TWI427041B - Combined with the adsorption and oxidation and activation of water pollutants - Google Patents
Combined with the adsorption and oxidation and activation of water pollutants Download PDFInfo
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本發明係有關於一種「兼具吸附性與氧化性及活化性之水中污染物處理方法」，尤指一種以過硫酸鹽之穩定性為基礎結合低價之吸附劑與含鐵活化劑之水污染整法方法者。 The present invention relates to a method for treating water contaminants having both adsorption and oxidation and activating properties, and more particularly to a combination of a low-cost adsorbent and an iron-containing activator based on the stability of persulfate. The method of polluting the whole method.
地下水被汽油等石油碳氫化合物所污染是一個愈趨普遍且嚴重的問題，而造成油污染之主要來源包括地下儲油槽漏油、油管破裂、及地面油品亦外洩漏等，由於加油站及大型儲油槽的管線設備多設置於地表層下，隨著設備老舊、地震、施工不良或其他人為因素，洩漏機會隨之增加；在美國有兩百萬個以上的儲油槽，據估計有35%儲油槽可能在漏油(Bedient et al.,1999)，目前台灣油污染案件有逐漸增加之趨勢，而土壤及地下水污染問題，已是國內外關注的重要議題。 The groundwater is polluted by petroleum hydrocarbons such as gasoline, which is an increasingly common and serious problem. The main sources of oil pollution include oil spills in underground oil storage tanks, oil pipe rupture, and leakage of ground oil, due to gas stations and The pipeline equipment of large oil storage tanks is mostly placed under the surface layer. With the old equipment, earthquake, poor construction or other human factors, the leakage opportunity increases. There are more than 2 million oil storage tanks in the United States, estimated to be 35. % oil storage tanks may be leaking oil (Bedient et al., 1999). At present, there is a trend of increasing oil pollution in Taiwan, and soil and groundwater pollution has become an important issue at home and abroad.
傳統處理/整治受污染地下水技術，如抽取處理法(pump and treat,R&T)是最廣泛被使用於各污染場址之技術，但傳統方法常耗時甚久，且長期整治所需之花費亦可能增高，目前受污染場址之整治復育，基於成本及相關考量，大多採取現地(in-site)整治之方式(US EPA,2004)。 Conventional treatment/remediation of contaminated groundwater technologies, such as pump and treat (R&T), is the most widely used technique for contaminated sites, but traditional methods often take a long time and the cost of long-term remediation is also It may increase, and the current remediation of contaminated sites, based on cost and related considerations, mostly takes the form of in-site remediation (US EPA, 2004).
現地化學氧化法(in situ chemical oxidation,ISCO)為將 氧化劑注入受污染區域，藉以破壞目標污染物之整治方法，理想條件下污染物將完全氧化成二氧化碳、水及其他無害物質(ITRC,2005)，常見的氧化劑種類包括過氧化氫(H2O2)[芬頓試劑(Fenton’s reagent)]、過錳酸鹽(permanganate)、過硫酸鹽(persulfate)及臭氧等，而利用過硫酸鹽當做氧化劑是目前較新發展出來的現地化學處理程序(ITRC,2005)，過硫酸鹽為一強氧化劑，經熱或金屬(如二價鐵)活化可產生硫酸根自由基(SO4 -˙)，快速降解污染物(Shiying et al.,2008；Chen et al.,2009)，而目前習知之現地化學氧化法，多如附件一(該係 鈞局於98年7月1日所公開之公開編號第200927672號之「於含有水之污染介質中可持續釋放氧化劑以降解污染物之方法及其釋氧化劑組成物」，該申請日期為96年12月31日)及附件二(該係 鈞局於93年4月11日所核准專利公告號第583145號之「一種具有持續釋放氧氣功能的人造釋氧合成物」，該申請日期為90年10月22日)所示，而由附件一、二之申請專利範圍及圖式中可分析得知，其尚有下述之缺失：(一)其僅以過硫酸鹽或以水泥與過硫酸鹽組成釋氧化劑物質，去除水中污染物，惟過硫酸鹽在未活化下去除污染物之效果有待加強；(二)其欲加速污染物之移除，需額外加熱或添加過渡金屬如二價鐵催化過硫酸鹽，除造成整治成本增加外，二價鐵氧化成三價鐵後，將會沉澱造成阻塞，降低含水層之 滲透性。 In situ chemical oxidation (ISCO) is a method for remediation of target pollutants by injecting an oxidant into a contaminated area. Under ideal conditions, the pollutants will be completely oxidized into carbon dioxide, water and other harmless substances (ITRC, 2005). Common oxidant species include hydrogen peroxide (H 2 O 2 ) [Fenton's reagent], permanganate, persulfate, and ozone, while using persulfate as an oxidant. It is a relatively new in-situ chemical treatment program (ITRC, 2005). Persulfate is a strong oxidant. It can generate sulfate radicals (SO 4 - ̇) by heat or metal (such as