CN114368835B - Full autotrophic denitrification method - Google Patents
Full autotrophic denitrification method Download PDFInfo
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- CN114368835B CN114368835B CN202210038288.6A CN202210038288A CN114368835B CN 114368835 B CN114368835 B CN 114368835B CN 202210038288 A CN202210038288 A CN 202210038288A CN 114368835 B CN114368835 B CN 114368835B
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/28—Anaerobic digestion processes
- C02F3/286—Anaerobic digestion processes including two or more steps
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/06—Nutrients for stimulating the growth of microorganisms
Abstract
The invention discloses a full autotrophic biological denitrification method, which adopts combination denitrification of denitrifying bacteria and anaerobic ammoxidation bacteria to convert ammonium and nitrate in wastewater into nitrogen, simultaneously deeply removes nitrate and ammonia nitrogen in the wastewater, does not need to add an organic carbon source and is completely autotrophic, obviously reduces the energy consumption and cost of denitrification, can run for a long time, ensures that the total nitrogen of the effluent of a bioreactor is less than or equal to 1 mg N/L, and ensures that the water quality can reach the class III standard of surface water.
Description
Technical Field
The invention relates to the technical field of biological denitrification, in particular to a full autotrophic biological denitrification method.
Background
The existing biological denitrification of wastewater mainly adopts a nitrification-denitrification technology, ammonium is firstly oxidized into nitrite by aerobic ammonia oxidizing bacteria, then nitrite is oxidized into nitrate by aerobic nitrite oxidizing bacteria, namely the processes of nitrosation and nitrification, and then acetic acid, methanol and the like are introduced in a mode of adding an organic carbon source, and nitrate is reduced into nitrogen by denitrifying bacteria, namely the process of denitrification. The nitrification process is an aerobic autotrophic process, the denitrification process is an anaerobic heterotrophic process, and the nitrification-denitrification technology has the common problems of long process route, high energy consumption, need of adding an organic carbon source, high cost and the like.
Anaerobic ammoxidation is a relatively energy-saving biological denitrification technology, and the principle is as follows: part of ammonium radical is oxidized into nitrite by ammonia oxidizing bacteria, and then nitrite and residual ammonium radical are converted into nitrogen together under the catalysis of anammox bacteria. In the actual operation process, measures such as dissolved oxygen, hydraulic retention time and the like are required to be controlled, so that the nitrifying process only reaches the step of nitrite, nitrite is prevented from being further oxidized into nitrate, and the denitrification technology has larger control difficulty although no organic matters are required to be added. In addition, the actual wastewater generally contains a plurality of nitrate nitrogen besides ammonia nitrogen, and the conventional anaerobic ammonia oxidation denitrification method can not remove the nitrate nitrogen in the wastewater, so that the denitrification requirement can not be met.
Disclosure of Invention
In order to solve the problems, the invention provides a full autotrophic biological denitrification method.
The invention adopts the following technical scheme:
the method is carried out by adopting a fully autotrophic biological denitrification device, the device comprises a bioreactor and a gas generator, the bioreactor comprises a water inlet end and a water outlet end, the water inlet end is arranged at the bottom end of the bioreactor, the water outlet end is arranged above the side wall of the bioreactor, a porous carrier is filled in the bioreactor, the porous carrier comprises a first reaction section and a second reaction section which are respectively adsorbed with corresponding denitrification microorganisms, the second reaction section is arranged above the first reaction section, and the gas generator is used for generating mixed gas and guiding the mixed gas into the bioreactor, wherein the mixed gas comprises hydrogen and carbon dioxide.
Further, the denitrifying microorganism comprises a denitrifying bacteria and an anaerobic ammonia oxidizing bacteria, wherein the denitrifying bacteria are adsorbed on the first reaction section of the porous carrier, the anaerobic ammonia oxidizing bacteria are adsorbed on the second reaction section of the porous carrier, and the denitrifying bacteria contain hydrogenase which can oxidize hydrogen to obtain energy for the growth of bacteria and reduce nitrate to nitrite.
Further, a gas disperser is arranged in the bioreactor near the water inlet end and is used for dispersing the mixed gas.
