TW202313476A - Method for recovering zinc-68 isotope from the preparation method of copper-64 - Google Patents
Method for recovering zinc-68 isotope from the preparation method of copper-64 Download PDFInfo
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/20—Recycling
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Abstract
Description
本發明係有關一種回收鋅-68同位素之方法,尤其是一種自銅-64製程回收鋅-68同位素之方法。The present invention relates to a method for recovering zinc-68 isotope, especially a method for recovering zinc-68 isotope from copper-64 process.
近年來,正子斷層攝影(Positron Emission Tomography,簡稱PET)以飛快的速度崛起,成為醫學上一項重要的診斷造影模式,主要被用來確定癌症的發生與嚴重性、神經系統的狀況以及心血管方面的疾病。In recent years, Positron Emission Tomography (PET) has risen rapidly and has become an important diagnostic imaging mode in medicine. It is mainly used to determine the occurrence and severity of cancer, the condition of the nervous system and the cardiovascular system. aspects of the disease.
目前PET已被公認在某些疾病判定方面特別有效,包括判斷癌症是否存在,是否已擴散轉移,對治療是否有所反應,檢查癌症是否復發以及病患在治療後是否已不再有癌細胞,使用PET特別有效的癌症包括肺癌、頭頸癌、大腸直腸癌、食道癌、淋巴瘤、黑色素瘤、乳癌、甲狀腺癌、子宮頸癌、胰臟癌以及腦瘤。At present, PET has been recognized as particularly effective in certain diseases, including judging whether cancer exists, whether it has spread, whether it responds to treatment, whether the cancer recurs, and whether the patient no longer has cancer cells after treatment. Cancers in which PET is particularly effective include lung, head and neck, colorectal, esophagus, lymphoma, melanoma, breast, thyroid, cervix, pancreas, and brain tumors.
簡言之,使用PET造影,需在病人身上注射放射性藥物,放射性藥物在病人體內釋出訊號,而被體外的PET掃瞄儀所接收,繼而形成影像,利用PET所攝得的影像可顯現出器官或組織(如腫瘤)的化學變化。In short, to use PET imaging, it is necessary to inject radiopharmaceuticals into the patient. The radiopharmaceuticals release signals in the patient's body, which are received by the PET scanner outside the body and then form images. The images captured by PET can show A chemical change in an organ or tissue, such as a tumor.
再者,放射性同位素依其釋出之輻射線種類之不同,研製成核醫藥物劑型後,可應用於疾病之診斷或治療。迴旋加速器為臨床核醫藥物之重要同位素產生器,可產製鉈-201、銦-111、碘-123、氟-18及鎵-67等中長半衰期同位素,以及碳-11、氧-15及氮-13等短半衰期之核種,應用於心血管疾病、甲狀腺功能、腫瘤、發炎及代謝疾病等等之診斷。Furthermore, radioactive isotopes can be used in the diagnosis or treatment of diseases after they are developed into nucleated pharmaceutical dosage forms according to the types of radiation they release. The cyclotron is an important isotope generator for clinical nuclear medicine. It can produce medium and long half-life isotopes such as thallium-201, indium-111, iodine-123, fluorine-18 and gallium-67, as well as carbon-11, oxygen-15 and Nuclear species with a short half-life such as nitrogen-13 are used in the diagnosis of cardiovascular diseases, thyroid function, tumors, inflammation and metabolic diseases, etc.
隨著核子醫學之進展與臨床之需求,迴旋加速器除了診斷用同位素之研製,對於治療用同位素之產製與應用亦漸受注意,其中兼具診斷與治療功能之放射性同位素銅-64尤其受到重視。With the development of nuclear medicine and clinical needs, in addition to the development of isotopes for diagnosis, cyclotrons have gradually attracted attention to the production and application of isotopes for treatment. Among them, the radioactive isotope copper-64, which has both diagnostic and therapeutic functions, has received special attention. .
