TWI489489B - Decontaminator and treatment method for radioactive waste - Google Patents
Decontaminator and treatment method for radioactive waste Download PDFInfo
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本發明係有關於一種放射性廢料的除污方法，特別是指一種能有效降低放射性廢料污染核種活度之處理方法及其處理劑。 The invention relates to a method for decontaminating radioactive waste, in particular to a treatment method capable of effectively reducing the activity of radioactive waste contaminated nuclear species and a treatment agent thereof.
放射性廢料係指放射性廢水、廢氣和固體廢物，其主要來自核工業、核電廠、放射性醫療、以及核能應用的科學研究等。隨著原子能工業發展和放射性同位素日趨廣泛應用，放射性廢料日趨增多，如不經處理或處理不當而外排，會使環境遭受放射性污染，不僅影響動植物的生長，惡化水體，且危害人體健康，甚至對後代產生不良影響。 Radioactive waste refers to radioactive waste water, waste gas and solid waste, mainly from the nuclear industry, nuclear power plants, radiological health, and scientific research in nuclear energy applications. With the development of the atomic energy industry and the widespread use of radioisotopes, radioactive waste is increasing. If it is discharged without treatment or improper treatment, it will cause radioactive pollution to the environment, affecting not only the growth of animals and plants, but also the deterioration of water bodies and harm to human health. Have an adverse effect on future generations.
習知的放射性廢料處理方法為稀釋分散、濃縮貯存以及回收利用，然放射性廢料經濃縮後之廢物貯存只是暫時性措施，存在著不安全原素，必須將放射性廢液或濃縮物等廢物轉化成為穩定的固化體，才能安全地予以轉運、貯存和處置。又放射性廢料處置包括對放射性排出物的控制處置(稀釋處置)和廢物的最終處置，其中放射性排出物(液體、氣體)向環境中稀釋排放時必須控制在正式規定的排放標準以下，以管制含放射性物質(如氣體或液體)之排放，如我國行政院原子能委員會於1970年即發布「游離輻射防護安全標準」，規範核種活度(單位為貝克，Becquevel,Bq)管制限值；而放射性廢料最終處置意味著不再需要人工管理，不考慮將廢物再回取的可能，因此，為防止放射性廢料對自然環境和人類的危害，須將它與生物圈很好地隔離，令處置中的放射物質逐漸衰退，其危害性經極長久的時間後始會消失。 The conventional methods for treating radioactive waste are dilution, concentration, storage and recycling. However, the storage of waste after concentration of radioactive waste is only a temporary measure. There are unsafe elements, and waste such as radioactive waste or concentrate must be converted into A stable solidified body can be safely transported, stored and disposed of. The disposal of radioactive waste includes the control and disposal of radioactive effluents (dilution disposal) and the final disposal of waste. The radioactive effluent (liquid, gas) must be controlled below the officially stipulated emission standards when diluted to the environment. Emissions of radioactive materials (such as gases or liquids), such as the Atomic Energy Commission of the Executive Yuan of China, issued the "Safety Standard for Free Radiation Protection" in 1970, regulating the regulatory activities (in Beck, Becquevel, Bq) regulatory limits; Final disposal means no manual management is required, and the possibility of recycling waste is not considered. Therefore, in order to prevent the harmful effects of radioactive waste on the natural environment and human beings, it must be well isolated from the biosphere, so that the radioactive substances in disposal Gradually decline, its harmfulness will disappear after a very long time.
就以上之情況而言，實有需要開發經濟有效的放射性廢料處理方法，可以快速將放射性廢料的活度(或總活度)削減至較低的狀況，甚至降低至放射性廢料管制標準值以下。 In the above case, there is a need to develop a cost-effective radioactive waste treatment method that can quickly reduce the activity (or total activity) of radioactive waste to a lower level or even below the radioactive waste control standard.
