TWI754986B - Method and system for processing ammoniacal nitrogen waste solution - Google Patents

Method and system for processing ammoniacal nitrogen waste solution Download PDF

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TWI754986B
TWI754986B TW109122937A TW109122937A TWI754986B TW I754986 B TWI754986 B TW I754986B TW 109122937 A TW109122937 A TW 109122937A TW 109122937 A TW109122937 A TW 109122937A TW I754986 B TWI754986 B TW I754986B
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ammonia nitrogen
nitrogen wastewater
ammonia
electrolyte
absorption tower
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TW202202445A (en
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曾堯宣
郭維庭
黃文慶
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環創源科技股份有限公司
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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
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/20—Treatment of water, waste water, or sewage by degassing, i.e. liberation of dissolved gases
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B21/00—Nitrogen; Compounds thereof
    • C01B21/02—Preparation of nitrogen
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
    • C01B3/047—Decomposition of ammonia
    • 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
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

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Abstract

A method and a system for processing ammoniacal nitrogen waste solution are provided. The method includes: providing an ammoniacal nitrogen waste solution; performing an ammonia extraction process, to extract gaseous ammonia from the ammoniacal nitrogen waste solution; transforming the gaseous ammonia into ammonium ion; performing an electrolysis reaction by using sodium chloride solution as an electrolyte, to produce a solution containing hypochlorous acid; and mixing the ammonium ion with the solution containing hypochlorous acid, to transform the ammonium ion into nitrogen gas.

Description

氨氮廢水的處理方法及處理系統Ammonia nitrogen wastewater treatment method and treatment system

本發明是有關於一種廢水的處理方法及處理系統，且特別是有關於一種氨氮廢水的處理方法及處理系統。The present invention relates to a treatment method and treatment system of waste water, and in particular, to a treatment method and treatment system of ammonia nitrogen waste water.

氮以分子態的氮、有機氮、氨氮（ammoniacal nitrogen）、硝態氮、亞硝態氮、硫氰化物及氰化物等形式存在於廢水中。特別來說，氨氮是指水中以游離氨（NH 3）和銨離子（NH 4 +）形式存在的氮。含有氨氮的廢水（亦稱為氨氮廢水）為一種普遍的工業廢水。若將氨氮廢水直接排入河川或湖泊，將引起因藻類及微生物大量繁殖而造成的優氧化問題。另一方面，若氨氮存在於飲用水中，則可能對人體造成致癌的風險。因此，如何將氨氮廢水中的氨氮轉化為對生態系統無害的產物成為本領域中的重要課題之一。 Nitrogen exists in wastewater in the form of molecular nitrogen, organic nitrogen, ammoniacal nitrogen, nitrate nitrogen, nitrous nitrogen, thiocyanide and cyanide. In particular, ammonia nitrogen refers to nitrogen present in water in the form of free ammonia (NH 3 ) and ammonium ions (NH 4 + ). Ammonia nitrogen-containing wastewater (also known as ammonia nitrogen wastewater) is a common industrial wastewater. If ammonia nitrogen wastewater is directly discharged into rivers or lakes, it will cause optimal oxidation problems caused by the proliferation of algae and microorganisms. On the other hand, ammonia nitrogen may pose a carcinogenic risk to humans if present in drinking water. Therefore, how to convert ammonia nitrogen in ammonia nitrogen wastewater into products that are harmless to the ecosystem has become one of the important topics in this field.

本揭露提供一種氨氮廢水的處理方法及處理系統，可有效地將氨氮轉化為對環境與人體無害的氮氣。The present disclosure provides a treatment method and treatment system for ammonia nitrogen wastewater, which can effectively convert ammonia nitrogen into nitrogen that is harmless to the environment and human body.

本揭露的其中一態樣提供一種氨氮廢水的處理方法，包括：提供氨氮廢水；對所述氨氮廢水進行脫氨處理，以將所述氨氮廢水中的氨氮轉化為氣態氨；將所述氣態氨轉化為離子銨；以氯化鈉水溶液作為電解液而進行電解反應，以產生含有次氯酸的溶液；以及混合所述離子銨與所述含有次氯酸的溶液，以將所述離子銨降解為氮氣。One aspect of the present disclosure provides a method for treating ammonia nitrogen wastewater, including: providing ammonia nitrogen wastewater; performing deamination treatment on the ammonia nitrogen wastewater to convert the ammonia nitrogen in the ammonia nitrogen wastewater into gaseous ammonia; converting into ionic ammonium; performing an electrolytic reaction with an aqueous sodium chloride solution as an electrolyte to produce a solution containing hypochlorous acid; and mixing the ionic ammonium and the hypochlorous acid-containing solution to degrade the ionic ammonium for nitrogen.

在一些實施例中，藉由超重力吹脫設備進行所述脫氨處理。In some embodiments, the deamination process is carried out by a supergravity stripping device.

在一些實施例中，在進行所述脫氨處理前更包括將鹼液加入所述氨氮廢水。In some embodiments, before the deamination treatment is performed, adding alkali liquor to the ammonia nitrogen wastewater is further included.

在一些實施例中，將所述氣態氨轉化為所述離子銨的方法包括使所述氣態氨在吸收塔內水解於所述電解液中。In some embodiments, the method of converting the gaseous ammonia to the ionic ammonium includes hydrolyzing the gaseous ammonia in the electrolyte within an absorption tower.

在一些實施例中，所述電解液的pH值高於或等於預設pH值時啟動所述電解反應，且所述電解液的所述pH值低於所述預設pH值時中斷所述電解反應。In some embodiments, the electrolysis reaction is started when the pH value of the electrolyte is higher than or equal to a preset pH value, and the electrolysis reaction is interrupted when the pH value of the electrolyte solution is lower than the preset pH value electrolytic reaction.