銅-64的半衰期適中(12.7小時),可以釋出511keV的能量,適合用於PET造影,亦可釋放1346keV之貝它射線,兼具治療之潛力。銅-64結合上適當之配位子(例如小分子化合物、胜肽或單株抗體)可應用於疾病之診斷或治療用途。Copper-64 has a moderate half-life (12.7 hours) and can release energy of 511keV, which is suitable for PET imaging. It can also release beta rays of 1346keV, which has therapeutic potential. Copper-64 combined with appropriate ligands (such as small molecular compounds, peptides or monoclonal antibodies) can be used in the diagnosis or treatment of diseases.
然而,銅-64之半衰期僅為12.7小時,不易保存,有鑑於此,通常以30MeV中型迴旋加速器進行銅-64同位素之研製,其係將高豐度穩定同位素鎳-64電鍍於固體靶後,以15~18MeV的質子射束照射,再經分離純化步驟,可獲得高純度之放射性同位素銅-64。However, the half-life of copper-64 is only 12.7 hours, and it is not easy to preserve. In view of this, the development of copper-64 isotope is usually carried out in a 30MeV medium-sized cyclotron, which is to electroplate the high-abundance stable isotope nickel-64 on the solid target. Irradiate with a proton beam of 15-18 MeV, and then undergo separation and purification steps to obtain high-purity radioactive isotope copper-64.
但是,高豐度穩定同位素的鎳-64價格相當昂貴。為節省成本,目前已建立以鋅-68固體靶經迴旋加速器照射研製鎵-67同位素的技術。並參考鋅-68的核反應圖,可知其產生之核種除了鎵-66、鎵-67以及鎵-68外,另一重要的產物即為銅-64。However, nickel-64, a highly abundant stable isotope, is quite expensive. In order to save cost, the technology of preparing gallium-67 isotope with zinc-68 solid target through cyclotron irradiation has been established. And referring to the nuclear reaction diagram of zinc-68, it can be seen that in addition to gallium-66, gallium-67 and gallium-68, another important product is copper-64.
然而,雖已建立鋅-68固體靶經迴旋加速器照射同時產製兩種具有應用價值的放射性同位素鎵-67以及銅-64之技術。但,鋅-68固體靶之價格昂貴,如若單純依靠進口無法符合使用者之實際使用所需。However, the technology of simultaneously producing two valuable radioisotopes gallium-67 and copper-64 through cyclotron irradiation on a zinc-68 solid target has been established. However, the price of zinc-68 solid target is expensive, and it cannot meet the actual needs of users if only relying on imports.
為此,節省原料藥費用、降低核醫製藥成本,並且在充分供應病患使用而不受限制的情況下,減少對環境的污染,為本技術領域人員所要解決的問題。For this reason, it is a problem to be solved by those skilled in the art to save the cost of raw materials, reduce the cost of nuclear medicine, and reduce the pollution to the environment under the condition of sufficient supply to patients without restriction.
本發明之主要目的,係提供一種自銅-64製程回收鋅-68同位素之方法,在鋅-68固體靶經迴旋加速器照射,產製放射性同位素銅-64之製程中,進一步回收鋅-68再次利用於銅-64製程,以減少原物料成本。The main purpose of the present invention is to provide a method for reclaiming zinc-68 isotope from the copper-64 process, in which the zinc-68 solid target is irradiated by a cyclotron to produce the radioactive isotope copper-64, further reclaiming zinc-68 again It is used in the copper-64 process to reduce the cost of raw materials.
為了達到上述目的及功效,本發明揭示了一種自銅-64製程回收鋅-68同位素之方法,其步驟包含:取一銅-64水洗殘液與一氫氧化物進行一沉澱反應,反應生成一氫氧化鋅;取該氫氧化鋅進行一pH值調整,調整該氫氧化鋅至pH值10~11之間;取該氫氧化鋅進行一電鍍反應,反應形成一含鋅離子之成品液;以及取該含鋅離子之成品液進行一加熱濃縮處理,形成一鋅-68同位素。In order to achieve the above purpose and effect, the present invention discloses a method for recovering zinc-68 isotope from the copper-64 process. Zinc hydroxide; take the zinc hydroxide to adjust the pH value, and adjust the zinc hydroxide to a pH value between 10 and 11; take the zinc hydroxide to perform an electroplating reaction, and react to form a finished solution containing zinc ions; and The product solution containing zinc ions is subjected to a heat concentration treatment to form a zinc-68 isotope.
