CN101704595A - Method for removing nitrates from water - Google Patents
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- CN101704595A CN101704595A CN200910191670A CN200910191670A CN101704595A CN 101704595 A CN101704595 A CN 101704595A CN 200910191670 A CN200910191670 A CN 200910191670A CN 200910191670 A CN200910191670 A CN 200910191670A CN 101704595 A CN101704595 A CN 101704595A
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Abstract
The invention discloses a method for removing nitrates from water, which is characterized in that: a catalytic reduction unit and an electrolysis unit cooperate; the CO2 generated at the anode of the electrolysis unit is used to adjust the pH value of inlet water; the hydrogen generated at the cathode of the electrolysis unit is used as a reductant; a water flow and the hydrogen are allowed to pass through a catalytic reduction reaction area in a mode of reverse flows; the retention time of the water flow and the hydrogen is prolonged; and the nitrates in water are reduced into nitrogen in the presence of a catalyst such as a supported metal Pd or metals Pd-Cu. The anode of the electrolysis unit is made of a graphite plate and the cathode of the electrolysis unit is made of a carbon fiber plate. The method has the advantages that: nitrate-containing raw water can be continuously treated without any additional medicaments or reagents; the process is performed automatically after power is turned on; the products of electrolysis are reasonably arranged and utilized; the related device is simple in process, optimized in structure, high in treatment efficiency and convenient in use.
Description
Technical field
The present invention relates to water technology and equipment technical field, specifically relate to a kind of method of removing nitrate in groundwater.
Background technology
In recent years,, especially synthesize developing rapidly of chemical industry, petrochemical complex, agricultural chemicals and agrochemical industry along with the development of industrial and agricultural production, and a large amount of dischargings of trade effluent and municipal effluent, increasing nitrate pollutants enters body of groundwater.As lake, river and the reservoir of urban water resource, its pollution of waterhead phenomenon is serious day by day, and the drinking water safety problem that nitrate causes in the water has become one of principal element that threatens human health.Nitrate is deleterious to the Mammals organism, and nitrate is converted into ammonium in vivo, and an intermediate steps of its process is that nitrate is converted into nitrite.Nitrite may cause the congenital heart defect syndromes of baby, also is the precursor of carinogenicity aminated compounds.Therefore, the technology of nitrate has become the important topic that those skilled in the art study in the removal water body.
At present, the method for nitrate mainly contains in the removal water: physics method, biological denitrificaion method and chemical reduction method.The physics method is removed the nitrate in the underground water, and required expense is higher, and the transfer of nitrate pollutants just takes place or concentrates, and in fact it is not removed up hill and dale.Though the biological denitrificaion method can thoroughly be reduced into nitrogen with nitrate, capacity of resisting impact load is low, has secondary pollution, and complex process, is not suitable for small-scale and dispersion to problems such as water treatments.Chemical reduction method comprises metal simple-substance reduction method, hydrogen catalysis reduction method and electrochemical reducing, the metal simple-substance reduction method is to be that reductive agent is a nitrogen with nitrate reduction with metal simple-substances such as iron, aluminium, zinc, its reaction conditions is difficult to control, easily produces by product and causes secondary pollution; The hydrogen catalysis reduction method is to be reductive agent with hydrogen, under catalyst action nitrate is reduced, and its speed of response is fast, can avoid the secondary pollution to water, but the solubleness of hydrogen in water is low, and inflammable and explosive, and inconvenience is arranged when using.Electrochemical reducing is a kind of method of denitration that recently just develops, and is reductive agent with the electronics, need not add catalyzer, but be in theoretical research stage so far.
