CN107024521B - Detect sewage concentration's biosensor - Google Patents
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- CN107024521B CN107024521B CN201710269994.0A CN201710269994A CN107024521B CN 107024521 B CN107024521 B CN 107024521B CN 201710269994 A CN201710269994 A CN 201710269994A CN 107024521 B CN107024521 B CN 107024521B
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- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
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Abstract
The invention provides a biosensor for detecting sewage concentration, which is of a tubular structure and comprises an anode chamber (1), an air cathode (2), a carbon brush (6) and a water distribution plate (7). The anode chamber (1) is filled with carbon materials, and the carbon brush (6) is adopted for conducting electricity to form a composite microorganism enrichment system. The biosensor adopts a continuous feeding mode, and the Biochemical Oxygen Demand (BOD) detection range is 50-1000 mg/L. The biosensor has the advantages of stable operation, no need of strict anaerobic operation, strong tolerance, low maintenance cost and the like, and can be used for monitoring the two-stage anaerobic fermentation process of the HYTHANE, including but not limited to the detection of municipal sewage, agricultural wastewater and other sewage.
Description
Technical Field
The invention belongs to the technical field of water quality monitoring, and particularly relates to a biosensor for detecting sewage concentration.
Background
With the rapid development of economy, the industrialization and urbanization construction process of China is gradually accelerated, and the problem of environmental pollution is brought, and the problem of water pollution is the most prominent. The microbial fuel cell can convert chemical energy of organic matters into electric energy, and provides a new way for removing organic pollutants in the environment and producing clean energy.
Biochemical Oxygen Demand (BOD) is an important indicator of water quality monitoring. The traditional BOD monitoring needs 5 days, takes long time and is not suitable for real-time online monitoring. A microbial fuel cell is a device that converts chemical energy into electrical energy, and under certain conditions, the electricity generation and current are proportional to the concentration of metabolic substrates or the number of microorganisms added to the anode compartment, so that both can be used for rapid BOD detection.
The two-stage anaerobic fermentation can improve the utilization rate of raw materials and the yield of biomass energy to the maximum extent. However, the indexes of the current two-stage anaerobic fermentation online monitoring mainly comprise volatile organic acid, pH, dissolved oxygen and the like, while BOD is not effectively monitored in real time, and the detection of BOD is still in the research stage.
Chinese patent "carbon nanotube carrier type microbial electrochemical device for continuously treating sewage and generating electricity" (publication No. CN 103326052A) discloses an anode material of a carbon nanotube, which can continuously and efficiently treat sewage, and the used device is a double-chamber structure, but no further research is carried out on water quality detection.
Chinese patent publication No. CN101620201A provides a biochemical oxygen demand measuring method, which constructs a single-chamber air cathode mediator-free microbial fuel cell, and obtains a good linear curve by using intermittent feeding, but has the problems of repeated cleaning of intermittent feeding and small measuring range.
Chinese patent publication No. CN103207230 discloses a method for constructing a two-chamber microbial fuel cell type BOD sensor using potassium permanganate as cathode electron acceptor, which greatly expands the BOD detection range, but potassium permanganate needs to be added in the cathode chamber, and the electrical signal is interfered by metal ions during long-term operation.
The Chinese patent (publication No. CN 103326052A) uses the microbial fuel cell for organic fermentation process detection, and has stable operation and timely signal, but adopts a double-chamber structure, needs a cathode chamber for oxygen supply, and has complex operation.
Disclosure of Invention
The invention aims to provide a biosensor for detecting sewage concentration, which aims at overcoming the defects of the prior art, realizes continuous and rapid detection of water quality, enlarges the detection range, and has the characteristics of low cost, simple operation, and being exquisite and portable.
The technical scheme adopted by the invention for solving the technical problems is as follows:
a biosensor for detecting sewage concentration is of a tubular structure and comprises an anode chamber 1, an air cathode 2, a carbon brush 6 and a water distribution plate 7.