Further, the device also comprises a water pump, wherein the water pump is used for guiding the wastewater to be treated into the bioreactor from the water inlet end.
Further, a method for denitrification of total autotrophs comprises the following steps:
s1, filling a porous carrier in a bioreactor;
s2, inoculating denitrifying bacteria and anaerobic ammonia oxidizing bacteria to a first reaction section and a second reaction section on the porous carrier respectively;
s3, introducing mixed gas of hydrogen and carbon dioxide into the water inlet end of the bioreactor;
s4, introducing wastewater to be treated into the water inlet end of the bioreactor, and performing circulating operation firstly, wherein continuous flow operation is changed into when the biomass of the denitrifying bacteria hydroxide and the anaerobic ammonia oxidizing bacteria in the porous carrier is maximized;
s5, according to denitrification conditions, the flow of the wastewater is gradually adjusted to control the residence time of the wastewater in the bioreactor until the denitrification efficiency is maximized.
Further, the porous carrier adopts any one or any two of ceramics, diatomite, zeolite and fiber.
Further, the denitrifying bacteria are pure denitrifying bacteria or enriched denitrifying bacteria.
Further, the anaerobic ammonia oxidizing bacteria are pure anaerobic ammonia oxidizing bacteria or enrichment of anaerobic ammonia oxidizing bacteria.
Further, the mixed gas of the hydrogen and the carbon dioxide is generated by any one mode of methanol pyrolysis, natural gas pyrolysis, biomass pyrolysis or mixing pure hydrogen and pure carbon dioxide.
After the technical scheme is adopted, compared with the background technology, the invention has the following advantages:
1. aiming at the problem that the wastewater contains ammonia nitrogen and nitrate nitrogen, the invention provides a method for combined denitrification by adopting denitrifying bacteria and anaerobic ammonia oxidizing bacteria, which utilizes the denitrifying bacteria to convert the nitrate nitrogen into nitrite nitrogen, and then converts the nitrite nitrogen and the ammonia nitrogen into nitrogen by the anaerobic ammonia oxidizing bacteria, so that the ammonia nitrogen and the nitrate nitrogen in the wastewater can be removed deeply at the same time to meet the denitrification requirement;
2. the mixed gas of the hydrogen and the carbon dioxide introduced into the bioreactor not only plays a role in removing oxygen in the bioreactor to provide an anaerobic environment, but also serves as an inorganic carbon source of the hydrogen oxidation denitrifying bacteria and the anaerobic ammonia oxidation bacteria to provide energy, in addition, the hydrogen oxidation denitrifying bacteria contain hydrogenase which can oxidize the hydrogen to obtain energy for the growth of bacteria and the reduction of nitrate into nitrite, and the anaerobic ammonia oxidation bacteria further convert nitrite generated in the last step and ammonia in wastewater into nitrogen, so that the denitrification method does not need to add an additional organic carbon source and is completely autotrophic, and the energy consumption and cost of denitrification are obviously reduced;
3. the denitrifying bacteria and the anaerobic ammonia oxidizing bacteria are loaded on the porous material by pure species or high-purity concentrates, so that effective interception in functional bacteria is realized, very high denitrification rate can be realized when high-concentration and low-concentration nitrogen-containing wastewater is treated, the difficult problem of poor denitrification effect due to low microorganism content in low-ammonia nitrogen wastewater is solved, deep denitrification in water is realized, and the quality of effluent water from a bioreactor can reach the class III standard of surface water;
4. the invention also provides a corresponding denitrification device which has simple structure and easy control, two types of bacteria are simultaneously fixed in the bioreactor containing the porous carrier, and mixed gas of hydrogen and carbon dioxide is introduced into the bioreactor through the gas generator, so that the deep removal of nitrate nitrogen and ammonia nitrogen is simultaneously completed in one bioreactor, the device can be operated for a long time under the condition of not adding an organic carbon source, and the total nitrogen in the effluent of the reactor is less than or equal to 1 mg N/L.