為尋求經濟有效的放射性廢料處理方法，發明人在研發「高濃度含氟廢水處理劑及其處理方法(發明專利申請案號TW101148588)」時，由其利用某些中藥材與天然礦石混合物處理高濃度含氟廢水的實施例獲得啟發：若能變更相關中藥材配方，經燉煮後所得的濾液，對放射性廢棄物及廢水的放射性活度是否具有某種程度的去除效率。發明人於是仿照燉煮中藥的方法，研究出一種特別的放射性廢料除污劑及其處理方法，可將放射性活度較高的放射性廢料處理至放射性活度相對較低的狀態；由於本發明之除污劑組成複雜，其詳細降低放射性廢料放射性活度的原理機制尚非十分清楚，但本發明之除污劑送交行政院原子能委員會核能研究所進行除污測試，將除污劑加入放射性污染廢土中，經處理後之廢土放射性活度消除4%，過濾後之濾液無放射性污染；又本發明之除污劑加入放射性污染廢水中，經處理後之廢水放射性活度消除1~13%。雖然測試結果所得到的放射性活度消除率不高，但本發明經實證確實可消除廢棄物及廢水放射性活度的結果，相較於習知技術卻是具有新穎性及進步性，尤其本發明放射性廢料除污劑所採用的原料均是便宜的中藥材，大幅降低放射性廢料除污劑製造成本，可直接降低產業放射性廢棄物及廢水處理成本。以下將依次說明本發明之放射性廢料除污劑組成、製造方法及放射性廢料處理方法。 In order to find a cost-effective method for treating radioactive waste, the inventors have developed a high-concentration fluorine-containing wastewater treatment agent and its treatment method (Invention Patent Application No. TW101148588), which utilizes a mixture of certain Chinese herbal medicines and natural ore. The example of the concentration of fluorine-containing wastewater was inspired: if the relevant Chinese herbal medicine formula can be changed, the filtrate obtained after stewing has a certain degree of removal efficiency for the radioactive waste and wastewater activity. The inventor then developed a special radioactive waste decontaminating agent and a treatment method thereof according to the method of stewing traditional Chinese medicine, and can treat the radioactive waste with higher radioactivity to a state with relatively low radioactivity; The composition of the decontaminant is complicated, and the principle mechanism of reducing the radioactivity of the radioactive waste is not fully understood. However, the decontaminant of the present invention is sent to the Nuclear Energy Research Institute of the Atomic Energy Commission of the Executive Yuan for decontamination testing, and the decontaminant is added to the radioactive contamination. In the waste soil, the radioactivity of the treated waste soil is eliminated by 4%, and the filtered filtrate is free of radioactive contamination; and the decontaminant of the present invention is added to the radioactive contaminated wastewater, and the treated radioactive activity is eliminated 1~13 %. Although the radioactivity elimination rate obtained by the test result is not high, the present invention proves that the result of waste and wastewater radioactivity can be eliminated, and is novel and advanced compared with the prior art, especially the present invention. The raw materials used in the radioactive waste decontaminants are cheap Chinese herbal medicines, which greatly reduce the manufacturing cost of radioactive waste decontaminants, and can directly reduce the cost of industrial radioactive waste and wastewater treatment. Hereinafter, the composition, manufacturing method and radioactive waste disposal method of the radioactive waste detergent of the present invention will be sequentially described.
本發明之放射性廢料除污劑，其主要技術特徵在於該除污劑係由中藥材組合而成，該中藥材組合係至少選自於下列25種中藥材物質所構成之群組：欖仁樹、紅花、厚朴、天麻、黃蓮、山藥、麻黃、半夏、丁香、芍藥、海帶、核桃、地瓜葉、海芙蓉、肉桂粉、阿波羅、棕櫚、油麻菜籽、向日葵、茶樹、香蕉、榕亞屬、南瓜、檸檬及仙人掌。以放射性廢料除污劑組合物之重量百分比為100%，其主要技術特徵在於該除污劑至少包含欖仁樹重量百分比1~4.2%、紅花重量百分比0.5~4.5%、厚朴重量百分比1.5~4.1%、天麻重量百分比2~4.1%、黃蓮重量百分比1.5~4.3%、山藥重量百分比1.2~4.2%、麻黃重量百分比0.8~4.1%、半夏重量百分比1.2~4%、丁香重量百分比0.8~4.1%、芍藥重量百分比1.2~4.1%、海帶重量百分比0.5~4.1%、核桃重量百分比1.2~4%、地瓜葉重量百分比1~4.2%、海芙蓉重 量百分比1.3~4.1%、肉桂粉重量百分比0.5~4.3%、阿波羅重量百分比1.5~4%、棕櫚重量百分比1~4.1%、油麻菜籽重量百分比2~4.3%、向日葵重量百分比2~4.2%、茶樹重量百分比1.5~4.1%、香蕉重量百分比2.4~4.4%、榕亞屬重量百分比2~4%、南瓜重量百分比2~4.2%、檸檬重量百分比1.5~4.2%，其餘重量百分比為仙人掌。 