-28 | 2019-04-26 | 同济大学 | Bioelectrochemistry produces hydrogen and purifying plant and system |
| CN109761340A (en) * | 2019-03-26 | 2019-05-17 | 长春工程学院 | Tiny ecosystem period suitching type microorganism electrolysis cell and its operation method |
| CN110204033A (en) * | 2019-05-08 | 2019-09-06 | 南开大学 | A kind of method that microorganism electrochemical ammoniumization recycles nitrate nitrogen in waste water |
| CN112458487A (en) * | 2020-09-03 | 2021-03-09 | 南昌航空大学 | Medium-alkali asymmetric microbial electrolytic cell and application thereof in hydrogen production |
| EP4001461A3 (en) * | 2020-11-24 | 2022-06-01 | Yong Won Jeon | Method of producing hydrogen from alcoholic beverage factory wastewater using microbial electrolysis cell |
| CN115094431A (en) * | 2022-05-20 | 2022-09-23 | 中国电建集团华东勘测设计研究院有限公司 | Solar-driven microbial-electrolysis hydrogen-production synchronous organic sewage treatment system, control method and application |
| CN116162662A (en) * | 2022-12-07 | 2023-05-26 | 中国电建集团贵阳勘测设计研究院有限公司 | Hydrogen production method by using photo-assisted single-chamber microbial electrolytic cell |
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| CN102650063A (en) * | 2012-05-17 | 2012-08-29 | 大连理工大学 | Method for recovering elementary-substance cobalt from lithium cobaltate in one step by utilizing microbial electrolysis cell |
| CN102864463A (en) * | 2012-08-29 | 2013-01-09 | 杭州净洋环保科技有限公司 | H2 collection system for kitchen wastes |
| CN103865957B (en) * | 2012-12-13 | 2016-12-21 | 中国科学院城市环境研究所 | A kind of method combining hydrogen-producing acetogens and product electricity bacterium enhanced biological hydrogen manufacturing usefulness |
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| CN105803001B (en) * | 2016-05-06 | 2019-05-28 | 河海大学 | A method of realizing that excess sludge produces hydrogen using microorganism electrolysis cell |
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| CN108569757B (en) * | 2018-05-09 | 2020-11-03 | 南开大学 | Method for treating sulfonamide wastewater and synchronously producing hydrogen by using electrochemical device |
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| CN109680289A (en) * | 2018-12-28 | 2019-04-26 | 同济大学 | Manifold type bioelectrochemistry produces hydrogen and purifying plant, system and produces hydrogen methods |
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| CN109554720A (en) * | 2019-01-03 | 2019-04-02 | 江南大学 | A method of improving microorganism electrolysis cell methane production and purity |
| CN109761340A (en) * | 2019-03-26 | 2019-05-17 | 长春工程学院 | Tiny ecosystem period suitching type microorganism electrolysis cell and its operation method |
| CN110204033A (en) * | 2019-05-08 | 2019-09-06 | 南开大学 | A kind of method that microorganism electrochemical ammoniumization recycles nitrate nitrogen in waste water |
| CN110204033B (en) * | 2019-05-08 | 2021-07-23 | 南开大学 | Method for recovering nitrate nitrogen in wastewater through microbial electrochemical ammonification |
| CN112458487A (en) * | 2020-09-03 | 2021-03-09 | 南昌航空大学 | Medium-alkali asymmetric microbial electrolytic cell and application thereof in hydrogen production |
| EP4001461A3 (en) * | 2020-11-24 | 2022-06-01 | Yong Won Jeon | Method of producing hydrogen from alcoholic beverage factory wastewater using microbial electrolysis cell |
| CN115094431A (en) * | 2022-05-20 | 2022-09-23 | 中国电建集团华东勘测设计研究院有限公司 | Solar-driven microbial-electrolysis hydrogen-production synchronous organic sewage treatment system, control method and application |
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