本發明提供一實施例,其內容在於自銅-64製程回收鋅-68同位素之方法,其中於取一銅-64水洗殘液與一氫氧化物進行一沉澱反應之步驟中,該銅-64水洗殘液係包含一鋅離子、一鎵離子以及一銅離子。The present invention provides an embodiment, which is a method for recovering zinc-68 isotope from the copper-64 process, wherein in the step of taking a copper-64 washing raffinate and a hydroxide for a precipitation reaction, the copper-64 The washing raffinate contains a zinc ion, a gallium ion and a copper ion.
本發明提供一實施例,其內容在於自銅-64製程回收鋅-68同位素之方法,其中於取一銅-64水洗殘液與一氫氧化物進行一沉澱反應之步驟中,該銅-64水洗殘液係由一銅-64製程中回收而來,該銅-64製程係由一質子束照射一鋅-68固體靶。The present invention provides an embodiment, which is a method for recovering zinc-68 isotope from the copper-64 process, wherein in the step of taking a copper-64 washing raffinate and a hydroxide for a precipitation reaction, the copper-64 The washing residue is recovered from a copper-64 process in which a proton beam irradiates a zinc-68 solid target.
本發明提供一實施例,其內容在於自銅-64製程回收鋅-68同位素之方法,其中於取一銅-64水洗殘液與一氫氧化物進行一沉澱反應之步驟中,該氫氧化物係氫氧化鈉。The present invention provides an embodiment, which is a method for recovering zinc-68 isotope from the copper-64 process, wherein in the step of taking a copper-64 washing raffinate and a hydroxide for a precipitation reaction, the hydroxide Department of sodium hydroxide.
本發明提供一實施例,其內容在於自銅-64製程回收鋅-68同位素之方法,其中於取該氫氧化鋅進行一pH值調整之步驟中,該pH值調整係透過一氫氧化鈉及一鹽酸進行調整。The present invention provides an embodiment, the content of which is the method for recovering zinc-68 isotope from the copper-64 process, wherein in the step of taking the zinc hydroxide to adjust the pH value, the pH value adjustment is through a sodium hydroxide and A hydrochloric acid to adjust.
本發明提供一實施例,其內容在於自銅-64製程回收鋅-68同位素之方法,其中於取該氫氧化鋅進行一pH值調整之步驟後,進一步包含步驟:取該氫氧化鋅進行一真空過濾製程。The present invention provides an embodiment, the content of which is the method for recovering zinc-68 isotope from the copper-64 process, wherein after the step of adjusting the pH value of the zinc hydroxide, further comprising the step of: taking the zinc hydroxide for a Vacuum filtration process.
本發明提供一實施例,其內容在於自銅-64製程回收鋅-68同位素之方法,其中於取該氫氧化鋅進行一電鍍反應之步驟中,於該電鍍反應中係進一步加入一氮氣。The present invention provides an embodiment, which is a method for recovering zinc-68 isotope from the copper-64 process, wherein in the step of taking the zinc hydroxide for an electroplating reaction, a nitrogen gas is further added to the electroplating reaction.
為使貴審查委員對本發明之特徵及所達成之功效有更進一步之瞭解與認識,謹佐以實施例及配合說明,說明如後:In order to enable your review committee members to have a further understanding and understanding of the characteristics of the present invention and the achieved effects, the following examples and accompanying descriptions are hereby provided:
有鑑於核原料藥費用昂貴,無法充分供應病患使用的影響。據此,本發明遂提出一種自銅-64製程回收鋅-68同位素之方法,以解決習知技術所造成之問題。In view of the high cost of nuclear raw materials, it cannot be fully supplied to patients. Accordingly, the present invention proposes a method for recovering zinc-68 isotope from the copper-64 process to solve the problems caused by the prior art.