The main technical feature of the radioactive waste decontaminating agent of the present invention is that the decontaminating agent is composed of a combination of Chinese herbal medicines, and the Chinese herbal medicine combination is at least selected from the group consisting of the following 25 Chinese herbal medicine substances: Terminalia , safflower, magnolia, gastrodia, yellow lotus, yam, ephedra, pinellia, clove, peony, kelp, walnut, sweet potato leaf, sea hibiscus, cinnamon powder, apollo, palm, linseed, sunflower, tea tree, Bananas, genus, pumpkins, lemons and cacti. The weight percentage of the radioactive waste desiccant composition is 100%, and the main technical feature thereof is that the decontaminant comprises at least 1% to 4.2% by weight of Terminalia, 0.5% to 4.5% by weight of safflower, and 1.5% by weight of Magnolia. 4.1%, Tianma weight percentage 2~4.1%, Huanglian weight percentage 1.5~4.3%, Yam weight percentage 1.2~4.2%, ephedra weight percentage 0.8~4.1%, Pinellia weight percentage 1.2~4%, lilac weight percentage 0.8 ~4.1%, weight percentage of peony 1.2-4.1%, kelp weight percentage 0.5~4.1%, walnut weight percentage 1.2~4%, sweet potato leaf weight percentage 1~4.2%, Haifulong heavy Amount percentage 1.3~4.1%, cinnamon powder weight percentage 0.5~4.3%, Apollo weight percentage 1.5~4%, palm weight percentage 1~4.1%, oilseed rape seed weight percentage 2~4.3%, sunflower weight percentage 2~4.2 %, tea tree weight percentage 1.5~4.1%, banana weight percentage 2.4~4.4%, 榕 subgenus weight percentage 2~4%, pumpkin weight percentage 2~4.2%, lemon weight percentage 1.5~4.2%, and the remaining weight percentage is cactus.
本發明放射性廢料除污劑之製造方法，其步驟包含：(a)將中藥材分別於粉碎機中進行粉碎1~30分鐘，使得到粒徑在1mm以下之中藥材，當作摻配之細粉原料；(b)以放射性廢料除污劑之重量百分比為100%，取欖仁樹重量百分比1~4.2%、紅花重量百分比0.5~4.5%、厚朴重量百分比1.5~4.1%、天麻重量百分比2~4.1%、黃蓮重量百分比1.5~4.3%、山藥重量百分比1.2~4.2%、麻黃重量百分比0.8~4.1%、半夏重量百分比1.2~4%、丁香重量百分比0.8~4.1%、芍藥重量百分比1.2~4.1%、海帶重量百分比0.5~4.1%、核桃重量百分比1.2~4%、地瓜葉重量百分比1~4.2%、海芙蓉重量百分比1.3~4.1%、肉桂粉重量百分比0.5~4.3%、阿波羅重量百分比1.5~4%、棕櫚重量百分比1~4.1%、油麻菜籽重量百分比2~4.3%、向日葵重量百分比2~4.2%、茶樹重量百分比1.5~4.1%、香蕉重量百分比2.4~4.4%、榕亞屬重量百分比2~4%、南瓜重量百分比2~4.2%、檸檬重量百分比1.5~4.2%，其餘重量百分比為仙人掌，放入混拌機中；(c)將上述混拌機中之中藥材粉末，進行充分混拌1~60分鐘，獲得組成均勻之組合物後，即成為粉狀放射性廢料除污劑。 The method for manufacturing a radioactive waste decontaminating agent according to the present invention comprises the steps of: (a) pulverizing the Chinese medicinal material in a pulverizer for 1 to 30 minutes, respectively, so that the medicinal material having a particle diameter of 1 mm or less is used as a blending fine. (b) 100% by weight of radioactive waste decontaminant, 1~4.2% by weight of Terminalia, 0.5~4.5% by weight of safflower, 1.5~4.1% by weight of Magnolia, and 100% by weight of Tianma 2~4.1%, Huanglian weight percentage 1.5~4.3%, yam weight percentage 1.2~4.2%, ephedra weight percentage 0.8~4.1%, Pinellia weight percentage 1.2~4%, lilac weight percentage 0.8~4.1%, peony weight Percentage 1.2~4.1%, kelp weight percentage 0.5~4.1%, walnut weight percentage 1.2~4%, sweet potato leaf weight percentage 1~4.2%, Haifulong weight percentage 1.3~4.1%, cinnamon powder weight percentage 0.5~4.3%, Abo Luo weight percentage 1.5~4%, palm weight percentage 1~4.1%, oilseed rape seed weight percentage 2~4.3%, sunflower weight percentage 2~4.2%, tea tree weight percentage 1.5~4.1%, banana weight percentage 2.4~4.4%榕 subgenus weight percentage 2~4%, pumpkin weight percentage 2~4.2% The weight percentage of lemon is 1.5~4.2%, and the remaining weight percentage is cactus, which is put into the mixing machine; (c) the Chinese medicinal material powder in the above mixing machine is thoroughly mixed for 1~60 minutes to obtain a composition with uniform composition. After that, it becomes a detergent for powdered radioactive waste.