Drawings
FIG. 1 is a schematic view of a denitrification apparatus according to the present invention;
FIG. 2 is a graph showing the variation of the concentration of tri-nitrogen in water fed and discharged by combined denitrification in the fourth embodiment with time;
FIG. 3 is a graph showing the concentration of ammonia nitrogen and nitric acid in the water fed from the nitration reaction in the fifth embodiment over time;
FIG. 4 is a graph showing the concentration of ammonia nitrogen and nitric acid in water fed into and discharged from the combined denitrification process in the fifth embodiment.
Reference numerals illustrate:
1. a bioreactor; 11. a water inlet end; 111. a water inlet; 112. an air inlet; 12. a water outlet end; 121. a water outlet; 122. an air outlet; 13. a first sampling port; 14. a second sampling port;
2. a gas generator; 21. a gas flow meter; 22. a gas circulation pump;
3. a porous support; 31. a first reaction section; 32. a second reaction section;
4. a gas disperser;
5. a water pump;
6. a gas collection chamber.
Description of the embodiments
The present invention will be described in further detail with reference to the drawings and examples, in order to make the objects, technical solutions and advantages of the present invention more apparent. It should be understood that the specific embodiments described herein are for purposes of illustration only and are not intended to limit the scope of the invention.
Examples
As shown in fig. 1, a total autotrophic biological nitrogen removal device comprises a bioreactor 1 and a gas generator 2, wherein the bioreactor 1 comprises a water inlet end 11 and a water outlet end 12, the inside of the bioreactor 1 is filled with a porous carrier 3, the porous carrier 3 comprises a first reaction section 31 and a second reaction section 32 which are respectively adsorbed with corresponding nitrogen removal microorganisms, and the gas generator 2 is used for generating mixed gas and guiding the mixed gas into the bioreactor 1.
A gas disperser 4 is also arranged in the bioreactor 1 near the water inlet end 11, and the gas disperser 4 is used for dispersing the mixed gas. The side wall of the bioreactor 1 is respectively provided with a first sampling port 13 and a second sampling port 14 at the first reaction section 31 and the second reaction section 32, and the first sampling port 13 and the second sampling port 14 are used for sampling and observing water quality in the bioreactor 1 in real time. The water inlet end 11 of the bioreactor 1 is provided with a water inlet 111 and an air inlet 112, and the water outlet end 12 is provided with a water outlet 121 and an air outlet 122. The diameter of the bioreactor 1 of this example is 10 cm, 1 m high.
The denitrifying microorganism comprises denitrifying bacteria which are adsorbed on the porous carrier 3 in a first reaction section 31 and anaerobic ammonia oxidizing bacteria which are adsorbed on the porous carrier 3 in a second reaction section 32.
The gas generator 2 of the present embodiment adopts a hydrogen and carbon dioxide mixed generator, and the generated mixed gas contains hydrogen and carbon dioxide. A gas collection chamber 6 communicated with the gas outlet 122 is arranged at the water outlet end 12 of the bioreactor 1, and the gas collection chamber 6 is used for collecting excessive mixed gas in the bioreactor 1; a gas circulation pump 22 is provided between the gas generator 2 and the gas inlet 112, the inlet of the gas circulation pump 22 being connected to both the gas generator 2 and the gas outlet 122 of the bioreactor 1 for circulating excess mixed gas in the bioreactor 1. A gas flow meter 21 is further provided between the gas circulation pump 22 and the gas inlet 112, and the flow rate of the mixed gas can be controlled by adjusting the switch of the gas flow meter 21.
And a water pump 5 is also included, and the water pump 5 is used for guiding the wastewater to be treated into the bioreactor 1 from the water inlet end 11.