The tubular structure of the biosensor is internally provided with an anode chamber 1, the top end of the tubular structure is provided with a cover 12, the cover 12 is provided with a discharge hole 4, and the bottom end of the tubular structure is of a funnel-shaped structure and is provided with a feed inlet 5. A water distribution plate 7 is arranged inside the bottom end of the tubular structure of the biosensor, the water distribution plate 7 is fixed on the inner side of the tubular structure, and water distribution holes are formed in the water distribution plate 7. The carbon brush 6 extends into the tubular structure of the biosensor through the cover 12 and extends into the water distribution holes to be fixed on the water distribution plate 7. The wall of the biosensor pipe is evenly distributed with round holes 3.
The anode chamber 1 is filled with a microorganism carrier.
Air cathode 2 includes waterproof carbon cloth and organic glass cylinder, and waterproof carbon cloth parcel organic glass cylinder is fixed in the biosensor pipe wall outside, covers round hole 3 on the pipe wall simultaneously. The side of the organic glass cylinder of the air cathode 2, which is contacted with the tube wall, is coated with a platinum-carbon catalyst. And titanium wires are wound on the outer side of the waterproof carbon cloth of the air cathode 2.
An external resistor 9 is connected in series between the air cathode 2 and the carbon brush 6 by a lead. The external resistor 9 is connected with the data acquisition card 10 in parallel, and the data acquisition card 10 is electrically connected with the electronic computer 11.
The Biochemical Oxygen Demand (BOD) detection range of the biosensor is 50-1000 mg/L.
When the biosensor is started, the anode chamber 1 is inoculated with organic sewage and anaerobic sludge.
The biosensor tubular structure is made of organic glass.
The diameter of the tubular structure of the biosensor is 3.5cm, the height of the tubular structure is 12cm, the wall thickness of the tubular structure is 0.5cm, and the total volume of the tubular structure is 115 mL.
The diameter of the round holes 3 is 2mm, the number of the round holes 3 is 200-220, and the total area of the round holes 3 is 6.6cm2。
The microbial carrier filled in the anode chamber 1 is one of carbon nano tubes, activated carbon and graphene.
The carbon brush 6 comprises a brush rod and brush bristles, and the brush bristles are circumferentially arranged on the brush rod; the total length of the brush rod is 12cm, wherein the length of a brushing area on the brush rod is 11 cm; the bristles are 1.5cm long.
The platinum-carbon catalyst contains 20% of platinum, and the platinum content distribution is as follows: the waterproof carbon cloth contained 0.5mg of platinum per square centimeter.
The side surface of the bottom of the tubular structure is also provided with a sampling port 8.
The invention has the beneficial effects that:
1) the invention provides a biosensor for detecting sewage concentration, wherein an anode chamber of the biosensor is filled with carbon materials, and a carbon brush is adopted for conducting electricity to form a composite microorganism enrichment system;
2) the biosensor for detecting the sewage concentration provided by the invention adopts continuous feeding, and can improve the BOD detection range to 50-1000 mg/L;
3) the biosensor for detecting the sewage concentration provided by the invention has the advantages of stable operation, no need of strict anaerobic operation, strong tolerance, low maintenance cost and the like;
4) the biosensor for detecting the sewage concentration can be used for monitoring a two-stage anaerobic fermentation process of hydrogen alkane, including but not limited to municipal sewage, agricultural wastewater and the like.
Drawings
FIG. 1 is a schematic view of a biosensor for detecting sewage concentration according to the present invention;
FIG. 2 is a Biochemical Oxygen Demand (BOD) standard curve of a biosensor for detecting sewage concentration according to the present invention.
Reference numerals:
1 anode chamber 2 air cathode 3 round hole 4 discharge hole
5 sampling port with 6 carbon brushes, 7 water distribution plates and 8 water distribution plates at feeding port
9 external resistor 10 data acquisition card 11 electronic computer 12 lid
Detailed Description
The invention will be further explained with reference to the drawings.