在一些實施例中，所述電解反應產生氫氣，且所述氨氮廢水的處理方法更包括將所述氫氣輸入至燃料電池。In some embodiments, the electrolysis reaction produces hydrogen, and the method for treating the ammonia nitrogen wastewater further includes inputting the hydrogen into a fuel cell.

本揭露的另一態樣提供一種氨氮廢水處理系統，包括：脫氨設備，經配置以接收氨氮廢水，並將所述氨氮廢水中的氨氮轉化為氣態氨；吸收塔，經配置以接收所述氣態氨，且將所述氣態氨轉化為離子銨；電解槽，經配置以電解作為電解液的氯化鈉水溶液，以形成含有次氯酸的溶液；以及反應槽，連通於所述電解槽與所述吸收塔，且經配置以使所述離子銨與所述含有次氯酸的溶液反應，而使所述離子銨降解為氮氣。Another aspect of the present disclosure provides an ammonia nitrogen wastewater treatment system, including: a deamination device configured to receive ammonia nitrogen wastewater and convert ammonia nitrogen in the ammonia nitrogen wastewater into gaseous ammonia; an absorption tower configured to receive the ammonia nitrogen wastewater gaseous ammonia, and converting the gaseous ammonia into ionic ammonium; an electrolytic cell configured to electrolyze an aqueous sodium chloride solution as an electrolyte to form a hypochlorous acid-containing solution; and a reaction cell in communication with the electrolytic cell and The absorption tower is configured to react the ionic ammonium with the hypochlorous acid-containing solution to degrade the ionic ammonium to nitrogen gas.

在一些實施例中，氨氮廢水處理系統更包括加藥器，經配置以將鹼液加入至所述氨氮廢水。In some embodiments, the ammonia nitrogen wastewater treatment system further includes a dosing device configured to add lye to the ammonia nitrogen wastewater.

在一些實施例中，所述脫氨設備為超重力吹脫設備。In some embodiments, the deamination device is a supergravity stripping device.

在一些實施例中，所述吸收塔連通於所述電解槽，所述電解槽中的所述電解液部分地回流至所述吸收塔，且所述氣態氨在所述吸收塔內水解於所述電解液中，以轉化為所述離子銨。In some embodiments, the absorption tower is in communication with the electrolysis cell, the electrolyte in the electrolysis cell is partially refluxed to the absorption tower, and the gaseous ammonia is hydrolyzed in the absorption tower in the absorption tower. in the electrolyte to be converted into the ionic ammonium.

在一些實施例中，氨氮廢水處理系統更包括：曝氣筒，連通於所述電解槽與所述反應槽之間，且經配置以對於所述電解反應的生成物進行氣液分離，其中所述反應槽接收所述曝氣筒所分離出的液體。In some embodiments, the ammonia nitrogen wastewater treatment system further includes: an aeration cylinder, which is communicated between the electrolysis tank and the reaction tank, and is configured to perform gas-liquid separation on the products of the electrolysis reaction, wherein the The reaction tank receives the liquid separated by the aeration cylinder.

在一些實施例中，氨氮廢水處理系統更包括：燃料電池，經配置以接收所述電解反應所生成的氫氣，且以所述氫氣作為燃料而產生電能。In some embodiments, the ammonia nitrogen wastewater treatment system further includes: a fuel cell configured to receive the hydrogen gas generated by the electrolysis reaction, and use the hydrogen gas as a fuel to generate electricity.

基於上述，本揭露所提供的氨氮廢水處理方法及處理系統藉由脫氨處理、電解反應與離子銨的降解反應而將危害環境與人體的氨氮轉化為無毒的氮氣。相較於將氨氮轉化為硫酸銨的其他處理方法，本揭露的氨氮廢水處理方法所得到的主要產物（亦即氮氣）可不必再進行其他處理。在一些實施例中，更可利用電解反應所產生的氫氣作為燃料電池的燃料，而產生電能。此外，在一些實施例中，採用超重力吹脫設備進行脫氨處理。相較於以氣提塔進行脫氨處理，超重力吹脫設備的脫氨效率更佳，且佔地面積更小。Based on the above, the ammonia nitrogen wastewater treatment method and treatment system provided by the present disclosure converts ammonia nitrogen that is harmful to the environment and human body into non-toxic nitrogen gas through deamination treatment, electrolysis reaction and degradation reaction of ionic ammonium. Compared with other treatment methods for converting ammonia nitrogen into ammonium sulfate, the main product (ie, nitrogen gas) obtained by the ammonia nitrogen wastewater treatment method of the present disclosure does not need to be subjected to other treatment. In some embodiments, the hydrogen gas generated by the electrolysis reaction can be used as the fuel of the fuel cell to generate electricity. Additionally, in some embodiments, the deamination process is performed using a supergravity stripping device. Compared with the deamination treatment with the stripper, the deamination efficiency of the supergravity stripping equipment is better, and the area is smaller.

圖1是依照本揭露一些實施例的氨氮廢水的處理方法的流程圖。圖2是依照本揭露一些實施例的氨氮廢水處理系統10的示意圖。以下將依據本揭露的一些實施例而以圖2的氨氮廢水處理系統10來實施氨氮廢水的處理方法。FIG. 1 is a flowchart of a method for treating ammonia nitrogen wastewater according to some embodiments of the present disclosure. FIG. 2 is a schematic diagram of an ammonia nitrogen wastewater treatment system 10 according to some embodiments of the present disclosure. Hereinafter, according to some embodiments of the present disclosure, the ammonia nitrogen wastewater treatment system 10 of FIG. 2 will be used to implement the ammonia nitrogen wastewater treatment method.