CN03178365.1 " a kind of method and apparatus of removing nitrate in the water ", announced that a kind of is reductive agent with hydrogen, in containing nitric acid salt solution, add load type bimetal catalyst, under the airtight anoxia condition, continuously feed hydrogen and make that nitrate thoroughly is reduced into nitrogen in the water.Wherein, the H that is adopted
2With the acidity adjustment material all be in addition, and be intermittent operation.When being used for experimental study, have flexibly, convenient, to advantages such as the adaptability of research approach are strong.But, be not suitable for continuous processing to drinking water, should not be used for water factory's production operation; Simultaneously, H
2With the acidity adjustment medicine and reagent carry and add to open-air, domestic applications is incompatible, and catalyzer suspends in water, treating water at last also must with could use after catalyzer separates.
CN200410098590.2 " metal modified active carbon fiber electrode and remove the method for nitrate with this electrode ", announced a kind of a kind of and a kind of base metal in precious metal such as palladium, platinum, gold, rhodium, the ruthenium such as copper, tin, indium, zinc, silver particles modified active carbon fiber of utilizing, make the electrode of nitrate in the reducible water, this electrode is a negative electrode, inactive, conductive material such as graphite, plumbous oxide is an anode, separate with proton exchange membrane between the anode and cathode, under the situation of energising, nitrate reduction.Negative electrode is the place that the nitrate catalytic reduction reaction takes place in this invention, because the Ka band negative electricity, can produce the effect of electrically repelling each other with same electronegative nitrate ion, and nitrate radical adheres on the cathod catalyst surface like this, so with negative electrode on the H of electrolysis generation
2The chance that catalytic reduction reaction takes place is just comparatively limited, so the effect of reaction efficiency, removal nitrate radical all is difficult to improve.
Summary of the invention
At the prior art above shortcomings, the purpose of this invention is to provide a kind of processing efficiency height, easy control of reaction conditions can not produce secondary pollution, and can handle the method for nitrate in the removal water that contains the former water of nitrate continuously, the water supply that especially is suitable for actual tap water is handled.
The object of the present invention is achieved like this: a kind of method of removing nitrate in the water, it is characterized in that, utilize catalytic reduction reaction unit and electrolytic reaction unit collaborative, the electrolytic reaction unit is set below the catalytic reduction reaction unit, pass through the unitary current of catalytic reduction reaction and down up pass through the catalytic reduction reaction district in the mode of adverse current with the hydrogen that the electrolytic reaction unit produces, making the nitrate reduction in the former water is that nitrogen is removed, and produces CO with the electrolysis cells anode
2Regulate the pH value of former water water inlet, make former water water inlet be in sour environment; Producing hydrogen with the electrolysis cells negative electrode is reductive agent, under the effect of catalyzer, makes that nitrate reduction is a nitrogen in the water, and its reaction equation is:
2NO
3 -+5H
2+2H
+＝N
2+6H
2O。
The catalyzer of catalytic reduction reaction unit configuration adopts the monometallic or the multimetallic catalyst of carried noble metal, transition metal, as the catalyzer of load P d or Pd-Cu.As further optimization, support of the catalyst adopts the high-specific surface area material, makes the catalyst reduction reaction unit of unit weight, unit volume can the more amount of metal of load, opens more nitrate generation catalytic reduction reaction thereby lure.
The electrolytic reaction unit adopts the same diaphragm electrolysis of bath composition, by barrier film, with catholyte gaseous product H
2, anode electrolysis gaseous product CO
2Separately, to collect respectively; Anode adopts graphite cake, and negative electrode adopts carbon fiber board; The graphite anode reaction is mainly: C+H
2O-4e=CO
2+ 4H
+(e
0=0.207V), because of its standard electric limit position than electrode reaction H
2O-2e=1/2O
2+ 2H
+(e
0=1.229V) much lower, more the electropotential that reacts on anode than oxygen acid radical ion is much lower, so the main CO that generates of anode electrode reaction
2Negative electrode adopts the hydrogen overvoltage of Pt, graphite, carbon fiber etc. very low, and cathodic reaction mainly generates H
2, electrolytic reaction is mainly: 2H
++ 2e=H
2
Current and hydrogen are with the mode process catalytic reduction reaction district of adverse current, and current, hydrogen prolonged in the residence time of catalyst filling layer, made NO
3 -, hydrogen strengthened to the mass transfer of catalyst surface, there is more NO the unit time simultaneously
3 -, H
2Contact with catalyzer.