Referring to fig. 1, a biosensor for detecting sewage concentration is a tubular structure, and includes an anode chamber 1, an air cathode 2, a carbon brush 6, and a water distribution plate 7. Wherein the content of the first and second substances,
the tubular structure of the biosensor is internally provided with an anode chamber 1, the top end of the tubular structure is provided with a cover 12, the cover 12 is provided with a discharge hole 4, and the bottom end of the tubular structure is of a funnel-shaped structure and is provided with a feed inlet 5. A water distribution plate 7 is arranged inside the bottom end of the tubular structure of the biosensor, the water distribution plate 7 is fixed on the inner side of the tubular structure, and water distribution holes are formed in the water distribution plate 7. The carbon brush 6 extends into the tubular structure of the biosensor through the cover 12 and extends into the water distribution holes to be fixed on the water distribution plate 7. The wall of the biosensor pipe is evenly distributed with round holes 3. Preferably, the number of the circular holes 3 is 200-220. The side surface of the bottom of the tubular structure is also provided with a sampling port 8.
The anode chamber 1 is filled with a microorganism carrier.
Air cathode 2 includes waterproof carbon cloth and organic glass cylinder, and waterproof carbon cloth parcel organic glass cylinder is fixed in the biosensor pipe wall outside, covers round hole 3 on the pipe wall simultaneously. The side of the organic glass cylinder of the air cathode 2, which is contacted with the tube wall, is coated with a platinum-carbon catalyst. And a circle of titanium wire is wound on the outer side of the waterproof carbon cloth of the air cathode 2. An external resistor 9 is connected in series between the air cathode 2 and the carbon brush 6 by a lead. The external resistor 9 is connected with the data acquisition card 10 in parallel, and the data acquisition card 10 is electrically connected with the electronic computer 11. The data acquisition card 10 acquires voltage signals at two ends of the load external resistor 9 and then transmits the voltage signals to the electronic computer 11 for data acquisition and processing.
Preferably, the tubular structure of the biosensor is made of organic glass.
Preferably, the biosensor tubular structure has a diameter of 3.5cm, a height of 12cm, a wall thickness of 0.5cm and a total volume of 115 mL.
Preferably, the diameter of the round holes 3 is 2mm, the number of the round holes 3 is 200-220, and the sum of the areas of the round holes 3 is 6.6cm2。
Preferably, the microbial carrier filled in the anode chamber 1 is one of carbon nanotubes, activated carbon and graphene.
Preferably, the carbon brush 6 includes a brush bar and bristles arranged circumferentially on the brush bar. The total length of the brush rod is 12cm, wherein the length of a bristle area on the brush rod is 11 cm. The bristles are 1.5cm long.
Preferably, the product number of the waterproof carbon cloth is W1S1005, the platinum content in the platinum-carbon catalyst is 20%, and the platinum content distribution is as follows: the waterproof carbon cloth contained 0.5mg of platinum per square centimeter.
The Biochemical Oxygen Demand (BOD) detection range of the biosensor is 50-1000 mg/L.
When the biosensor is started, organic sewage and anaerobic sludge are inoculated in the anode chamber 1, wherein the organic sewage is used as electrolyte, and the anaerobic sludge provides electrogenesis microorganisms.
The working process of the invention is as follows:
a biosensor for detecting the sewage concentration comprises the following steps of:
A) sludge is inoculated into the anode chamber 1 of the biosensor, the organic load is controlled to be 2.5g/L/d, the microorganism carrier filled in the anode chamber 1 enriches electrochemically active microorganisms, and the external resistor R is adjusted to be 100 omega. And when the voltage value acquired by the data acquisition card 10 is stable, the start of the biosensor is considered to be finished.
B) Preparing Biochemical Oxygen Demand (BOD) solutions with different concentrations.
C) Continuously feeding Biochemical Oxygen Demand (BOD) solutions with different concentrations in the step B) through a feeding port 5 and keeping a certain Hydraulic Retention Time (HRT).
D) And (3) measuring the continuous stable current I in the reaction process, drawing the concentration of the continuous stable current I of the biosensor to different Biochemical Oxygen Demand (BOD) and performing linear fitting to obtain a BOD standard curve.
E) And continuously feeding a water sample to be detected through the feeding hole 5, reading the voltage after the voltage value is stable, and calculating and determining the continuous stable current I' in the reaction process.
F) Substituting the I' obtained in the step E) into the standard curve in the step D) to calculate the BOD value.
Example 1
The two-stage anaerobic fermentation process of HYTHANE was monitored.