請參照圖1與圖2，進行步驟S100，以提供氨氮廢水。氨氮廢水中含有以游離氨（NH 3）以及離子銨（NH 4 +）形式存在的氮。在一些實施例中，氨氮廢水可來自於（但不限於）晶圓及半導體製造業、印刷電路板製造業、石化產業、化工產業等。此外，如圖2所示，氨氮廢水可預先存放於進料槽100中。 Referring to FIG. 1 and FIG. 2 , step S100 is performed to provide ammonia nitrogen wastewater. Ammonia nitrogen wastewater contains nitrogen in the form of free ammonia (NH 3 ) and ionic ammonium (NH 4 + ). In some embodiments, the ammonia nitrogen wastewater may come from (but not limited to) wafer and semiconductor manufacturing, printed circuit board manufacturing, petrochemical industry, chemical industry, and the like. In addition, as shown in FIG. 2 , the ammonia nitrogen wastewater can be stored in the feeding tank 100 in advance.

在步驟S102處，對氨氮廢水進行脫氨處理。在脫氨處理期間，將氨氮廢水中的離子銨轉變為游離氨，且藉由氣體吹脫而使溶液中的游離氨穿過氣液介面而形成氣態氨（或稱氨氣）。藉由脫氨處理，可將氨氮廢水中的含氮物質以氣態氨的形式萃取出。氨氮廢水中的其他物質可隨剩餘的溶液排出，或循環處理。如此一來，可避免氨氮廢水中的其他雜質進入氨氮廢水處理系統10的其他部分，而對此些部分造成腐蝕等問題。游離氨與離子銨可如式（1）所示而平衡地存在於氨氮廢水中。

Figure 02_image001
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Figure 02_image003
Figure 02_image005
Figure 02_image007
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Figure 02_image009
（1） 由示（1）可知，將氨氮廢水的pH值提高（亦即提高氫氧離子的濃度），可破壞平衡而迫使離子銨轉變為游離氨。在一些實施例中，可藉由添加鹼液至氨氮廢水中，來提高氨氮廢水的pH值。舉例而言，可調整鹼液的添加，而使氨氮廢水具有大於或等於12的pH值。此外，鹼液可例如是重量百分比為約40 %的氫氧化鈉溶液。如圖2所示，在一些實施例中，例如是氫氧化鈉溶液的鹼液可預先存放於加藥槽102中，隨後在進行脫氨處理前加入至來自於進料槽100的氨氮廢水。此外，在一些實施例中，用於進行氣體吹脫的設備（或稱為脫氨設備）可為超重力吹脫設備104。在此些實施例中，經混和的氨氮廢水與鹼液進入超重力吹脫設備104。在超重力吹脫設備104中，液體在超重力的作用下被拉伸或撕裂成微小液滴、孔隙流與液膜流。如此一來，顯著地增加氣液介面的面積，而大幅提高氣體吹脫的效率。上述的超重力意指強大的離心力。在一些實施例中，超重力吹脫設備104具有轉筒與馬達（均未繪示）。轉筒的旋轉軸周圍可具有空腔以容納上述的混合溶液，且上述空腔的周圍可填充有填料。馬達可經配置以使轉筒高速旋轉，進而產生強大的離心力（亦即超重力）。此強大的離心力可造成混合溶液如上述一般被拉伸或撕裂，且可與填料撞擊。另一方面，作為載氣的氣體（例如是空氣）可由進氣口G進入超重力吹脫設備104，而將所形成的氣態氨帶離超重力吹脫設備104。另一方面，剩餘的溶液可回流至進料槽100中而循環處理（如圖2的進料槽100與超重力吹脫設備104之間的箭號所示），或者排出氨氮廢水處理系統10。 At step S102, the ammonia nitrogen wastewater is subjected to deamination treatment. During the deamination treatment, the ionic ammonium in the ammonia nitrogen wastewater is converted into free ammonia, and the free ammonia in the solution passes through the gas-liquid interface by gas stripping to form gaseous ammonia (or ammonia). The nitrogen-containing substances in the ammonia nitrogen wastewater can be extracted in the form of gaseous ammonia through the deamination treatment. Other substances in ammonia nitrogen wastewater can be discharged with the remaining solution, or recycled. In this way, other impurities in the ammonia nitrogen wastewater can be prevented from entering other parts of the ammonia nitrogen wastewater treatment system 10 and causing problems such as corrosion to these parts. Free ammonia and ionic ammonium can exist in equilibrium in ammonia nitrogen wastewater as shown in formula (1).
Figure 02_image001
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Figure 02_image003
Figure 02_image005
Figure 02_image007
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Figure 02_image009
(1) As shown in (1), increasing the pH value of ammonia nitrogen wastewater (that is, increasing the concentration of hydroxide ions) can destroy the balance and force ionic ammonium into free ammonia. In some embodiments, the pH value of the ammonia nitrogen wastewater can be increased by adding lye to the ammonia nitrogen wastewater. For example, the addition of lye can be adjusted so that the ammonia nitrogen wastewater has a pH value greater than or equal to 12. In addition, the lye can be, for example, about 40% by weight sodium hydroxide solution. As shown in FIG. 2 , in some embodiments, lye such as sodium hydroxide solution can be stored in the dosing tank 102 in advance, and then added to the ammonia nitrogen wastewater from the feeding tank 100 before the deamination treatment. Additionally, in some embodiments, the apparatus for performing gas stripping (or referred to as a deamination apparatus) may be a hypergravity stripping apparatus 104 . In these embodiments, the mixed ammonia nitrogen wastewater and alkali liquor enter the supergravity stripping device 104 . In the supergravity stripping device 104, the liquid is stretched or torn into tiny droplets, pore flow and liquid film flow under the action of supergravity. In this way, the area of the gas-liquid interface is significantly increased, and the efficiency of gas stripping is greatly improved. The above-mentioned supergravity means a strong centrifugal force. In some embodiments, the hypergravity stripping device 104 has a drum and a motor (neither shown). A cavity may be provided around the rotating shaft of the rotating drum to accommodate the above-mentioned mixed solution, and the periphery of the above-mentioned cavity may be filled with fillers. The motor can be configured to rotate the bowl at high speed, thereby generating strong centrifugal force (ie, hypergravity). This strong centrifugal force can cause the mixed solution to be stretched or torn as described above and can collide with the filler. On the other hand, a gas (eg, air) as a carrier gas can enter the supergravity stripping device 104 through the gas inlet G, and the formed gaseous ammonia is taken out of the supergravity stripping device 104 . On the other hand, the remaining solution can be recycled into the feed tank 100 for recycling (as shown by the arrow between the feed tank 100 and the supergravity stripping device 104 in FIG. 2 ), or discharged out of the ammonia nitrogen wastewater treatment system 10 .