ferrous iron) activation. Degradation of pollutants (Shiying et al., 2008; Chen et al., 2009), and the current local chemical oxidation method, as in Annex I (the public number of the system published on July 1, 1998) 200927672 "Method for the sustainable release of oxidants in water-containing contaminating media to degrade pollutants and its oxidant composition", date of application is December 31, 1996) and Annex II (the system is in 1993) Approved on April 11, Announcement No. 583145, "An artificial oxygen release composition with sustained release of oxygen," the application date is October 22, 1990), and the scope and schema of the application can be found in Annexes I and II. It is found that there are still the following defects: (1) it only uses persulfate or cement and persulfate to form an oxidant substance to remove pollutants in water, but persulfate removes contaminants without activation. The effect needs to be strengthened; (2) it wants to accelerate the removal of pollutants, additional heating or addition of transition metals such as ferrous iron to catalyze persulfate, in addition to the increase in remediation costs, after the oxidation of ferrous iron into ferric iron, It will precipitate and cause blockage and reduce the permeability of the aquifer.
因此，若能研發出一種整合式之處理系統，該處理系統乃具有吸附性、活化性及氧化性，俾可加速污染物之降解，亦可延緩污染物之移動，降低污染物對下游之威脅，乃係本發明人所欲改良之問題所在。 Therefore, if an integrated treatment system can be developed, the treatment system has adsorption, activating and oxidizing properties, which can accelerate the degradation of pollutants, delay the movement of pollutants, and reduce the threat of pollutants to the downstream. It is the problem that the inventors want to improve.
故本發明人有鑑於此，乃思及創作的意念，遂以多年的經驗加以設計，經多方探討並試作樣品試驗，及多次修正改良，乃推出本發明。 Therefore, the present inventors have invented the present invention in view of the above, and the idea of creation and creation, which has been designed with many years of experience, has been explored and tested by many parties, and has been repeatedly modified and improved.
本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，其整合式處理系統主要係以過硫酸鹽之穩定性為基礎結合低價之吸附劑(天然沸石)與含鐵活化劑(即工業廢棄物之高爐石、轉爐石)，由於吸附劑與活化劑共同存在時，不但可吸附污染物且亦具有異相活化過硫酸鹽之作用，若能應用整治牆之原理，將吸附劑及活化劑與過硫酸鹽混合，製成可長期緩慢釋放過硫酸鹽之合成物質，則此氧化劑釋放物質所形成之整治牆，不但可延緩污染物流過之時間，亦可藉由異相催化作用有效去除污染物，讓此系統具有氧化、吸附及活化過硫酸鹽之特性，以用來處理受有機物污染之水及地下水；藉此，係能構成該兼具吸附性與氧化性及活 化性之水中污染物處理方法者。 The invention discloses an aqueous pollutant treatment method with adsorption, oxidation and activation, and the integrated treatment system is mainly based on the stability of persulfate combined with a low-cost adsorbent (natural zeolite) and iron-containing activation. Agent (ie blast furnace stone and converter stone of industrial waste), because the adsorbent and the activator coexist, not only can adsorb pollutants but also have the function of heterogeneous activated persulfate. If the principle of rectifying the wall can be applied, it will adsorb The agent and the activator are mixed with the persulfate to form a synthetic substance capable of slowly releasing the persulfate for a long period of time, and the rectifying wall formed by the oxidizing agent releasing material not only delays the flow of the contaminant, but also acts by heterogeneous catalysis. Effectively removes contaminants, allowing the system to oxidize, adsorb and activate persulfate to treat water and groundwater contaminated with organic matter; thereby, it can constitute both adsorption and oxidation and live Chemical water treatment methods.