Two-stage anaerobic fermentation of hydrogen alkane: an upflow anaerobic sludge blanket reactor (UASB) is adopted for hydrogen-alkane two-stage anaerobic fermentation. The working volume of an upflow anaerobic sludge blanket reactor (UASB) is 2.5L, the fermentation temperature is 37 ℃, and the hydraulic retention time HRT is 24 h. The organic load of the hydrogen-producing stage of the two-stage anaerobic fermentation of the HYTHANE is 10gCOD/L/d, and the organic load of the methanogenic stage is 5 gCOD/L/d. The upflow anaerobic sludge blanket reactor (UASB) was operated for 2 months, during which time the pH, oxidation-reduction potential (ORP) and gas production in the reactor were monitored in real time.
After an up-flow anaerobic sludge bed reactor (UASB) is stabilized, the hydrogen yield of the hydrogen production stage is 0.94L/L/d, the pH value is stabilized at 3.7, the methane yield of the methane production stage is 1.64L/L/d, and the pH value is stabilized at 7.
After the upflow anaerobic sludge blanket reactor (UASB) is operated stably, a biosensor is installed at the fermentation end, and the two-stage anaerobic fermentation process of the HYTHANE is monitored. The working process of the biosensor is as follows:
A) sludge is inoculated into the anode chamber 1 of the biosensor, the organic load is controlled to be 2.5g/L/d, the microorganism carrier filled in the anode chamber 1 enriches electrochemically active microorganisms, and the external resistor R is adjusted to be 100 omega. And when the voltage value acquired by the data acquisition card 10 is stable, the start of the biosensor is considered to be finished.
Wherein, the microorganism carrier in the anode chamber 1 of the biosensor is a carbon nano tube and a carbon brush. The number of the circular holes 3 of the biosensor is 210. The sludge is digested sludge from a minired Men sewage treatment plant in Beijing.
B) Preparing Biochemical Oxygen Demand (BOD) solutions with different concentrations and adjusting the pH value.
Wherein, the Biochemical Oxygen Demand (BOD) solution concentration is respectively as follows: 89mg/L, 181mg/L, 267mg/L, 448mg/L, 622g/L, 800g/L, 889 mg/L. The pH values are all adjusted to 7.
C) The Biochemical Oxygen Demand (BOD) solutions of different concentrations in step a) were fed continuously through the feed port 5 and the hydraulic retention time HRT was kept at 2 hours.
D) And (3) measuring the continuous stable current I in the reaction process, drawing the concentration of the continuous stable current I of the biosensor to different Biochemical Oxygen Demand (BOD) and performing linear fitting to obtain a BOD standard curve. The resulting standard curve is:
I＝0.0024BOD+0.4726
wherein, the standard deviation is: r2＝0.9806。
Wherein, the detection time of the stable current I is 8 h.
E) And continuously feeding a water sample to be detected through the feeding hole 5, reading the voltage after the voltage value is stable, and calculating and determining the continuous stable current I' in the reaction process.
Wherein, the water sample to be detected and the measured continuous stable current I' are respectively:
a. hydrogen production stage: diluting the fermentation effluent by 30 times and continuously stabilizing the current I'1It was 1.24 mA.
b. A methanogenesis stage: the fermented effluent of the methanogenesis stage is measured as the steady current I'2And was 2.58 mA.
F) Substituting the I' obtained in the step E) into the standard curve in the step D) to calculate the BOD value. The standard curve is shown in fig. 2. The BOD values were calculated to be 319mg/L and 878mg/L, respectively.
The existing BOD detector is adopted to detect the two-stage fermentation water, and the measured BOD concentrations are 275mg/L and 750mg/L respectively.
The BOD value measured by the biosensor is compared with the value measured by the existing BOD measuring instrument, so that the absolute errors of the BOD value measured by the biosensor are respectively 16% and 17%. Therefore, the condition of organic matters in the anaerobic reactor can be effectively reflected by the biosensor in the design.