在步驟S104處，將脫氨處理所得到的氣態氨轉變為離子銨。在一些實施例中，可將脫氨處理所得到的氣態氨水解，而形成離子銨與氫氧離子。此處所使用的水溶液可為隨後將進行的電解反應所使用的電解液，例如是氯化鈉水溶液。在一些實施例中，如圖2所示，氣態氨在吸收塔106中水解而形成離子銨。另一方面，載氣可經由連接於吸收塔106的排氣管108而排出。此外，在一些實施例中，可在排氣管108的路徑上設置抽氣設備110，以利於氣體的排放。如將參照步驟S106所描述，電解反應所使用的電解液（氯化鈉水溶液）可回流至吸收塔106中，而用於溶解氣態氨。此外，隨著電解反應與隨後的降解反應的進行，電解液的pH值可逐漸下降。舉例而言，電解液的pH值可由8.9以上逐漸下降至8.9以下。如式（1）所示，pH值降低（亦即氫氧離子濃度降低）時可使平衡往反應物方向移動，而確保溶於水溶液中的游離氨轉變為離子銨。另一方面，隨著離子銨的形成，水溶液的pH值可逐漸上升。在一些實施例中，吸收塔106內的電解液之pH值可控制在預設值（例如是8.9）以下。At step S104, the gaseous ammonia obtained by the deamination treatment is converted into ionic ammonium. In some embodiments, gaseous ammonia resulting from the deamination process can be hydrolyzed to form ionic ammonium and hydroxide ions. The aqueous solution used here may be an electrolytic solution used in an electrolysis reaction to be performed later, for example, an aqueous sodium chloride solution. In some embodiments, as shown in Figure 2, gaseous ammonia is hydrolyzed in absorber 106 to form ionic ammonium. On the other hand, the carrier gas can be exhausted through the exhaust pipe 108 connected to the absorption tower 106 . In addition, in some embodiments, a suction device 110 may be provided on the path of the exhaust pipe 108 to facilitate the discharge of gas. As will be described with reference to step S106, the electrolyte (aqueous sodium chloride solution) used in the electrolysis reaction may be returned to the absorption tower 106 for dissolving gaseous ammonia. In addition, as the electrolysis reaction and subsequent degradation reactions proceed, the pH value of the electrolyte can gradually decrease. For example, the pH value of the electrolyte can be gradually decreased from above 8.9 to below 8.9. As shown in formula (1), a decrease in pH (ie, a decrease in hydroxide ion concentration) can shift the equilibrium toward the reactant, ensuring that free ammonia dissolved in the aqueous solution is converted into ionic ammonium. On the other hand, the pH of the aqueous solution can gradually increase with the formation of ionic ammonium. In some embodiments, the pH value of the electrolyte in the absorption tower 106 can be controlled below a preset value (eg, 8.9).

在步驟S106處，進行電解反應。在一些實施例中，以氯化鈉水溶液作為電解液，而進行此電解反應。氯化鈉溶於水中形成鈉離子與氯離子。在陽極處，如式（2）所示，氯離子被氧化而形成氯分子，且伴隨產生電子。另一方面，如式（3）所示，水分子在陰極處被還原而形成氫氣與氫氧離子。