(一)本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，其整合式處理系統中含有過硫酸鹽及低價之吸附劑與含鐵活化劑，過硫酸鹽具氧化性，低價吸附劑不但具有吸附能力，且位於活化劑表面之過渡金屬如鐵，亦具有活化過硫酸鹽之能力，不但可加速污染物之去除，亦可延緩污染物之移動，降低污染物對下游之威脅。 (1) The method for treating water contaminants having both adsorption, oxidation and activating properties according to the present invention, wherein the integrated treatment system contains persulfate and a low-cost adsorbent and an iron-containing activator, and the persulfate is oxidized. The low-cost adsorbent not only has the adsorption capacity, but also the transition metal such as iron on the surface of the activator has the ability to activate persulfate, which not only accelerates the removal of pollutants, but also delays the movement of pollutants and reduces pollutants. The threat to the downstream.
(二)本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，轉爐石及高爐石皆為工業廢棄物，本整合式處理系統之研發將提供工業廢棄物另一資源再利用管道，俾減去該工業廢棄物後續處理之困難與麻煩。 (2) The method for treating water pollutants having both adsorption, oxidation and activating properties of the present invention, converter stone and blast furnace stone are industrial wastes, and the research and development of the integrated treatment system will provide another resource for industrial waste. By using the pipeline, the difficulties and troubles of the subsequent disposal of the industrial waste are reduced.
(三)本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，其活化劑可自行催化過硫酸鹽，產生硫酸根自由基，以增強氧化能力。 (3) The method for treating water contaminants having both adsorptivity, oxidizing property and activating property of the present invention, wherein the activator can catalyze persulfate by itself to generate sulfate radicals to enhance the oxidizing ability.
(四)本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，其吸附劑具有現地自淨之功能，且該整合式處理系統無需使用大量的吸附劑，以降低污染場址整治之成本。 (4) The method for treating water pollutants having both adsorption, oxidation and activating properties according to the invention, wherein the adsorbent has the function of self-purification, and the integrated treatment system does not need to use a large amount of adsorbent to reduce the pollution site. The cost of remediation.
(五)本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，其可依場址狀況及整治時程之需求，適度調整過硫酸鹽、 吸附劑與活化劑之結合比例，以獲得最佳之整治成效。 (5) The method for treating water pollutants having both adsorption, oxidation and activating properties according to the present invention, which can appropriately adjust persulfate according to site conditions and requirements of remediation time course. The combination ratio of adsorbent and activator to obtain the best remediation effect.
(六)本發明之兼具吸附性與氧化性及活化性之水中污染物處理方法，其同時具有氧化、活化及吸附之功用，可有效去除污染物並延緩污染物流至下游受體之時間者。 (6) The method for treating water pollutants having both adsorption, oxidation and activating properties of the present invention, which simultaneously has the functions of oxidation, activation and adsorption, can effectively remove pollutants and delay the flow of pollutants to downstream receptors. .