Claims (6)
1. A biosensor for detecting sewage concentration, the biosensor is a tubular structure, and is characterized in that: the biosensor comprises an anode chamber (1), an air cathode (2), a carbon brush (6) and a water distribution plate (7); wherein the content of the first and second substances,
the inside of the tubular structure of the biosensor is provided with an anode chamber (1), the top end of the tubular structure is provided with a cover (12), the cover (12) is provided with a discharge hole (4), and the bottom end of the tubular structure is provided with a funnel-shaped structure and a feed hole (5); a water distribution plate (7) is arranged inside the bottom end of the tubular structure of the biosensor, the water distribution plate (7) is fixed on the inner side of the tubular structure, and water distribution holes are formed in the water distribution plate (7); the carbon brush (6) passes through the cover (12) and extends into the tubular structure of the biosensor, and extends into the water distribution hole to be fixed on the water distribution plate (7); round holes (3) are uniformly distributed on the wall of the biosensor tube;
the anode chamber (1) is filled with a microorganism carrier;
the air cathode (2) comprises waterproof carbon cloth and an organic glass cylinder, the organic glass cylinder is wrapped by the waterproof carbon cloth and fixed on the outer side of the tube wall of the biosensor, and meanwhile, the waterproof carbon cloth covers the round hole (3) on the tube wall; one side of the organic glass cylinder of the air cathode (2) which is contacted with the tube wall is coated with a platinum-carbon catalyst; titanium wires are wound on the outer side of the waterproof carbon cloth of the air cathode (2);
an external resistor (9) is connected between the air cathode (2) and the carbon brush (6) in series through a lead; the external resistor (9) is connected with the data acquisition card (10) in parallel, and the data acquisition card (10) is electrically connected with the electronic computer (11);
the Biochemical Oxygen Demand (BOD) detection range of the biosensor is 889 mg/L;
when the biosensor is started, organic sewage and anaerobic sludge are inoculated in the anode chamber (1);
the microbial carrier filled in the anode chamber (1) is a carbon nano tube;
the platinum-carbon catalyst contains 20% of platinum, and the platinum content distribution is as follows: the waterproof carbon cloth contained 0.5mg of platinum per square centimeter.
2. The biosensor for detecting sewage concentration according to claim 1, wherein: the biosensor tubular structure is made of organic glass.
3. The biosensor for detecting sewage concentration according to claim 1, wherein: the diameter of the tubular structure of the biosensor is 3.5cm, the height of the tubular structure is 12cm, the wall thickness of the tubular structure is 0.5cm, and the total volume of the tubular structure is 115 mL.
4. The biosensor for detecting sewage concentration according to claim 1, wherein: the diameter of the round holes (3) is 2mm, the number of the round holes (3) is 200-220, and the sum of the areas of the round holes (3) is 6.6cm2。
5. The biosensor for detecting sewage concentration according to claim 1, wherein: the carbon brush (6) comprises a brush rod and brush bristles, and the brush bristles are circumferentially arranged on the brush rod; the total length of the brush rod is 12cm, wherein the length of a brushing area on the brush rod is 11 cm; the bristles are 1.5cm long.
6. The biosensor for detecting sewage concentration according to claim 1, wherein: the side surface of the bottom of the tubular structure is also provided with a sampling port (8).
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| CN104458862A (en) * | 2014-12-02 | 2015-03-25 | 清华大学 | Water quality monitoring device and preparation method thereof |
| CN106450398A (en) * | 2016-10-06 | 2017-02-22 | 浙江大学 | Method for quickly building microbial fuel cell nitrification system |
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| CA2765767C (en) * | 2009-06-16 | 2017-09-26 | Cambrian Innovation, Inc. | Systems and devices for treating and monitoring water, wastewater and other biodegradable matter |
| CN101620201B (en) * | 2009-08-03 | 2012-07-18 | 广东省生态环境与土壤研究所 | Measuring method of biochemical oxygen demand and BOD sensor and applications |
| CN103964572B (en) * | 2014-05-16 | 2015-10-14 | 宜兴市产品质量监督检验所 | Biomembrane electrode and UASB coupled reactor |
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| CN106198689A (en) * | 2016-08-12 | 2016-12-07 | 中国科学院重庆绿色智能技术研究院 | A kind of device measuring coulomb Biochemical oxygen demand |
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