Figure 02_image011
→
Figure 02_image013
+
Figure 02_image015
（2） 6
Figure 02_image017
+
Figure 02_image015
→ 3
Figure 02_image019
+
Figure 02_image021
（3） 如式（4）所示，於陽極處所產生的氯分子可水解而形成次氯酸、氫離子與氯離子。
Figure 02_image013
+
Figure 02_image023
Figure 02_image005
Figure 02_image025
+
Figure 02_image027
+
Figure 02_image029
（4） 氯分子水解所形成的次氯酸可用於降解離子銨。如隨後所說明，在降解反應中，亦產生氫離子。綜觀電解反應與降解反應，電解液中的氫離子濃度可隨著電解反應與降解反應的進行而提高。換言之，電解液的pH值可隨著電解反應與降解反應的進行而下降。由式（4）可知，增加氫離子濃度（亦即降低電解液的pH值）不利於在電解反應期間產生將用於降解反應的次氯酸。因此，可根據電解液的pH值來判斷是否啟動電解反應。具體而言，電解液的pH值大於特定預設值（例如是pH值8.9）時再啟動電解反應，以確保次氯酸的生成。另一方面，電解液的pH值小於上述特定預設值時，則中斷電解反應。需說明的是，在步驟S104中，在將氣態氨轉變為離子銨的過程中會使水溶液（亦即電解液）的pH值上升。因此，在步驟S106中可不需額外地藉由例如是加入鹼液的方法來提高電解液的pH值。電解液的pH值自然會隨著步驟S104的進行而提高，且僅需控制在電解液的pH大於上述特定預設值時啟動電解反應。在一些實施例中，於電解槽112內進行上述的電解反應。電解槽112與吸收塔106連通，且電解槽112中的電解液可經由回流管114回流至吸收塔106，而作為水解氣態氨之用。在一些實施例中，電解槽112中的陽極可包括鍍有釕的鈦板，而電解槽112的陰極可包括經過酸洗的鈦板。 At step S106, an electrolysis reaction is performed. In some embodiments, the electrolysis reaction is carried out with an aqueous sodium chloride solution as the electrolyte. Sodium chloride dissolves in water to form sodium and chloride ions. At the anode, as shown in formula (2), chloride ions are oxidized to form chlorine molecules with accompanying electron generation. On the other hand, as shown in formula (3), water molecules are reduced at the cathode to form hydrogen gas and hydroxide ions.
Figure 02_image011
→
Figure 02_image013
+
Figure 02_image015
(2) 6
Figure 02_image017
+
Figure 02_image015
→ 3
Figure 02_image019
+
Figure 02_image021
(3) As shown in formula (4), the chlorine molecules generated at the anode can be hydrolyzed to form hypochlorous acid, hydrogen ions and chloride ions.
Figure 02_image013
+
Figure 02_image023
Figure 02_image005
Figure 02_image025
+
Figure 02_image027
+
Figure 02_image029
(4) Hypochlorous acid formed by hydrolysis of chlorine molecules can be used to degrade ionic ammonium. As will be explained later, in the degradation reaction, hydrogen ions are also generated. Looking at the electrolysis and degradation reactions, the concentration of hydrogen ions in the electrolyte can increase with the progress of the electrolysis and degradation reactions. In other words, the pH of the electrolyte can decrease as the electrolysis and degradation reactions proceed. It can be seen from formula (4) that increasing the concentration of hydrogen ions (that is, reducing the pH value of the electrolyte) is not conducive to the generation of hypochlorous acid that will be used for the degradation reaction during the electrolysis reaction. Therefore, whether to start the electrolysis reaction can be determined according to the pH value of the electrolyte. Specifically, when the pH value of the electrolyte is greater than a specific preset value (eg, pH value of 8.9), the electrolysis reaction is started to ensure the generation of hypochlorous acid. On the other hand, when the pH value of the electrolyte is lower than the above-mentioned specific preset value, the electrolysis reaction is interrupted. It should be noted that, in step S104, the pH value of the aqueous solution (that is, the electrolyte) is raised during the process of converting gaseous ammonia into ionic ammonium. Therefore, in step S106, there is no need to increase the pH of the electrolyte solution by, for example, adding alkali solution. The pH value of the electrolyte will naturally increase with the progress of step S104, and it is only necessary to control the start of the electrolysis reaction when the pH of the electrolyte is greater than the above-mentioned specific preset value. In some embodiments, the above-mentioned electrolysis reaction is performed in the electrolytic cell 112 . The electrolytic cell 112 is communicated with the absorption tower 106 , and the electrolyte in the electrolytic cell 112 can be returned to the absorption tower 106 via the return pipe 114 for hydrolysis of gaseous ammonia. In some embodiments, the anode in the electrolysis cell 112 may comprise a titanium plate plated with ruthenium, and the cathode of the electrolysis cell 112 may comprise an acid washed titanium plate.

在步驟S108處，進行離子銨的降解反應。如式（5）所示，步驟S104所得到的銨離子可與步驟S106所得到的次氯酸反應，而將銨離子降解為氮分子（氮氣），且產生水分子、氫離子與氯離子。

Figure 02_image031
+
Figure 02_image025
→
Figure 02_image033
+
Figure 02_image023
+
Figure 02_image035
+
Figure 02_image037
（5） 經上述降解反應後，離子銨轉變為無毒的氮氣。如此一來，氨氮廢水中將對環境與人體造成不利影響的游離氨與銨離子最終轉化為無毒的氮氣。相較於將氨氮轉化為硫酸銨的處理方法，本揭露的氨氮廢水處理方法所得到的主要產物（氮氣）可不必再進行其他處理。由式（2）至式（5）可知，降解反應所生成的氫離子以及伴隨次氯酸而生成的氫離子可多於電解反應所產生的氫氧離子，使得電解液的pH值隨著電解反應與降解反應的進行而下降。如參照步驟S106所說明，為確保用於降解反應的次氯酸的生成，可控制電解反應在電解液的pH值在大於特定預設值時再啟動。在一些實施例中，含有離子銨的電解液可由吸收塔106進入電解槽112（例如是經由加壓設備116加壓後進入電解槽112），且來自於吸收塔106與電解槽112的生成物可依序進入曝氣筒118與反應槽120。將如下參照步驟S112所說明，電解反應的產物可在曝氣筒118中進行氣液分離，而排出氣態的生成物（如式（3）所述，電解反應的氣態生成物包括氫氣）。另一方面，來自於吸收塔106與電解槽112的含有離子銨與次氯酸的溶液可經由曝氣筒118而進入反應槽120，且銨離子的降解反應可發生於反應槽120中。在一些實施例中，銨離子的降解反應更可少量地發生於電解槽112以及連通於電解槽112的曝氣筒118與吸收塔106內。在此些實施例中，儘管銨離子的降解反應可能發生於多處，但此降解反應可能仍主要地發生於反應槽120中。 At step S108, a degradation reaction of ionic ammonium is performed. As shown in formula (5), the ammonium ions obtained in step S104 can react with the hypochlorous acid obtained in step S106 to degrade the ammonium ions into nitrogen molecules (nitrogen) and generate water molecules, hydrogen ions and chloride ions.
Figure 02_image031
+
Figure 02_image025
→
Figure 02_image033
+
Figure 02_image023
+
Figure 02_image035
+
Figure 02_image037
(5) After the above degradation reaction, the ionic ammonium is converted into non-toxic nitrogen gas. In this way, the free ammonia and ammonium ions in the ammonia nitrogen wastewater that will adversely affect the environment and human body are finally converted into non-toxic nitrogen gas. Compared with the treatment method of converting ammonia nitrogen into ammonium sulfate, the main product (nitrogen) obtained by the ammonia nitrogen wastewater treatment method of the present disclosure does not need to be subjected to other treatments. From formula (2) to formula (5), it can be seen that the hydrogen ions generated by the degradation reaction and the hydrogen ions generated by the hypochlorous acid can be more than the hydroxide ions generated by the electrolysis reaction, so that the pH value of the electrolyte increases with the electrolysis. The reaction and degradation reaction progressed and decreased. As described with reference to step S106, in order to ensure the generation of hypochlorous acid for the degradation reaction, the electrolysis reaction can be controlled to restart when the pH value of the electrolyte is greater than a specific preset value. In some embodiments, the electrolyte containing ionic ammonium may enter the electrolytic cell 112 from the absorption tower 106 (eg, enter the electrolytic cell 112 after being pressurized by the pressurizing device 116 ), and the product from the absorption tower 106 and the electrolytic cell 112 It can enter the aeration cylinder 118 and the reaction tank 120 in sequence. As will be described below with reference to step S112, the product of the electrolysis reaction can be separated into gas and liquid in the aeration cylinder 118, and the gaseous product is discharged (as described in formula (3), the gaseous product of the electrolysis reaction includes hydrogen). On the other hand, the solution containing ionic ammonium and hypochlorous acid from the absorption tower 106 and the electrolytic cell 112 can enter the reaction tank 120 through the aeration cylinder 118 , and the degradation reaction of ammonium ions can take place in the reaction tank 120 . In some embodiments, the degradation reaction of ammonium ions may occur in a small amount in the electrolytic cell 112 and the aeration cylinder 118 and the absorption tower 106 in communication with the electrolytic cell 112 . In such embodiments, although the degradation reaction of ammonium ions may occur in multiple places, the degradation reaction may still mainly occur in the reaction tank 120 .