以下將進一步說明本發明之一種自銅-64製程回收鋅-68同位素之方法之其包含之特性、所搭配之結構及方法:A method for recovering zinc-68 isotope from the copper-64 process of the present invention will be further described below, including its included characteristics, matching structure and method:
首先,請參閱第1圖,其係本發明之一實施例之步驟流程圖。如圖所示,本發明之一種自銅-64製程回收鋅-68同位素之方法,其步驟包含:First of all, please refer to FIG. 1, which is a flowchart of the steps of an embodiment of the present invention. As shown in the figure, a method of recovering zinc-68 isotope from the copper-64 process of the present invention, the steps include:
S1:取銅-64水洗殘液與氫氧化物進行沉澱反應,反應生成氫氧化鋅;S1: Take the copper-64 water washing residue and carry out precipitation reaction with hydroxide to form zinc hydroxide;
S2:取氫氧化鋅進行pH值調整,調整氫氧化鋅至pH值10~11之間;S2: Take zinc hydroxide to adjust the pH value, and adjust the zinc hydroxide to a pH value between 10 and 11;
S3:取氫氧化鋅進行電鍍反應,反應形成含鋅離子之成品液;以及S3: taking zinc hydroxide for electroplating reaction to form a finished solution containing zinc ions; and
S4:取含鋅離子之成品液進行加熱濃縮處理,形成鋅-68同位素。S4: Take the finished liquid containing zinc ions and conduct heat concentration treatment to form zinc-68 isotope.
如步驟S1所示,取一銅-64水洗殘液與一氫氧化物進行一沉澱反應,反應生成一氫氧化鋅,其中該氫氧化物係氫氧化鈉。且,本發明之該銅-64水洗殘液係由一銅-64製程中回收而來,該銅-64製程係由一質子束照射一鋅-68固體靶。As shown in step S1, take a copper-64 washing residue and carry out a precipitation reaction with a hydroxide to form zinc hydroxide, wherein the hydroxide is sodium hydroxide. Moreover, the copper-64 washing residue of the present invention is recovered from a copper-64 process, and the copper-64 process is a zinc-68 solid target irradiated by a proton beam.
其本發明之該銅-64製程之詳細流程如下:本發明係採迴旋加速器之銅基銀靶,先將高豐度的鋅-68(豐度大於98%以上)電鍍於該銅基銀靶之靶面上(形成該鋅-68固體靶),並送入迴旋加速器之照射,接著在經29±2 MeV之該質子撞擊反應,接著在以當量濃度9N之HCL溶液溶解後,經由化學純化分離程序,得到鎵-67同位素。並同時收集了鎵-67酸流洗廢液。The detailed process of the copper-64 manufacturing process of the present invention is as follows: the present invention adopts the copper-based silver target of the cyclotron, and first electroplates high-abundance zinc-68 (abundance greater than 98%) on the copper-based silver target on the target surface (forming the zinc-68 solid target), and sent to the cyclotron for irradiation, followed by the proton impact reaction at 29 ± 2 MeV, and then dissolved in the HCL solution with an equivalent concentration of 9N, and chemically purified Separation procedure yields gallium-67 isotope. At the same time, gallium-67 acid washing waste liquid was collected.
之後,將鎵-67酸流洗廢液通過充填有陽離子交換樹脂(AG50W-X2, 100-200mesh, hydrogen form)之第一管柱,並繼續加入10 mL之9N之HCl溶液清洗第一管柱,並收集第一管柱之流出液。再,將第一管柱之流出液通過充填有陰離子交換樹脂(AG 1-X8, 100-200mesh, chloride form, Bio-Rad)之第二管柱,並繼續加入40 mL之9N之HCl溶液清洗第二管柱,並收集第二管柱之流出液。Afterwards, pass the gallium-67 acid washing waste liquid through the first column filled with cation exchange resin (AG50W-X2, 100-200mesh, hydrogen form), and continue to add 10 mL of 9N HCl solution to wash the first column , and collect the effluent from the first column. Then, pass the effluent from the first column through the second column filled with anion exchange resin (AG 1-X8, 100-200mesh, chloride form, Bio-Rad), and continue to add 40 mL of 9N HCl solution to wash the second column, and collect the effluent of the second column.