Anode electrolysis product carbonic acid gas causes water inlet place of former water after collecting, by the multilayer lateral partitions be adverse current with Yuan Shui, baffling contacts mixing; Lateral partitions one end alternately is communicated with up and down.
Compared to existing technology, the present invention has following beneficial effect:
1, the present invention adopts electrochemical method reduction nitrate, need not add any medicament, can avoid going out the water generates secondary pollution.Utilize catalytic reduction unit and electrolysis cells collaborative, produce CO with the electrolysis cells anode
2Regulate the pH value of water inlet, producing hydrogen with the electrolysis cells negative electrode is reductive agent, make current and hydrogen mode process catalytic reduction reaction district with adverse current, increase current and hydrogen the residence time in the catalytic reduction reaction district, under the effect of catalyzer such as loaded metal Pd or Pd-Cu, make that nitrate is reduced to nitrogen in the water.
2, the inventive method can be handled continuously to the former water that contains nitrate, do not need in addition the hydrogen source hydrogen supply, need not add medicine and reagent carry out acidity adjustment, easy to operate, connect the power supply last handling process and carry out automatically, electrolysate is rationally arranged to utilize the processing efficiency height.
3, simple, the constitution optimization of related apparatus structure, the processing efficiency height, easy to use.
Description of drawings
Fig. 1 is a structural representation of implementing a kind of concrete facilities and equipments of the present invention.
Fig. 2 is a water inlet configuration carbonic acid gas acidity adjustment cell structure enlarged diagram among Fig. 1;
Fig. 3 is the left view of Fig. 1 device;
Fig. 4 is the A-A sectional view of Fig. 1.
Embodiment
The present invention is described in further detail below in conjunction with the drawings and specific embodiments.
The inventive method is the catalytic reduction reaction principle based on nitrate, during enforcement, the catalyzer of catalyst reduction reaction unit configuration adopts the monometallic or the multimetallic catalyst of carried noble metal, transition metal, as the various catalyzer of load P d or Pd-Cu.Described catalyzer is placed in the accommodating body, and the bottom is provided with the diaphragm electrolysis reaction zone, by the electrolytic anode product C O that collects
2Former water water inlet is adjusted to sour environment, makes it flow into the catalytic reduction reaction district, from the H of below electrolysis cathode from catalyzer top uniform distribution
2Rising enters the catalytic reduction reaction district, is counter-current flow with pending water in the catalytic reduction reaction district, and nitrate is under catalyst action, by H in the pending water
2Reduction generates the nitrogen G﹠W, thereby is able to remove from water.Pending water and H
2The district is counter-current flow at catalytic reduction reaction, has increased water and H
2In the duration of contact in catalytic reduction reaction district, make the unit time that more NO be arranged
3 -, H
2Contact with catalyzer, improved reaction efficiency greatly, strengthened treatment effect.
Further, the electrolytic reaction district adopts graphite anode and charcoal fiberboard negative electrode.Like this, present method removes that nitrate has a style of one's own in the water, need not in addition the hydrogen source hydrogen supply, need not in addition that medicine and reagent carries out acidity adjustment, have implement convenient, efficient is high, save hydrogen source and medicine carries and advantage such as transportation cost.