在步驟S110處，排出降解反應所生成的氣態生成物。如式（5）所示，離子銨的降解反應的氣態生成物可為氮氣。在一些實施例中，於反應槽120中進行的降解反應所生成的氮氣經由排氣管122而回流至吸收塔106，且經由連通於吸收塔106的排氣管108排出。在離子銨的降解反應也會少量地發生於電解槽112、曝氣筒118與吸收塔106的實施例中，在吸收塔106中所產生的氮氣可經由排氣管108排出。另一方面，在電解槽112中所產生的氮氣可進入曝氣筒118，而與可能產生於曝氣筒118中分離出的氣體一併回流至吸收塔106（例如是經由排氣管124的回流路徑124a而回流至吸收塔106），再由連通於吸收塔106的排氣管108排出。At step S110, gaseous products generated by the degradation reaction are discharged. As shown in formula (5), the gaseous product of the degradation reaction of ionic ammonium may be nitrogen gas. In some embodiments, the nitrogen gas generated by the degradation reaction in the reaction tank 120 is returned to the absorption tower 106 through the exhaust pipe 122 and discharged through the exhaust pipe 108 connected to the absorption tower 106 . In the embodiment in which the degradation reaction of ionic ammonium also occurs in a small amount in the electrolytic cell 112 , the aeration cylinder 118 and the absorption tower 106 , the nitrogen gas generated in the absorption tower 106 can be discharged through the exhaust pipe 108 . On the other hand, the nitrogen gas generated in the electrolytic cell 112 may enter the aeration drum 118 and be returned to the absorption tower 106 (eg, via the exhaust pipe 124) together with the gas that may be generated in the aeration drum 118 separated out. The return path 124a is returned to the absorption tower 106 ), and then discharged through the exhaust pipe 108 communicated with the absorption tower 106 .

在步驟S112處，取出電解反應的氣態生成物。如式（2）、式（3）所示，電解反應的氣態生成物可為氫氣。在一些實施例中，發生於電解槽112中的電解反應（或者是發生於電解槽112內的電解反應與發生於電解槽112及/或曝氣筒118內的降解反應）之生成物在連通於電解槽112的曝氣筒118中進行氣液分離。經分離出來的氣體可包括電解反應的氣態生成物（亦即氫氣），或可包括電解反應與降解反應兩者的氣態生成物（亦即氫氣與氮氣兩者）。此外，可藉由連通於曝氣筒118的排氣管124取出曝氣筒118所分離出的氣體。在曝氣筒118所分離出的氣體包括電解反應所生成的氫氣與降解反應所生成的氮氣的實施例中，曝氣筒118內氫氣所佔的比例可能明顯高於氮氣。換言之，在此些實施例中，曝氣筒118中氮氣的比例可能相當低。然而，曝氣筒118所分離出的氣體的各成分的比例可隨著製程條件與製程設備而改變，本揭露並不以此為限。At step S112, the gaseous product of the electrolysis reaction is taken out. As shown in formula (2) and formula (3), the gaseous product of the electrolysis reaction may be hydrogen. In some embodiments, the products of the electrolysis reaction that occurs in the electrolytic cell 112 (or the electrolytic reaction that occurs in the electrolytic cell 112 and the degradation reaction that occurs in the electrolytic cell 112 and/or the aerator 118 ) are in communication with each other. Gas-liquid separation is performed in the aeration cylinder 118 of the electrolytic cell 112 . The separated gas may include the gaseous product of the electrolysis reaction (ie, hydrogen), or may include the gaseous product of both the electrolysis reaction and the degradation reaction (ie, both hydrogen and nitrogen). In addition, the gas separated by the aeration cylinder 118 can be taken out through the exhaust pipe 124 connected to the aeration cylinder 118 . In the embodiment in which the gas separated by the aeration cylinder 118 includes hydrogen generated by the electrolysis reaction and nitrogen generated by the degradation reaction, the proportion of hydrogen in the aeration cylinder 118 may be significantly higher than that of nitrogen. In other words, in such embodiments, the proportion of nitrogen in the aeration tank 118 may be quite low. However, the ratio of each component of the gas separated by the aeration cylinder 118 can be changed with process conditions and process equipment, and the present disclosure is not limited thereto.