Examples
1. Screening of denitrifying bacteria for hydrogen oxidation
The source of the screening strain is sludge in a denitrification tank of a sewage treatment plant, and a proper amount of strain to be screened is added into the prepared autotrophic denitrification culture medium. The autotrophic denitrification culture medium comprises the following components: KNO (KNO) 3 1 g/L，NaHCO 3 1.2 g/L，KH 2 PO 4 0.2 g/L. The culture was performed in a 150 mL anaerobic jar, the anaerobic jar was filled with a liquid of 50. 50 mL and filled with an excessive amount of hydrogen. The change of the nitrate radical concentration is measured by sampling every day, when the nitrate radical concentration is reduced to below 0.5mg N/L, nitrate radical and hydrogen are added, the bacterial liquid is transferred after the nitrate radical is added twice, the transfer quantity is 20% (10 mL), and the components of the culture medium are the same as the above. And transferring again after all nitrate is reduced to nitrogen, repeating the process for three times, and obtaining pure seeds of the denitrifying bacteria by adopting an anaerobic agar plate coating method. The agar plates were composed as follows: KNO (KNO) 3 1 g/L，NaHCO 3 1.2 g/L，KH 2 PO 4 0.2 g/LPeptone 0.1 g/L and agar concentration 2%. The headspace of the plate was filled with hydrogen and sealed with a seal. After about three days, individual colonies were grown on the solid medium and plated onto new agar plates, and this was repeated three times. Single colonies were picked into peptone 1 g/L, yeast powder 0.5 g/L, naCl 2 g/L medium. 200 Shaking culture at rpm until OD600 = 1.0, centrifuging bacterial liquid at 2000 g for 3 min, and water washing and centrifuging to obtain bacterial mud. The bacterial mud is fixed in volume in autotrophic denitrification culture medium, and is cultivated in a sealed way, and the bottle is filled with hydrogen. Its denitrification capacity was measured. The isolated and purified bacteria were subjected to 16S rDNA sequencing, and the classification of the denitrifying bacteria was Thauera mechernichensis, and the purity was 99.95%.
2. Domestication and enrichment of anaerobic ammonia oxidizing bacteria
The source of the screening strain is anaerobic sludge in an anaerobic tank of a sewage treatment plant. And adding a proper amount of anaerobic sludge into the configured anaerobic ammonia oxidation culture medium. The anaerobic ammonia oxidation culture medium comprises the following components: NH (NH) 4 Cl 0.21 g/L，NaNO 2 0.36g/L，NaHCO 3 1.2 g/L，KH 2 PO 4 0.2 g/L. The anaerobic bottle was used for closed culture with a 150 mL anaerobic bottle filled with a liquid volume of 120 mL and filled with an excess of argon for removing oxygen from the water. The ammonium and nitrite concentration changes were measured by daily sampling, and the molar ratio of ammonium to nitrite removal was measured to be approximately 1:1.32, the successful domestication of anaerobic ammonia oxidizing bacteria in anaerobic sludge is indicated. And (5) measuring the ammonium and nitrite contents in the anaerobic bottle to be lower than 0.5mg N/L, and continuously supplementing the ammonium, nitrite and sodium bicarbonate into the bottle to supplement enough carbon sources and nitrogen sources for the growth and propagation of the anaerobic ammonium oxidation bacteria. And (3) obtaining the high-purity enriched anaerobic ammonia oxidizing bacteria through long-term culture. The enriched bacteria were subjected to 16S rDNA sequencing, and the classification of the anaerobic ammonium oxidation bacteria was Candidatus Kuenenia, and the purity was 51.95%.
Examples
Immobilization of biological carriers of denitrifying bacteria and anaerobic ammonia oxidizing bacteria:
the bioreactor of this example had a diameter of 10 cm and a height of 100 cm, and was packed with ceramic porous material having a diameter of about 5 mm, and the voids of the ceramic material were 60%.
The simulated wastewater contains ammonia nitrogen, nitrite nitrogen and nitrate nitrogen, and comprises the following specific components: NH (NH) 4 Cl 0.31 g/L，NaNO 2 0.35 g/L，KNO 3 0.5 g/L，NaHCO 3 1.2 g/L，KH 2 PO 4 0.2 g/L。
The bottom of the bioreactor is provided with a gas disperser, and the mixed gas of hydrogen and carbon dioxide generated by methanol pyrolysis is introduced. The gas generated by methanol pyrolysis comprises 70% of hydrogen and about 25% of carbon dioxide.