When present method is specifically implemented, can adopt as described in Figure 1 device to implement, as shown in Figures 1 to 4, this apparatus structure is: comprise reactor accommodating body 1, wherein, described accommodating body 1 top is catalytic reduction reaction district 2, and the bottom is an electrolysis zone 3, separate by gas distributing chamber 4 between described catalytic reduction reaction district 2 and the electrolysis zone 3, the gas distributing chamber top board is an air distribution plate 5; Produce hydrogen with electrolysis zone and make the requirement that nitrate ion is reduced at catalyst surface, electrolysis zone generation carbonic acid gas is used to regulate water inlet acidity adaptation catalytic reduction reaction as reductive agent; Hydrogen enters catalytic reduction reaction district 2 by the flowing hole 6 of uniform setting on the air distribution plate 5 in the gas distributing chamber 4, and hydrogen and current can pass through from flowing hole 6; 2 dispose catalyzer in the described catalytic reduction reaction district; Former water by behind the carbonic acid gas acidity adjustment chamber 8, enters catalytic reduction reaction district 2 by the accommodating body sidewall overflow above the catalyzer from water inlet pipe 7; The accommodating body top is provided with venting port 9; Some negative electrodes 10, anode 11 are staggeredly arranged in parallel in the described electrolysis zone 3, adopt electrolytic film 12 to be divided into positive column, cathodic area between each group negative electrode 10 and the anode 11, the electrolytic film hole allows water and ion to pass through, and the gas that negative electrode 10, anode 11 are produced separates; Anode 11 adopts graphite, and the top, positive column is provided with and links to each other with carbon dioxide collection tube 14 communicating pipe 13, and carbon dioxide collection tube 14 is connected to former water water inlet acidity adjustment chamber 8, contacts after vertical dividing plate 15 upper spaces are discharged by venting port 9 with former water; Negative electrode 10 adopts carbon fiber board, and top, cathodic area dividing plate is provided with flowing hole 16 hydrogen supply G﹠W streams to be passed through.Negative electrode 10, anode 11 by lead respectively with direct supply 17-utmost point ,+extremely link to each other.Rising pipe 18 is positioned at electrolysis zone 3 belows.Wherein said carbonic acid gas acidity adjustment chamber 8, as shown in Figure 2, described carbonic acid gas is with before former water water inlet 5 contacts, on 8 water levels of carbonic acid gas acidity adjustment chamber, described carbon dioxide collection tube 14 extends from top to bottom by the inverted u-shaped pipe, and 8 bottoms, carbonic acid gas acidity adjustment chamber are located in the air outlet; Alternately be horizontally arranged with some plane clapboards 19 in the carbonic acid gas acidity adjustment chamber 8, current, carbonic acid gas adverse current, baffling contact in acidity adjustment chamber 8 are passed through, so both avoided former water water inlet directly to flow to bottom electrolysis zone 3 along carbon dioxide collection tube 14, can realize that again carbonic acid gas fully contacts with water, strengthen the acidity adjustment of carbonic acid gas water inlet.Also tiling has the permeable pad 20 of palm fiber pad above the catalyzer in described reduction reaction district 2, and it is even as far as possible to make water enter the water distribution in catalytic reduction reaction district 2, and avoiding into, water directly washes away catalyst filling.
Below based on above-mentioned device for carrying out said, enumerate the treatment effect that experiment embodiment removes nitrate in the water to this method and be described further.
Example 1: device accommodating body volume is 30L, wherein, and the γ-Al of supported palladium-copper bi-metal in the catalytic reduction reaction district
2O
3Catalyst particle size 1.0-3.5mm, BET specific surface area 238m
2/ g, Pd 5.1wt%, Cu 1.8wt%,, volume 15L, electrolysis zone volume 15L (containing the electrode volume) handles former water and is prepared by saltpetre, concentration 30mg/L, condition is as follows:
Electrode: anode: graphite electrode plate 350*180*40,5
Negative electrode: carbon fiber board 350*180*5,6
Interelectrode distance: 2mm
Strength of current: 1.0mA
Voltage: 2.0V
Temperature: 20-25 ℃
Flow: 20L/h
Handling back water quality is:
NO
2 -Less than 0.003mg/L, NO
3 -0.05mg/L, clearance 99.8%.