在步驟S114處，將電解反應的氣態生成物輸入至燃料電池126。如式（2）、式（3）所示，電解反應的氣態生成物可為氫氣。在一些實施例中，連通於曝氣筒118的排氣管124可分支為回流路徑124a與燃料電池進料路徑124b。曝氣筒118所分離出的氣體之一部分可沿著回流路徑124a而回到吸收塔106，且可經由排氣管108而被排出。此外，曝氣筒118所分離出的氣體之另一部分可沿著燃料電池進料路徑124b而輸入至燃料電池126。如上所述，曝氣筒118所分離出的氣體的實質上所有部分或大部分為氫氣。在燃料電池126的陽極處，藉由催化劑而將此輸入的氫氣氧化，而形成帶正電的氫離子與帶負電的電子。氫離子可通過燃料電池126中的電解液而到達陰極。另一方面，電子則無法通過電解液，而是經由例如是導線的導電路徑而到達陰極，且產生電流。如此一來，可產生電能。在陰極處，上述的離子、電子以及額外輸入至燃料電池126的氧氣進行反應，而生成水。在一些實施例中，藉由燃料電池126所產生的電能可至少部分地回饋至電解槽112等設備，進而降低氨氮廢水處理系統10的總能耗。At step S114 , the gaseous product of the electrolysis reaction is input to the fuel cell 126 . As shown in formula (2) and formula (3), the gaseous product of the electrolysis reaction may be hydrogen. In some embodiments, the exhaust pipe 124 communicating with the aeration cylinder 118 may branch into a return path 124a and a fuel cell feed path 124b. A portion of the gas separated by the aerator 118 may be returned to the absorption tower 106 along the return path 124a and may be discharged through the exhaust pipe 108 . Additionally, another portion of the gas separated by the aerator 118 may be input to the fuel cell 126 along the fuel cell feed path 124b. As mentioned above, substantially all or most of the gas separated by the aerator 118 is hydrogen. At the anode of the fuel cell 126, this input hydrogen gas is oxidized by a catalyst to form positively charged hydrogen ions and negatively charged electrons. Hydrogen ions can pass through the electrolyte in the fuel cell 126 to reach the cathode. Electrons, on the other hand, cannot pass through the electrolyte, but reach the cathode via a conductive path, such as a wire, and generate an electric current. In this way, electrical energy can be generated. At the cathode, the aforementioned ions, electrons, and additional oxygen input to the fuel cell 126 react to produce water. In some embodiments, the electrical energy generated by the fuel cell 126 can be at least partially fed back to the electrolysis cell 112 and other equipment, thereby reducing the total energy consumption of the ammonia nitrogen wastewater treatment system 10 .

在一些實施例中，反應槽120內的溶液更可循環利用。在此些實施例中，儘管未繪示，反應槽120內的溶液可回流至進料槽100或吸收塔106。此外，以上僅基於方便而依序介紹各步驟，此些步驟可能實際上是同步進行的。In some embodiments, the solution in the reaction tank 120 is more recyclable. In such embodiments, although not shown, the solution in the reaction tank 120 may be refluxed to the feed tank 100 or the absorption tower 106 . In addition, the above steps are described in sequence for convenience only, and these steps may actually be performed simultaneously.

綜上所述，本揭露所提供的氨氮廢水處理方法及處理系統藉由脫氨處理、電解反應與離子銨的降解反應而將危害環境與人體的氨氮轉化為無毒的氮氣。相較於將氨氮轉化為硫酸銨的其他處理方法，本揭露的氨氮廢水處理方法所得到的主要產物（亦即氮氣）可不必再進行其他處理。在一些實施例中，更可利用電解反應所產生的氫氣作為燃料電池的燃料，而產生電能。此外，在一些實施例中，採用超重力吹脫設備進行脫氨處理。相較於以氣提塔進行脫氨處理，超重力吹脫設備的脫氨效率更佳，且佔地面積更小。To sum up, the ammonia nitrogen wastewater treatment method and treatment system provided by the present disclosure convert ammonia nitrogen that is harmful to the environment and human body into non-toxic nitrogen gas through deammonia treatment, electrolysis reaction and degradation reaction of ionic ammonium. Compared with other treatment methods for converting ammonia nitrogen into ammonium sulfate, the main product (ie, nitrogen gas) obtained by the ammonia nitrogen wastewater treatment method of the present disclosure does not need to be subjected to other treatment. In some embodiments, the hydrogen gas generated by the electrolysis reaction can be used as the fuel of the fuel cell to generate electricity. Additionally, in some embodiments, the deamination process is performed using a supergravity stripping device. Compared with the deamination treatment with the stripper, the deamination efficiency of the supergravity stripping equipment is better, and the area is smaller.

10:氨氮廢水處理系統 100:進料槽 102:加藥槽 104:超重力吹脫設備 106:吸收塔 108、122、124:排氣管 110:抽氣設備 112:電解槽 114:回流管 116:加壓設備 118:曝氣筒 120:反應槽 124a:回流路徑 124b:燃料電池進料路徑 126:燃料電池 G:進氣口 S100、S102、S104、S106、S108、S110、S112、S114:步驟 10: Ammonia nitrogen wastewater treatment system 100: Feed chute 102: Dosing tank 104: Supergravity stripping equipment 106: Absorption tower 108, 122, 124: exhaust pipe 110: Extraction equipment 112: Electrolyzer 114: Return pipe 116: Pressurized equipment 118: Aerator 120: Reaction tank 124a: Return Path 124b: Fuel cell feed path 126: Fuel Cell G: Air intake S100, S102, S104, S106, S108, S110, S112, S114: Steps

圖1是依照本揭露一些實施例的氨氮廢水的處理方法的流程圖。 圖2是依照本揭露一些實施例的氨氮廢水處理系統的示意圖。 FIG. 1 is a flowchart of a method for treating ammonia nitrogen wastewater according to some embodiments of the present disclosure. 2 is a schematic diagram of an ammonia nitrogen wastewater treatment system according to some embodiments of the present disclosure.