本發明態樣之一為粉狀之放射性廢料除污劑，該粉狀組合物之優點易於保存，又為了實際應用之方便性，本發明另一態樣為液狀放射性廢料除污劑，其製造方法可由前述步驟(c)所製造的粉狀放射性廢料除污劑放入燉煮鍋中，再加入適量的水，其中粉狀放射性廢料除污劑與水的重量比為1：2~1：10；再將燉煮鍋內物質加熱升溫至沸騰後，維持95~110℃，持續燉煮30分鐘至2小時；最後經固液分離程序，移除固體物，即得液狀放射性廢料除污劑。此外本發明之液狀放射性廢料除污劑液之另一製造方法，亦可直接使用未粉碎前之25種中藥材組合物(其各別中藥成份之重量比 等同粉狀放射性廢料除污劑各別中藥成份之重量比)替代粉狀放射性廢料除污劑，然後依前述液狀放射性廢料除污劑之製造方法製得功效相當的液狀除污劑。 One aspect of the present invention is a powdery radioactive waste decontaminating agent, the advantages of the powdery composition are easy to preserve, and for practical convenience, another aspect of the present invention is a liquid radioactive waste decontaminating agent. The manufacturing method can be prepared by the step (c) of the powdered radioactive waste decontaminant into a stew pot, and then adding an appropriate amount of water, wherein the weight ratio of the powder radioactive waste desiccant to water is 1:2~1 :10; then heat the material in the stew pot to boiling, maintain 95 ~ 110 ° C, continue to cook for 30 minutes to 2 hours; finally through the solid-liquid separation process, remove the solids, that is, liquid radioactive waste Stain. In addition, in another method for producing the liquid radioactive waste decontaminating liquid of the present invention, it is also possible to directly use 25 kinds of Chinese herbal medicine compositions before the pulverization (the weight ratio of the respective traditional Chinese medicine ingredients) Corresponding to the weight ratio of the respective traditional Chinese medicine components of the powdered radioactive waste decontaminant), the powdery radioactive waste decontaminating agent is replaced, and then the liquid detergent is used according to the manufacturing method of the liquid radioactive waste decontaminant.
本發明之液狀放射性廢料除污劑除可應用於降低或消除放射性廢料中放射性核種活度之污染程度，茲就放射性廢棄物及廢水之除污處理方法分述如下： The liquid radioactive waste decontaminant of the present invention can be applied to reduce or eliminate the pollution degree of the radioactive nuclear activity in the radioactive waste. The decontamination treatment method of the radioactive waste and the waste water is described as follows:
A.放射性廢棄物處理方法 A. Radioactive waste treatment method
放射性廢棄物處理方法係在反應槽設備中，藉由將液狀放射性廢料除污劑加入被污染之放射性廢棄物中，經攪拌、靜置及固液分離等處理單元後，所得濾液之放射性活度低於管制標準(可直接排放)，而處理後所得固體物之放射性活度可得到某種程度的降低量，其步驟包含：(a)首先將待處理之放射性廢棄物導入反應槽內，再加入適量液狀放射性廢料除污劑，其中放射性廢棄物與除污劑重量比為200：1~1：2；(b)利用攪拌器將反應槽內所含之物質充分攪拌1~60分鐘使其混合均勻；(c)然後靜置6小時至30天；(d)最後經固液分離程序，排除液體，即得處理後放射性核種污染活性降低之廢棄物。 The radioactive waste treatment method is carried out in a reaction tank apparatus by adding a liquid radioactive waste decontaminant to the contaminated radioactive waste, and after stirring, standing, solid-liquid separation and the like, the radioactive activity of the obtained filtrate The degree is lower than the control standard (which can be directly discharged), and the activity of the solid obtained after the treatment can be reduced to some extent. The steps include: (a) first introducing the radioactive waste to be treated into the reaction tank. Then add appropriate amount of liquid radioactive waste decontaminant, wherein the weight ratio of radioactive waste to decontaminant is 200:1~1:2; (b) stir the material contained in the reaction tank with a stirrer for 1~60 minutes. It is evenly mixed; (c) then allowed to stand for 6 hours to 30 days; (d) Finally, the solid-liquid separation procedure is used to remove the liquid, that is, the waste having reduced radioactive nuclear species polluting activity after treatment.