最後,再加入適量之約1N至2N之HCl溶液於第二管柱中,並收集其流出液。其流出液包含高純度銅-64同位素。並在流出液流出後,進一步加入適量的水於第二管柱,並收集其流出之液體,即為本發明之該銅-64水洗殘液。故,本發明之該銅-64水洗殘液係包含一鋅離子、一鎵離子以及一銅離子。Finally, an appropriate amount of about 1N to 2N HCl solution was added to the second column, and the effluent was collected. Its effluent contains high-purity copper-64 isotope. And after the effluent flows out, further add an appropriate amount of water to the second column, and collect the liquid that flows out, which is the copper-64 water washing raffinate of the present invention. Therefore, the copper-64 washing raffinate of the present invention contains a zinc ion, a gallium ion and a copper ion.
接續如步驟S2所示,取該氫氧化鋅進行一pH值調整,調整該氫氧化鋅至pH值10~11之間,該pH值調整係透過一氫氧化鈉及一鹽酸進行調整。該pH值調整之詳細流程如下:逐次加入2N NaOH溶液,直至該氫氧化鋅之pH值達到10至11之間,若pH值小於10加入2N NaOH,大於11則加入HCl(0.1至0.5N)。使該氫氧化鋅大量沉澱並淅出。Then, as shown in step S2, the zinc hydroxide is taken to adjust the pH value, and the zinc hydroxide is adjusted to a pH value between 10 and 11. The pH value adjustment is adjusted through sodium hydroxide and hydrochloric acid. The detailed process of the pH value adjustment is as follows: add 2N NaOH solution one by one until the pH value of the zinc hydroxide reaches between 10 and 11, if the pH value is less than 10, add 2N NaOH, if it is greater than 11, add HCl (0.1 to 0.5N) . The zinc hydroxide was allowed to precipitate in large quantities and was pumped out.
接續步驟S2後,取該氫氧化鋅持續攪拌0.5~2小時(較佳為1小時),電熱板磁石轉速設定300〜500RPM。接續進一步包含步驟S21:取該氫氧化鋅進行一真空過濾製程。該真空過濾製程後,再使用300ml之三次水漂洗該氫氧化鋅(此時已為濾餅狀)。After step S2 is continued, the zinc hydroxide is continuously stirred for 0.5-2 hours (preferably 1 hour), and the rotating speed of the electric heating plate magnet is set at 300-500 RPM. The process further includes step S21: taking the zinc hydroxide and performing a vacuum filtration process. After the vacuum filtration process, use 300ml of water to rinse the zinc hydroxide (in the shape of a filter cake) three times.
再者,如步驟S3所示,取該氫氧化鋅於濾杯中進行一電鍍反應,並於該電鍍反應中進一步加入一氮氣促溶。於此該電鍍反應中,每1公克之該氫氧化鋅應加入20ml之該電鍍前驅液。該電鍍反應後形成一含鋅離子之成品液,並暫存於成品瓶中。Furthermore, as shown in step S3, the zinc hydroxide is taken in the filter cup to perform an electroplating reaction, and a nitrogen gas is further added to the electroplating reaction to promote dissolution. In the electroplating reaction, 20 ml of the electroplating precursor solution should be added to every 1 gram of the zinc hydroxide. After the electroplating reaction, a finished solution containing zinc ions is formed, which is temporarily stored in the finished bottle.
於該電鍍反應後,再用300ml之三次水漂洗濾杯,並將濾杯中剩餘之該含鋅離子之成品液暫存於成品瓶中。After the electroplating reaction, rinse the filter cup with 300ml of water three times, and temporarily store the finished solution containing zinc ions remaining in the filter cup in the finished product bottle.