S100、S102、S104、S106、S108、S110、S112、S114:步驟S100, S102, S104, S106, S108, S110, S112, S114: Steps

Claims (10)

一種氨氮廢水的處理方法，包括：提供氨氮廢水；對所述氨氮廢水進行脫氨處理，以將所述氨氮廢水中的氨氮轉化為氣態氨；將所述氣態氨轉化為離子銨；以氯化鈉水溶液作為電解液而進行電解反應，以產生含有次氯酸的溶液以及氫氣；混合所述離子銨與所述含有次氯酸的溶液，以將所述離子銨降解為氮氣；以及將所述氫氣輸入至燃料電池。 A method for treating ammonia nitrogen wastewater, comprising: providing ammonia nitrogen wastewater; performing deamination treatment on the ammonia nitrogen wastewater to convert the ammonia nitrogen in the ammonia nitrogen wastewater into gaseous ammonia; converting the gaseous ammonia into ionic ammonium; An aqueous sodium solution is electrolytically reacted as an electrolyte to generate a solution containing hypochlorous acid and hydrogen; the ionic ammonium is mixed with the solution containing hypochlorous acid to degrade the ionic ammonium into nitrogen gas; and the Hydrogen is input to the fuel cell. 如請求項1所述的氨氮廢水的處理方法，其中藉由超重力吹脫設備進行所述脫氨處理。 The method for treating ammonia nitrogen wastewater according to claim 1, wherein the deamination treatment is performed by means of a supergravity stripping device. 如請求項1所述的氨氮廢水的處理方法，其中在進行所述脫氨處理前更包括將鹼液加入所述氨氮廢水。 The method for treating ammonia nitrogen wastewater according to claim 1, further comprising adding lye to the ammonia nitrogen wastewater before performing the deamination treatment. 如請求項1所述的氨氮廢水的處理方法，其中將所述氣態氨轉化為所述離子銨的方法包括使所述氣態氨在吸收塔內水解於所述電解液中。 The method for treating ammonia nitrogen wastewater according to claim 1, wherein the method for converting the gaseous ammonia into the ionic ammonium comprises hydrolyzing the gaseous ammonia in the electrolyte in an absorption tower. 如請求項1所述的氨氮廢水的處理方法，其中所述電解液的pH值高於或等於預設pH值時啟動所述電解反應，且所述電解液的所述pH值低於所述預設pH值時中斷所述電解反應。 The method for treating ammonia nitrogen wastewater according to claim 1, wherein the electrolysis reaction is started when the pH value of the electrolyte solution is higher than or equal to a preset pH value, and the pH value of the electrolyte solution is lower than the pH value of the electrolyte solution. The electrolysis reaction is interrupted at a preset pH value. 一種氨氮廢水處理系統，包括： 脫氨設備，經配置以接收氨氮廢水，並將所述氨氮廢水中的氨氮轉化為氣態氨；吸收塔，經配置以接收所述氣態氨，且將所述氣態氨轉化為離子銨；電解槽，經配置以電解作為電解液的氯化鈉水溶液，以形成含有次氯酸的溶液以及氫氣；反應槽，連通於所述電解槽與所述吸收塔，且經配置以使所述離子銨與所述含有次氯酸的溶液反應，而使所述離子銨降解為氮氣；以及燃料電池，經配置以接收所述電解反應所生成的所述氫氣，且以所述氫氣作為燃料而產生電能。 An ammonia nitrogen wastewater treatment system, comprising: Ammonia removal equipment configured to receive ammonia nitrogen wastewater and convert ammonia nitrogen in the ammonia nitrogen wastewater into gaseous ammonia; an absorption tower configured to receive the gaseous ammonia and convert the gaseous ammonia into ionic ammonium; an electrolytic cell , is configured to electrolyze an aqueous sodium chloride solution as an electrolyte to form a solution containing hypochlorous acid and hydrogen; a reaction tank is connected to the electrolytic cell and the absorption tower, and is configured to make the ionic ammonium and The solution containing hypochlorous acid reacts to degrade the ionic ammonium to nitrogen gas; and a fuel cell is configured to receive the hydrogen gas generated by the electrolysis reaction and use the hydrogen gas as a fuel to generate electrical energy. 如請求項6所述的氨氮廢水處理系統，更包括加藥器，經配置以將鹼液加入至所述氨氮廢水。 The ammonia nitrogen wastewater treatment system of claim 6, further comprising a dosing device configured to add lye to the ammonia nitrogen wastewater. 如請求項6所述的氨氮廢水處理系統，其中所述脫氨設備為超重力吹脫設備。 The ammonia nitrogen wastewater treatment system according to claim 6, wherein the deamination equipment is a supergravity stripping equipment. 如請求項6所述的氨氮廢水處理系統，其中所述吸收塔連通於所述電解槽，所述電解槽中的所述電解液部分地回流至所述吸收塔，且所述氣態氨在所述吸收塔內水解於所述電解液中，以轉化為所述離子銨。 The ammonia nitrogen wastewater treatment system according to claim 6, wherein the absorption tower is communicated with the electrolytic cell, the electrolyte in the electrolytic cell is partially returned to the absorption tower, and the gaseous ammonia is stored in the electrolytic cell. It is hydrolyzed in the electrolyte in the absorption tower to be converted into the ionic ammonium. 如請求項6所述的氨氮廢水處理系統，更包括：曝氣筒，連通於所述電解槽與所述反應槽之間，且經配置以對於所述電解反應的生成物進行氣液分離，其中所述反應槽接收所述曝 氣筒所分離出的液體。 The ammonia nitrogen wastewater treatment system according to claim 6, further comprising: an aeration cylinder, connected between the electrolysis tank and the reaction tank, and configured to perform gas-liquid separation on the product of the electrolysis reaction, wherein the reaction tank receives the exposure The liquid separated from the gas cylinder.
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