B.放射性廢水處理方法 B. Radioactive wastewater treatment method
放射性廢水處理方法係在反應槽設備中，藉由將液狀放射性廢料除污劑加入被污染之放射性廢水中，經攪拌及靜置等處理單元後，所得混合液體之放射性活度低可得到某種程度的降低量，其步驟包含：(a)首先將待處理之放射性廢水導入反應槽內，再加入適量液狀放射性廢料除污劑，其中含氟廢水量與除污劑重量比為200：1~1：2；(b)利用攪拌器將反應槽內所含之物質充分攪拌1~60分鐘使其混合均勻；(c)然後靜置6小時至30天，即得處理後放射性核種污染活性降低之廢水。 The radioactive waste water treatment method is in the reaction tank equipment, by adding the liquid radioactive waste decontaminant to the contaminated radioactive waste water, and after stirring and resting the treatment unit, the radioactive activity of the obtained mixed liquid is low to obtain a certain The step of reducing the degree includes: (a) first introducing the radioactive waste water to be treated into the reaction tank, and then adding an appropriate amount of liquid radioactive waste decontaminant, wherein the ratio of the amount of the fluorine-containing waste water to the decontaminant is 200: 1~1:2; (b) stir the material contained in the reaction tank with a stirrer for 1~60 minutes to make it evenly mixed; (c) then let stand for 6 hours to 30 days, then the radioactive nuclear pollution after treatment Waste water with reduced activity.
10‧‧‧中藥材原料 10‧‧‧Chinese herbal medicine raw materials
12‧‧‧粉碎 12‧‧‧ smash
14‧‧‧粉狀放射性廢料除污劑 14‧‧‧Powdered radioactive waste decontaminant
15‧‧‧水 15‧‧‧ water
20‧‧‧摻配 20‧‧‧ blending
30‧‧‧加熱升溫 30‧‧‧heating up
40‧‧‧控溫燉煮 40‧‧‧Warm temperature stew
50‧‧‧固液分離 50‧‧‧ Solid-liquid separation
55‧‧‧藥渣固體 55‧‧‧Dregnose solids
60‧‧‧液狀放射性廢料除污劑 60‧‧‧ Liquid radioactive waste decontaminant
70‧‧‧待處理之放射性廢棄物 70‧‧‧ Radioactive waste to be disposed of
75‧‧‧待處理之放射性廢水 75‧‧‧ Radioactive wastewater to be treated
80‧‧‧攪拌混合 80‧‧‧ Mixing and mixing
90‧‧‧靜置 90‧‧‧Stay
95‧‧‧濾液 95‧‧‧ filtrate
97‧‧‧放射性活度削減後之廢棄物 97‧‧‧Recycling waste after radioactivity reduction
99‧‧‧放射性活度削減後之廢水 99‧‧‧ Wastewater after reduction in radioactivity
第一圖 粉狀放射性廢料除污劑製造流程 The first picture of the powder radioactive waste decontaminant manufacturing process
第二圖 液狀放射性廢料除污劑製造流程 The second picture of the liquid radioactive waste decontaminant manufacturing process
第三圖 放射性廢棄物處理流程 Figure III Radioactive waste treatment process
第四圖 放射性廢水處理流程 The fourth picture of the radioactive wastewater treatment process
本發明之技術特徵及優點，在配合第一圖至第四圖之說明，並佐以數個較佳實施例之測試結果，將可使在此技術領域具有通常知識者可清楚明白。 The technical features and advantages of the present invention, as well as the description of the first to fourth figures, together with the test results of several preferred embodiments, will be apparent to those of ordinary skill in the art.