Example 2: device accommodating body volume is 30L, wherein, and the γ-Al of supported palladium-copper bi-metal in the catalytic reduction reaction district
2O
3Catalyst particle size 1.0-3.5mm, BET specific surface area 238m
2/ g, Pd 5.1wt%, Cu 1.8wt%,, volume 15L, electrolysis zone volume 15L (containing the electrode volume) handles former water and is prepared by saltpetre, concentration 50mg/L, condition is as follows:
Electrode: anode: graphite electrode plate 350*180*40,5
Negative electrode: carbon fiber board 350*180*5,6
Interelectrode distance: 2mm
Strength of current: 1.0mA
Voltage: 2.0V
Temperature: 20-25 ℃
Flow: 20L/h
Handling back water quality is:
NO
2 -Less than 0.01mg/L, NO
3 -0.12mg/L, clearance 99.8%.
Prove that through above-mentioned example present method can be removed nitrate in the water efficiently, practical function is very good.
Explanation is at last, above embodiment is only unrestricted in order to technical scheme of the present invention to be described, although the present invention is had been described in detail with reference to preferred embodiment, those of ordinary skill in the art is to be understood that, can make amendment or be equal to replacement technical scheme of the present invention, and not breaking away from the aim and the scope of technical solution of the present invention, it all should be encompassed in the middle of the claim scope of the present invention.
Claims (4)
1. method of removing nitrate in the water, it is characterized in that, adopt catalytic reduction reaction unit and electrolytic reaction unit synergy, pass through the unitary current of catalytic reduction reaction and down up pass through the catalytic reduction reaction district in the mode of adverse current with the hydrogen that the electrolytic reaction unit produces, making the nitrate reduction in the former water is that nitrogen is removed;
Described catalytic reduction reaction unit is arranged at the unitary top of electrolytic reaction; Produce CO with electrolytic reaction unit anode
2Regulate the pH value of former water water inlet, make former water water inlet be in sour environment; Producing hydrogen with the electrolysis cells negative electrode is reductive agent.
2. remove the method for nitrate in the water according to claim 1, it is characterized in that, the catalyzer of described catalytic reduction reaction unit configuration adopts the monometallic or the multimetallic catalyst of carried noble metal, transition metal; Be load P d or Pd-Cu catalyzer.
3. remove the method for nitrate in the water according to claim 1, it is characterized in that, described electrolytic reaction unit adopts the same diaphragm electrolysis of bath composition, with dipolar gas electrolysate H
2, CO
2Separately, to collect respectively; Anode adopts graphite cake, and negative electrode adopts carbon fiber board.
4. remove the method for nitrate in the water according to claim 1, it is characterized in that, described electrolytic reaction unit anode produces CO
2With former water by the multilayer lateral partitions be adverse current, baffling contacts mixing.