為使 貴審查委員對本發明之目的、特徵及功效能夠有更進一步之瞭解與認識，以下茲請配合【圖式簡單說明】詳述如后：通常根據本發明，先請由第一圖所示觀之，本發明係提供一種兼具吸附性與氧化性及活化性之水中污染物處理方法，其整合式處理系統(10)主要係以過硫酸鹽(11)之穩定性為基礎結合低價之吸附劑(12)(天然沸石)與含鐵活化劑(13)(即工業廢棄物之高爐石、轉爐石)，由於吸附劑(12)與活化劑(13)共存時，不但可吸附污染物且亦具有異相活化過硫酸鹽(11)之作用，若能應用整治牆之原理，將吸附劑(12)及活化劑(13)與過硫酸鹽(11)混合，製成可長期緩慢釋放過硫酸鹽(11)之合成物質，則此氧化劑釋放物質所形成之整治牆，不但可延緩污染物流過之時間，亦可藉由異相催化作用有效去除污染物，讓此系統具有氧化、吸附及活化過硫酸鹽(11)之特性，以用來處理受有機物污染之水及地下水，其中：過硫酸鹽(11)為一較為長效性之氧化劑，且其不傾向與土壤 中的有機物反應之特性亦使得過硫酸鹽(11)應用時所需之藥劑量較其他氧化劑為低，因此，過硫酸鹽氧化法之使用除了可有效去除污染物外，亦可降低污染場址整治之成本；天然沸石為較低價之吸附劑(12)，該係選用絲光沸石(日本試藥級)，而高爐石(blast furnace slag,BF Slag)及轉爐石(basic oxygen furnace slag,BOF Slag)為工業廢棄物，由於高爐石及轉爐石的粒徑不一，因此使用前先利用10~18mesh(1~2mm)篩網過篩，並以5% HCl進行酸洗去除雜質，而後以去離子水清洗數次，再將爐石置於105℃烘乾24小時後保存於乾燥箱(Cao et al.,2003)，而絲光沸石則因為是商業化產品，故在使用前並未進行前置處理，且依表1化學組成分析得知，二種活化劑(13)之含鐵量均介於2.5-37.7%間，鐵的存在顯示這些活化劑(13)具有活化過硫酸鹽(11)之潛力。 In order to enable your review committee to have a better understanding and understanding of the purpose, features and effects of the present invention, please refer to the following [detailed description of the drawings] as follows: usually according to the present invention, please first show by the first figure In view of the above, the present invention provides a method for treating water contaminants having both adsorption, oxidation and activating properties, and the integrated treatment system (10) is mainly based on the stability of persulfate (11). The adsorbent (12) (natural zeolite) and the iron-containing activator (13) (ie, blast furnace stone and converter stone of industrial waste) can not only adsorb pollution when the adsorbent (12) and the activator (13) coexist. And also has the function of heterogeneous activated persulfate (11). If the principle of rectifying the wall can be applied, the adsorbent (12) and the activator (13) are mixed with the persulfate (11) to form a long-term slow release. The synthetic material of persulfate (11), the remediation wall formed by the oxidant releasing material not only delays the flow of the contaminant, but also effectively removes the contaminant by heterogeneous catalysis, so that the system has oxidation, adsorption and Activate the characteristics of persulfate (11) to Treated water and groundwater contaminated by organic compounds, wherein: persulfates (11) is a relatively long-term nature of the oxidizing agent, and it tends not to soil The characteristics of the organic matter reaction also make the persulfate (11) application lower than other oxidants. Therefore, the use of the persulfate oxidation method can effectively remove the pollutants and reduce the pollution site. The cost of remediation; natural zeolite is a lower-priced adsorbent (12), which uses mordenite (Japanese reagent grade), while blast furnace slag (BF Slag) and converter stone (basic oxygen furnace slag, BOF Slag) is industrial waste. Due to the different particle sizes of blast furnace stone and converter stone, it is sieved with 10~18mesh (1~2mm) sieve before use and pickled with 5% HCl to remove impurities. The deionized water was washed several times, and the hearth was dried at 105 ° C for 24 hours and then stored in a dry box (Cao et al., 2003). Since the mordenite was a commercial product, it was not used before use. Pretreatment, and according to the chemical composition analysis of Table 1, the iron content of the two activators (13) are between 2.5 and 37.7%. The presence of iron indicates that these activators (13) have activated persulfate ( 11) The potential.
為瞭解本發明之整合式處理系統(10)對污染物移除之效率，我們以地下水中常見之污染物甲基第三丁基醚(methyl tert-butyl ether,MTBE)為目標污染物，利用本系統將其移除，並比較氧化、活化作用與吸附作用去除MTBE之差異性，由實驗結果可知，添加吸附劑(12)具有吸附作用，添加活化劑(13)有助於過硫酸鹽(11)之催化，促進MTBE之降解，且添加劑量越高，降解效率越佳，其原因應為活化劑(13)中所含之金屬物質如鐵作用所致。 In order to understand the efficiency of pollutant removal in the integrated treatment system (10) of the present invention, we use methyl tert-butyl ether (MTBE), a common pollutant in groundwater, as a target pollutant. The system removes it and compares the difference between oxidation, activation and adsorption to remove MTBE. From the experimental results, it is known that the addition of adsorbent (12) has adsorption, and the addition of activator (13) contributes to persulfate ( 11) Catalytic, promoting the degradation of MTBE, and the higher the amount of additives, the better the degradation efficiency, which is caused by the action of metal substances such as iron contained in the activator (13).