本發明粉狀及液狀放射性廢料除污劑之製造流程，參閱第一圖及第二圖，其步驟包含：(a)將中藥材(10)分別於粉碎機中進行粉碎(12)1~30分鐘，使得到粒徑在1mm以下之中藥材粉末，當作摻配之細粉原料；(b)進行摻配(20)，以放射性廢料除污劑之重量百分比為100%，取欖仁樹重量百分比1~4.2%、紅花重量百分比0.5~4.5%、厚朴重量百分比1.5~4.1%、天麻重量百分比2~4.1%、黃蓮重量百分比1.5~4.3%、山藥重量百分比1.2~4.2%、麻黃重量百分比0.8~4.1%、半夏重量百分比1.2~4%、丁香重量百分比0.8~4.1%、芍藥重量百分比1.2~4.1%、海帶重量百分比0.5~4.1%、核桃重量百分比1.2~4%、地瓜葉重量百分比1~4.2%、海芙蓉重量百分比1.3~4.1%、肉桂粉重量百分比0.5~4.3%、阿波羅重量百分比1.5~4%、棕櫚重量百分比1~4.1%、油麻菜籽重量百分比2~4.3%、向日葵重量百分比2~4.2%、茶樹重量百分比1.5~4.1%、香蕉重量百分比2.4~4.4%、榕亞屬重量百分比2~4%、南瓜重量百分比2~4.2%、檸檬重量百分比1.5~4.2%，其餘重量百分比為仙人掌，放入混拌機中；(c)將上述混拌機中之中藥材粉末，進行充分攪拌混合(80)1~60分鐘，獲得組成均勻之組合物，即為粉狀放射性廢料除污劑(14)；(d)將粉狀放射性廢料除污劑(14)放入燉煮鍋中，再加入適量的水(15)，其中粉狀放射性廢料除污劑與水的重量比為1：2~1：10；(e)再將燉煮鍋內物質加熱升溫(30)至沸騰後，維持95~110℃，持續燉煮(40)30分鐘至2小時； (f)最後經固液分離(50)程序，移除藥渣固體(55)後，即得液狀放射性廢料除污劑(60)。 The manufacturing process of the powdery and liquid radioactive waste decontaminating agent of the present invention is referred to the first figure and the second figure, and the steps thereof include: (a) pulverizing the Chinese medicinal material (10) in a pulverizer (12) 1~ 30 minutes, so that the particle size of 1mm or less of the medicinal material powder, as a blended fine powder raw material; (b) blending (20), with the radioactive waste decontaminant weight percentage of 100%, take Terminalia Tree weight percentage 1~4.2%, safflower weight percentage 0.5~4.5%, Magnolia weight percentage 1.5~4.1%, gastrodia weight percentage 2~4.1%, yellow lotus weight percentage 1.5~4.3%, yam weight percentage 1.2~4.2%, Ephedrine weight percentage 0.8~4.1%, Pinellia weight percentage 1.2~4%, lilac weight percentage 0.8~4.1%, peony weight percentage 1.2~4.1%, kelp weight percentage 0.5~4.1%, walnut weight percentage 1.2~4%, Sweet potato leaf weight percentage 1~4.2%, sea hibiscus weight percentage 1.3~4.1%, cinnamon powder weight percentage 0.5~4.3%, Apollo weight percentage 1.5~4%, palm weight percentage 1~4.1%, oilseed rape seed weight percentage 2~4.3%, sunflower weight percentage 2~4.2%, tea tree weight percentage 1.5~4.1%, banana weight The ratio is 2.4~4.4%, the weight percentage of the subgenus is 2~4%, the weight percentage of pumpkin is 2~4.2%, the weight percentage of lemon is 1.5~4.2%, and the remaining weight percentage is cactus, which is put into the mixer; (c) The medicinal material powder in the above mixing machine is thoroughly stirred and mixed (80) for 1 to 60 minutes to obtain a composition having a uniform composition, that is, a powdery radioactive waste decontaminating agent (14); (d) a powdery radioactive waste material The decontaminant (14) is placed in a stew pot, and then an appropriate amount of water (15) is added, wherein the weight ratio of the powdered radioactive waste desiccant to water is 1:2 to 1:10; (e) the stew is further The material in the skillet is heated and heated (30) to boiling, maintained at 95~110 ° C, and continuously stewed (40) for 30 minutes to 2 hours; (f) Finally, after the solid residue separation (50) procedure, the solid residue (55) is removed, and the liquid radioactive waste decontaminant (60) is obtained.