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|---|---|---|---|
| CN2009101916705A CN101704595B (en) | 2009-11-30 | 2009-11-30 | Method for removing nitrates from water |
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|---|---|---|---|
| CN2009101916705A CN101704595B (en) | 2009-11-30 | 2009-11-30 | Method for removing nitrates from water |
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| CN101704595B CN101704595B (en) | 2011-07-27 |
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| CN106006863A (en) * | 2016-05-15 | 2016-10-12 | 宜兴市凌泰环保设备有限公司 | Efficient self-control vertical type fixed-electrode electro-catalysis decontamination device |
| CN108408875A (en) * | 2018-04-17 | 2018-08-17 | 江苏达格水务有限公司 | A kind of superpower oxidation reflection device of water process ozone contact |
| CN109704505A (en) * | 2019-01-17 | 2019-05-03 | 大渊环境技术（厦门）有限公司 | A kind of plasma effluent purification method |
| CN110040903A (en) * | 2019-01-17 | 2019-07-23 | 大渊环境技术（厦门）有限公司 | A kind of deep purification of waste water device |
| CN110183009A (en) * | 2019-04-23 | 2019-08-30 | 皓禹(厦门)环保有限公司 | The regeneration device and its method of municipal sewage plant discharge water |
| CN111606495A (en) * | 2020-04-20 | 2020-09-01 | 西安建筑科技大学 | Two-stage catalytic denitrification device and method for removing nitrate in water |
| CN112429844A (en) * | 2020-10-23 | 2021-03-02 | 同济大学 | Method and system for deep denitrification of sewage |
| CN112591856A (en) * | 2020-12-04 | 2021-04-02 | 北京师范大学 | Electrocatalytic activity regulation and control method based on inert ion intercalation |
| CN114011251A (en) * | 2021-12-22 | 2022-02-08 | 南京水滴智能环保装备研究院有限公司 | Conductive film for efficiently removing nitrate in water and preparation method thereof |
| CN114380361A (en) * | 2021-12-10 | 2022-04-22 | 中国科学院生态环境研究中心 | Method for recovering uranium from uranium-containing wastewater and underground water through electrochemical reduction and enrichment in coexistence of nitrates |
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- 2009-11-30 CN CN2009101916705A patent/CN101704595B/en not_active Expired - Fee Related
Cited By (13)
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| CN106006863A (en) * | 2016-05-15 | 2016-10-12 | 宜兴市凌泰环保设备有限公司 | Efficient self-control vertical type fixed-electrode electro-catalysis decontamination device |
| CN108408875A (en) * | 2018-04-17 | 2018-08-17 | 江苏达格水务有限公司 | A kind of superpower oxidation reflection device of water process ozone contact |
| CN109704505A (en) * | 2019-01-17 | 2019-05-03 | 大渊环境技术（厦门）有限公司 | A kind of plasma effluent purification method |
| CN110040903A (en) * | 2019-01-17 | 2019-07-23 | 大渊环境技术（厦门）有限公司 | A kind of deep purification of waste water device |
| CN110183009A (en) * | 2019-04-23 | 2019-08-30 | 皓禹(厦门)环保有限公司 | The regeneration device and its method of municipal sewage plant discharge water |
| CN111606495A (en) * | 2020-04-20 | 2020-09-01 | 西安建筑科技大学 | Two-stage catalytic denitrification device and method for removing nitrate in water |
| CN112429844A (en) * | 2020-10-23 | 2021-03-02 | 同济大学 | Method and system for deep denitrification of sewage |
| CN112591856A (en) * | 2020-12-04 | 2021-04-02 | 北京师范大学 | Electrocatalytic activity regulation and control method based on inert ion intercalation |
| CN112591856B (en) * | 2020-12-04 | 2021-12-14 | 北京师范大学 | Electrocatalytic activity regulation and control method based on inert ion intercalation |
| CN114380361A (en) * | 2021-12-10 | 2022-04-22 | 中国科学院生态环境研究中心 | Method for recovering uranium from uranium-containing wastewater and underground water through electrochemical reduction and enrichment in coexistence of nitrates |
| CN114380361B (en) * | 2021-12-10 | 2023-06-30 | 中国科学院生态环境研究中心 | Method for recycling uranium in uranium-containing wastewater and groundwater through electrochemical reduction enrichment in coexistence of nitrate |
| CN114011251A (en) * | 2021-12-22 | 2022-02-08 | 南京水滴智能环保装备研究院有限公司 | Conductive film for efficiently removing nitrate in water and preparation method thereof |
| CN114011251B (en) * | 2021-12-22 | 2024-01-23 | 南京水滴智能环保装备研究院有限公司 | Conductive film for efficiently removing nitrate in water and preparation method thereof |
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Assignee: Guangxi Bamalilang Beverage Co., Ltd. Assignor: Chongqing University Contract record no.: 2012450000051 Denomination of invention: Method for removing nitrates from water Granted publication date: 20110727 License type: Exclusive License Open date: 20100512 Record date: 20120704 |
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