藉由上述兼具吸附性與氧化性及活化性之水中污染物處理方 法，其實際使用時，係將過硫酸鹽(11)及低價吸附劑(12)與含鐵活化劑(13)直接添加於受污染水及地下水中，藉由氧化、活化及吸附機制去除及破壞污染物(請同時由第二圖所示觀之)。 By treating the above-mentioned water pollutants with both adsorption and oxidation and activation In the actual use, the persulfate (11) and the low-valent adsorbent (12) and the iron-containing activator (13) are directly added to the contaminated water and groundwater, and are removed by oxidation, activation and adsorption mechanisms. And destroying pollutants (please view them as shown in the second figure).
或者，將過硫酸鹽(11)及低價吸附劑(12)與含鐵活化劑(13)包覆於水泥(20)中，再放置於受污染水及地下水中(請同時由第三圖所示觀之)，當水滲入水泥(20)，過硫酸鹽(11)即會釋放，可延長過硫酸鹽(11)於之存在時間，並藉由氧化、活化及吸附機制去除及破壞污染物，且因為在此半滲透性的合成物質中，過硫酸鹽(11)為氧化劑，砂可增加此物質之孔隙率以利釋放過硫酸鹽(11)，吸附劑(12)與活化劑(13)除具有吸附及異相催化功能外，亦可取代砂增加孔隙率，水泥為凝結劑，用以凝結各種組成物，將合成後之塊狀物放置陰涼處2~3天將可完全乾燥，其合成物表面具有微孔隙，可利過硫酸鹽(11)長期溶出釋放，由其累積釋放量之實驗結果顯示(該實驗之數值請同時由第四圖至第六圖所示觀之)，所有合成的氧化劑釋放物質，過硫酸鹽(11)累積釋放時間皆可維持約30天以上，前5天過硫酸鹽(11)之釋放量為最快，而後過硫酸鹽(11)釋放速率可達到穩定趨勢，顯示氧化劑釋放物質具有長期釋放氧化劑之效果。 Alternatively, the persulfate (11) and the low-cost adsorbent (12) and the iron-containing activator (13) are coated in the cement (20) and placed in the contaminated water and groundwater (please also by the third figure) As shown in the figure), when water penetrates into the cement (20), the persulfate (11) is released, which prolongs the existence of the persulfate (11), and removes and destroys the pollution by oxidation, activation and adsorption mechanisms. And because persulfate (11) is an oxidant in this semi-permeable synthetic material, sand can increase the porosity of the material to facilitate the release of persulfate (11), adsorbent (12) and activator ( 13) In addition to the adsorption and heterogeneous catalysis function, it can also replace the sand to increase the porosity. The cement is a coagulant, which is used to coagulate various components. The composited block can be completely dried after being placed in a cool place for 2~3 days. The surface of the composite has microporosity, which can be extended by long-term dissolution and release of sulfate (11). The experimental results of the cumulative release amount are shown (the values of the experiment are also shown in the fourth to sixth figures). All synthetic oxidant release materials, persulfate (11) cumulative release time can be maintained for more than 30 days, before The release of persulfate (11) was the fastest in 5 days, and the release rate of persulfate (11) reached a stable trend, indicating that the oxidant-releasing substance had the effect of releasing the oxidant for a long time.