A.本發明放射性廢棄物處理方法，請參閱第三圖，該處理方法係在反應槽設備中，藉由將液狀放射性廢料除污劑加入被污染之放射性廢棄物中，經攪拌、靜置及固液分離等處理單元後，所得濾液之放射性活度低於管制標準(可直接排放)，而所得固體物之放射性活度可得到某種程度的降低量，其步驟包含：(a)首先將待處理之放射性廢棄物(70)導入反應槽內，再加入適量液狀放射性廢料除污劑(60)，其中放射性廢棄物與除污劑重量比為200：1~1：2；(b)利用攪拌器將反應槽內所含之物質充分攪拌混合(80)1~60分鐘使其混合均勻；(c)然後靜置(90)6小時至30天；(d)最後經固液分離(50)程序，排除液體濾液(95)，即得放射性活度削減後之廢棄物(97)。 A. The method for treating radioactive waste according to the present invention, please refer to the third figure, which is added to the contaminated radioactive waste by adding the liquid radioactive waste detergent to the reaction tank equipment, stirring and standing. After the treatment unit such as solid-liquid separation, the activity of the obtained filtrate is lower than the control standard (which can be directly discharged), and the activity of the obtained solid matter can be reduced to some extent, and the steps include: (a) first Introducing the radioactive waste (70) to be treated into the reaction tank, and then adding an appropriate amount of liquid radioactive waste decontaminant (60), wherein the weight ratio of the radioactive waste to the decontaminant is 200:1~1:2; Using a stirrer, the contents of the reaction tank are thoroughly stirred and mixed (80) for 1 to 60 minutes to be uniformly mixed; (c) then allowed to stand (90) for 6 hours to 30 days; (d) finally separated by solid-liquid separation (50) Procedure, excluding liquid filtrate (95), that is, waste with reduced activity (97).
B.本發明放射性廢水處理方法，請參閱第四圖，該處理方法係在反應槽設備中，藉由將放射性廢料除污劑加入被污染之放射性廢水中，經攪拌及靜置等處理單元後，所得液體之放射性活度低可得到某種程度的降低量，其步驟包含：(a)首先將待處理之放射性廢水(75)導入反應槽內，再加入適量液狀放射性廢料除污劑(60)，其中放射性廢水量與除污劑重量比為200：1~1：2；(b)利用攪拌器將反應槽內所含之物質充分攪拌混合(80)1~60分鐘使其混合均勻；(c)然後靜置(90)6小時至30天，即得放射性活度削減後之廢水(99)。 B. The method for treating the radioactive waste water of the present invention, please refer to the fourth figure, which is carried out in the reaction tank equipment by adding the radioactive waste decontaminant to the contaminated radioactive waste water, stirring and standing after the treatment unit The low activity of the obtained liquid can be reduced to some extent. The steps include: (a) first introducing the radioactive waste water (75) to be treated into the reaction tank, and then adding an appropriate amount of liquid radioactive waste detergent ( 60), wherein the ratio of the amount of radioactive waste water to the concentration of the decontaminant is 200:1 to 1:2; (b) using a stirrer, the substance contained in the reaction tank is thoroughly stirred and mixed (80) for 1 to 60 minutes to be uniformly mixed. (c) Then, it is allowed to stand for (90) for 6 hours to 30 days, that is, the wastewater after the activity reduction (99) is obtained.