And respectively placing a proper amount of ceramic porous materials into the bacterial liquid of the pure cultured Thauera mechernichensis denitrifying bacteria and the enriched and purified anaerobic ammonia oxidizing bacteria. Standing for five days to allow the filler to fully adsorb bacterial liquid, allowing the bacterial to enter the micron holes, and respectively adding inorganic carbon source and nitrogen source into the two culture flasks to allow the bacterial to continuously grow and enrich in the biological filler. Then respectively placing the ceramic porous materials with adsorbed strains in a reactor, and respectively placing the ceramic porous materials with adsorbed denitrifying bacteria and the ceramic porous materials with adsorbed anaerobic ammonia oxidation bacteria in a first reaction section and a second reaction section. Introducing hydrogen into the bottom of the culture medium reactor in the bioreactor, firstly circularly running the reactor to maximize biomass of microorganisms in the porous carrier, then changing the reactor into continuous flow running, and gradually adjusting the hydraulic retention time from large to small according to denitrification condition until the denitrification efficiency is maximized.
Examples
The embodiment utilizes the combination of the denitrifying bacteria and the anaerobic ammonia oxidizing bacteria to treat the high ammonia nitrogen wastewater, and the high ammonia nitrogen wastewater is particularly aquaculture wastewater. The concentrations of ammonia nitrogen, nitrite nitrogen and nitrate nitrogen in the wastewater are respectively 50 mg N/L, 5mg N/L and 50 mg N/L, and the COD concentration is 100 mg O 2 The wastewater is stored in a reservoir and enters a bioreactor through a water pump, wherein the diameter of the bioreactor is 10 cm, the height of the bioreactor is 1 m, and porous carriers are respectively arranged in the bioreactor. Pure cultured Thauera mechernichensis denitrifying bacteria, enriched high-purity anaerobic ammonia oxidizing bacteria respectively adsorbed on a first reaction section and a second reaction section on a porous carrier, a gas disperser arranged at the bottom of the bioreactor, and a gasThe generator is a hydrogen and carbon dioxide mixed generation device, and the flow rate of the mixed gas is controlled to be about 20 mL/min through the switch of the gas flowmeter. Maintaining dissolved oxygen < 2 mg O in bioreactor 2 and/L. The water quality of the water inlet and outlet of the bioreactor which changes along with time is shown in figure 2, after 30 days of operation, ammonia nitrogen in the water is 0.3 mg N/L, nitrite nitrogen is 0.1 mg N/L and nitrate nitrogen is 0.5mg N/L, total nitrogen is less than or equal to 1 mg N/L, and the index of the three nitrogen reaches the standard of surface water III.
Examples
In the embodiment, the low ammonia nitrogen wastewater is treated by combining the denitrifying bacteria and the anaerobic ammonia oxidizing bacteria, and the low ammonia nitrogen wastewater is specifically municipal wastewater-like primary B effluent, wherein the ammonia nitrogen concentration is 15 mg N/L, and the nitrate concentration is 3 mg N/L. If the conventional anaerobic ammonia oxidation denitrification technology is adopted, part of ammonia nitrogen is required to be oxidized into nitrite nitrogen by utilizing aerobic Ammonia Oxidizing Bacteria (AOB), but the nitrite is further oxidized into nitrate due to the fact that the AOB and Nitrite Oxidizing Bacteria (NOB) belong to aerobic bacteria. In the embodiment, part of ammonia nitrogen wastewater is oxidized into nitrate under the condition of not limiting aeration, then the nitrate wastewater and the rest raw water enter a bioreactor together, dissolved oxygen is rapidly removed by a method of exposing mixed gas, and the speed of reducing nitrate into nitrite is controlled by a method of controlling hydrogen. Because only ammonia nitrogen exists, part of the wastewater can be nitrified to generate the nitrogen nitrate required by the invention. Part of the wastewater is subjected to traditional nitrification treatment to generate 15 mg N/L of nitrogen nitrate wastewater, the nitrified wastewater and the original ammonia nitrogen wastewater are mixed to form ammonia nitrogen and nitrogen nitrate wastewater, the ammonia nitrogen and nitrogen nitrate wastewater enter the denitrification device of the embodiment, and other parts are the same as the fourth embodiment. The water quality of the water inlet and outlet of the traditional nitration reactor which changes along with time is shown in figure 3, the water quality of the water inlet and outlet of the oxidation reactor which changes along with time is shown in figure 4, after 30 days of operation, ammonia nitrogen in the water outlet is less than or equal to 0.3 mg N/L, nitrite nitrogen is less than or equal to 0.2 mg N/L, nitrate nitrogen is less than or equal to 0.5mg N/L, total nitrogen is less than or equal to 1 mg N/L, and the three nitrogen index reaches the standard of surface water class III.