最後,如步驟S4所示,取該含鋅離子之成品液放置於800ml之燒杯內,並於電熱板上進行一加熱濃縮處理,其該加熱濃縮製程之溫度介於200至400℃之間(較佳為275℃)。又,磁石之轉速介於80至120 RPM之間(較佳為100 RPM),最終形成一鋅-68同位素。於此該加熱濃縮處理中,每要有1公克之鋅則需濃縮至20 ml之該含鋅離子之成品液。Finally, as shown in step S4, the finished product solution containing zinc ions is placed in an 800ml beaker, and a heating and concentration process is carried out on an electric heating plate, and the temperature of the heating and concentration process is between 200 and 400°C ( preferably 275°C). Also, the rotation speed of the magnet is between 80 to 120 RPM (preferably 100 RPM), and finally a zinc-68 isotope is formed. In this heat concentration treatment, every 1 gram of zinc needs to be concentrated to 20 ml of the finished solution containing zinc ions.
以下,為本發明之較佳實施例之詳細流程:取銅-64水洗殘液與氫氧化物(氫氧化鈉)進行沉澱反應,反應生成氫氧化鋅 。接續再將氫氧化鋅進行pH值調整,並調整至pH10~11之間。再者,進一步取氫氧化鋅持續攪拌1小時,電熱板磁石轉速設定300〜500RPM。接續進一步取氫氧化鋅進行真空過濾製程。真空過濾製程後,再使用300ml之三次水漂洗氫氧化鋅(此時已為濾餅狀)。The following is a detailed process of a preferred embodiment of the present invention: take the copper-64 water washing residue and carry out precipitation reaction with hydroxide (sodium hydroxide), and react to form zinc hydroxide. Then adjust the pH value of the zinc hydroxide, and adjust it to a pH between 10 and 11. Furthermore, further get zinc hydroxide and continue to stir for 1 hour, and the electric heating plate magnet speed setting is 300~500RPM. Continue to further take zinc hydroxide for vacuum filtration process. After the vacuum filtration process, use 300ml of water to rinse the zinc hydroxide (it is already in the form of a filter cake) three times.
又,取氫氧化鋅於濾杯中進行電鍍反應,並於電鍍反應中進一步加入氮氣促溶。再將電鍍反應後形成含鋅離子之成品液,暫存於成品瓶中。Also, take zinc hydroxide in the filter cup to carry out electroplating reaction, and further add nitrogen gas to promote dissolution in the electroplating reaction. After the electroplating reaction, a finished product solution containing zinc ions is formed, which is temporarily stored in the finished product bottle.
最後,將含鋅離子之成品液進行加熱濃縮處理(為275℃以及100RPM),並經加熱濃縮處理後,從含鋅離子之成品液中取得鋅-68同位素。Finally, heat and concentrate the product solution containing zinc ions (at 275° C. and 100 RPM), and obtain zinc-68 isotope from the product solution containing zinc ions after the heat concentration treatment.
故本發明實為一具有新穎性、進步性及可供產業上利用者,應符合我國專利法專利申請要件無疑,爰依法提出發明專利申請,祈 鈞局早日賜准專利,至感為禱。Therefore, the present invention is novel, progressive and can be used in industry. It should meet the patent application requirements of my country's patent law. I file an invention patent application in accordance with the law. I pray that the bureau will grant the patent as soon as possible. I sincerely pray.
惟以上所述者,僅為本發明之較佳實施例而已,並非用來限定本發明實施之範圍,舉凡依本發明申請專利範圍所述之形狀、構造、特徵及精神所為之均等變化與修飾,均應包括於本發明之申請專利範圍內。However, the above-mentioned ones are only preferred embodiments of the present invention, and are not used to limit the scope of the present invention. For example, all equal changes and modifications are made according to the shape, structure, characteristics and spirit described in the scope of the patent application of the present invention. , should be included in the patent application scope of the present invention.
S1~S4:步驟流程S1~S4: Step process
第1圖:其係本發明之一實施例之步驟流程圖。Fig. 1: It is a flowchart of the steps of one embodiment of the present invention.
S1~S4:步驟流程 S1~S4: Step process
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