藉由上述兼具吸附性與氧化性及活化性之水中污染物處理方法具有下列之優點：(一)其整合式處理系統(10)中含有過硫酸鹽 (11)及低價之吸附劑(12)與含鐵活化劑(13)，過硫酸鹽(11)具氧化性，低價吸附劑(12)具有吸附能力，而活化劑(13)表面之過渡金屬如鐵，亦具有活化過硫酸鹽(11)之能力，不但可加速污染物之去除，亦可延緩污染物之移動，降低污染物對下游之威脅；(二)轉爐石及高爐石皆為工業廢棄物，本整合式處理系統(10)之研發將提供工業廢棄物另一資源再利用管道，俾減去該工業廢棄物後續處理之困難與麻煩；(三)其活化劑(13)可自行催化過硫酸鹽(11)，產生硫酸根自由基，以增強氧化能力；(四)其吸附劑(12)具有現地自淨之功能，且該整合式處理系統(10)無需使用大量的吸附劑，以降低污染場址整治之成本；(五)可依場址狀況及整治時程之需求，適度調整過硫酸鹽(11)、吸附劑(12)與活化劑(13)之結合比例，以獲得最佳之整治成效；(六)本整合式處理系統(10)同時具有氧化、活化及吸附之功用，可有效去除污染物並延緩污染物流至下游受體之時間者。 The above-mentioned water contaminant treatment method having both adsorptivity, oxidizability and activating property has the following advantages: (1) the persulfate salt in the integrated treatment system (10) (11) and low-cost adsorbent (12) and iron-containing activator (13), persulfate (11) is oxidizing, low-priced adsorbent (12) has adsorption capacity, and activator (13) surface Transition metals such as iron also have the ability to activate persulfate (11), which not only accelerates the removal of pollutants, but also delays the movement of pollutants and reduces the threat of pollutants downstream; (2) converter stone and blast furnace stone For industrial waste, the development of this integrated treatment system (10) will provide another resource reuse pipeline for industrial waste, and reduce the difficulty and trouble of subsequent treatment of the industrial waste; (3) its activator (13) It can self-catalyze persulfate (11) to produce sulfate radicals to enhance oxidation capacity; (4) its adsorbent (12) has the function of self-purification, and the integrated treatment system (10) does not require a large amount of adsorption. To reduce the cost of remediation of contaminated sites; (5) to adjust the ratio of persulfate (11), adsorbent (12) and activator (13) according to the site conditions and the time of remediation. To achieve the best remediation results; (6) The integrated treatment system (10) has both oxidation and activity And the adsorption function, can effectively remove contaminants and contaminated stream to a time delay by a downstream receptor.
唯以上所述者，僅為本發明之一較佳實施例而已，當不能以之限定本發明實施之範圍；即大凡依本發明申請專利範圍所作之均等變化與修飾，皆應仍屬本創作專利涵蓋之範圍內。 The above is only a preferred embodiment of the present invention, and the scope of the present invention is not limited thereto; that is, the equal variation and modification of the scope of the patent application of the present invention should still belong to the present creation. Within the scope of the patent.
(10)‧‧‧整合式處理系統 (10) ‧‧‧Integrated Processing System
(11)‧‧‧過硫酸鹽 (11)‧‧‧Persulfate
(12)‧‧‧吸附劑 (12) ‧ ‧ sorbent
(13)‧‧‧活化劑 (13) ‧ ‧ activators
(20)‧‧‧水泥 (20) ‧‧‧Cement
第一圖：係本發明之方塊圖。 First Figure: is a block diagram of the present invention.
第二圖：係本發明之一種使用狀態圖。 Second Figure: A state of use diagram of the present invention.
第三圖：係本發明之另一種使用狀態圖。 Third Figure: Another use state diagram of the present invention.
第四圖：係本發明添加不同高爐石劑量活化過硫酸鹽對MTBE降解之影響圖。 The fourth figure is the effect of the addition of different blast furnace stone dosages of activated persulfate on the degradation of MTBE.
第五圖：係本發明添加不同轉爐石劑量活化過硫酸鹽對MTBE降解之影響圖。 Fig. 5 is a graph showing the effect of the addition of different converter stone dosages of activated persulfate on the degradation of MTBE in the present invention.
第六圖：係本發明沸石對MTBE之吸附去除效率圖。 Figure 6 is a graph showing the adsorption removal efficiency of the zeolite of the present invention for MTBE.
附件一：係本國專利公開編號第200927672號之公開影本。 Annex I: The public copy of National Patent Publication No. 200927672.
附件二：係本國專利公告號第583145號之公告影本。 Annex II: A copy of the announcement of National Patent Publication No. 583145.
(10)‧‧‧整合式處理系統 (10) ‧‧‧Integrated Processing System
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