The present invention is not limited to the above-mentioned embodiments, and any changes or substitutions that can be easily understood by those skilled in the art within the technical scope of the present invention are intended to be included in the scope of the present invention. Therefore, the protection scope of the present invention should be subject to the protection scope of the claims.
Claims (8)
1. A full autotrophic nitrogen removal method is characterized in that: the method is carried out by adopting a full autotrophic biological denitrification device, the device comprises a bioreactor and a gas generator, the bioreactor comprises a water inlet end and a water outlet end, the water inlet end is arranged at the bottom end of the bioreactor, the water outlet end is arranged above the side wall of the bioreactor, a porous carrier is filled in the bioreactor, the porous carrier comprises a first reaction section and a second reaction section, the first reaction section and the second reaction section are respectively adsorbed with corresponding denitrification microorganisms, the second reaction section is arranged above the first reaction section, and the gas generator is used for generating mixed gas and introducing the mixed gas into the bioreactor, and the mixed gas comprises hydrogen and carbon dioxide;
the denitrifying microorganism comprises denitrifying bacteria and anaerobic ammonia oxidizing bacteria, wherein the denitrifying bacteria are adsorbed on the first reaction section of the porous carrier, the anaerobic ammonia oxidizing bacteria are adsorbed on the second reaction section of the porous carrier, and the denitrifying bacteria contain hydrogenase which can oxidize hydrogen to obtain energy for the growth of thalli and reduce nitrate to nitrite.
2. A method of total autotrophic anammox as defined in claim 1, wherein: and a gas disperser is arranged in the bioreactor and close to the water inlet end, and the gas disperser is used for dispersing the mixed gas.
3. A method of total autotrophic anammox as claimed in claim 2, wherein: the device also comprises a water pump, wherein the water pump is used for guiding the wastewater to be treated into the bioreactor from the water inlet end.
4. A method of denitrification of total autotrophs as claimed in any one of claims 1-3, wherein: the method comprises the following steps:
s1, filling a porous carrier in a bioreactor;
s2, inoculating denitrifying bacteria and anaerobic ammonia oxidizing bacteria to a first reaction section and a second reaction section on the porous carrier respectively;
s3, introducing mixed gas of hydrogen and carbon dioxide into the water inlet end of the bioreactor;
s4, introducing wastewater to be treated into the water inlet end of the bioreactor, and performing circulating operation firstly, wherein continuous flow operation is changed into when the biomass of the denitrifying bacteria hydroxide and the anaerobic ammonia oxidizing bacteria in the porous carrier is maximized;
s5, according to denitrification conditions, the flow of the wastewater is gradually adjusted to control the residence time of the wastewater in the bioreactor until the denitrification efficiency is maximized.
5. The method for denitrification of an autotroph as claimed in claim 4, wherein: the porous carrier adopts any one or any two of ceramics, diatomite, zeolite and fibers.
6. The method for denitrification of total autotrophs as claimed in claim 5, wherein: the denitrifying bacteria are pure denitrifying bacteria or enriched denitrifying bacteria.
7. The method for denitrification of total autotrophs as claimed in claim 5, wherein: the anaerobic ammonia oxidizing bacteria are pure anaerobic ammonia oxidizing bacteria or enrichment of anaerobic ammonia oxidizing bacteria.
8. The method for denitrification of an autotroph as claimed in claim 4, wherein: the mixed gas of the hydrogen and the carbon dioxide is produced by any one mode of high-temperature methanol pyrolysis, natural gas pyrolysis, biomass pyrolysis or pure hydrogen and pure carbon dioxide.
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