取經粉碎(粒徑1mm以下)之欖仁樹、紅花、厚朴、天麻、黃蓮、山藥、麻黃、半夏、丁香、芍藥、海帶、核桃、地瓜葉、海芙蓉、肉桂粉、阿波羅、棕櫚、油麻菜籽、向日葵、茶樹、香蕉、榕亞屬、南瓜、檸檬及仙人掌等25種中藥材為原料，首先將此等中藥材原料粉末各別取200g，再將其混合均勻，使成為粉狀放射性廢料除污劑，然後取2500g粉 狀放射性廢料除污劑放入反應槽中，再加入自來水7,500mL，然後加熱至沸騰時，控制水溫於95~110℃，繼續燉煮1hr，且控制蒸發水量於2,500~5,000mL之間，再經固液分離移除固體後，所得之濾液，即成為液狀放射性廢料除污劑測試樣本(該除污劑樣本編號為WT-A)。 Trichoderma sinensis, safflower, magnolia, gastrodia elata, yam, yam, ephedra, pinellia, clove, peony, kelp, walnut, sweet potato leaf, sea hibiscus, cinnamon powder, Apollo 25 kinds of Chinese herbal medicines such as palm, linseed, sunflower, tea tree, banana, medlar, pumpkin, lemon and cactus are used as raw materials. First, take 200g of these raw materials of Chinese herbal medicine, and mix them evenly. Make a powdery radioactive waste decontaminant, then take 2500g powder The radioactive waste decontaminant is placed in the reaction tank, and then 7,500 mL of tap water is added, and then heated to boiling, the water temperature is controlled at 95-110 ° C, the stew is continued for 1 hr, and the amount of evaporated water is controlled between 2,500 and 5,000 mL. After the solid is removed by solid-liquid separation, the obtained filtrate becomes a liquid radioactive waste decontaminant test sample (the decontaminant sample number is WT-A).
取行政院原子能委員會核能研究所廢棄物處理廠之放射性廢土(污染核種為Cs-137，污染比活度為13.7Bq/g)為測試樣本一(樣本編號為WW-A)；取自於行政院原子能委員會核能研究所廢棄物處理廠之第一種放射性污染廢水(污染核種為Cs-137及Co-60，其中Cs-137污染比活度為7.02Bq/ml，Co-60污染比活度為32.4Bq/ml)為測試樣本二(樣本編號為WW-B)；取自於行政院原子能委員會核能研究所廢棄物處理廠之第二種放射性污染廢水(污染核種為Cs-137及Sr-90，其中Cs-137污染比活渡為170Bq/ml，Sr-90污染比活度為4060Bq/ml)為測試樣本三(樣本編號為WW-C)，測試樣本放射性核種污染比活度檢測結果如表一。 Take the radioactive waste soil of the waste treatment plant of the Nuclear Energy Research Institute of the Executive Yuan Atomic Energy Commission (contaminated nuclear species is Cs-137, the specific activity of pollution is 13.7Bq/g) as test sample 1 (sample number is WW-A); The first type of radioactive polluted wastewater from the Waste Treatment Plant of the Nuclear Energy Research Institute of the Atomic Energy Commission of the Executive Yuan (contaminated nuclear species are Cs-137 and Co-60, of which the specific activity of Cs-137 is 7.02 Bq/ml, and the specific gravity of Co-60 pollution The degree is 32.4Bq/ml) for test sample 2 (sample number is WW-B); the second radioactive contaminated wastewater from the waste treatment plant of the Nuclear Energy Research Institute of the Atomic Energy Commission of the Executive Yuan (contaminated nuclear species are Cs-137 and Sr) -90, wherein the Cs-137 pollution ratio is 170 Bq/ml, the Sr-90 pollution specific activity is 4060 Bq/ml) is the test sample 3 (sample number is WW-C), and the test sample radioactive nuclear pollution specific activity detection The results are shown in Table 1.
Sr-90分析方法採用中低強度放射性物質中Sr-89、Sr-90放化分析操作方法：本發明實施例之實驗係以美國Eichrom公司研發上市之Sr.Spec樹脂進行鍶純化，其後以閃爍計數儀將水溶液樣品直接量測(Cerenkov counting)，由純化後的總溶液中Y-90的生長，及Sr-90、Sr-89的衰變導致計數率的變化來計算Sr-90、Sr-89的活度。 Sr-90 analysis method uses Sr-89 and Sr-90 radiochemical analysis in medium and low intensity radioactive materials. The experimental method of the present invention is carried out by purifying the Sr. Spec resin developed by Eichrom Corporation of the United States, and then The scintillation counter directly measures the aqueous solution (Cerenkov counting), and calculates the Sr-90 and Sr- from the growth of the purified Y-90 in the total solution and the decay of the Sr-90 and Sr-89. 89 activity.
Cs-137、Co-60分析方法採用加馬能譜分析儀：加馬能譜分析主要是利用核種衰變時放出特性能階之幅射線，鑑定出加馬能譜分布的特性，以確定釋出此特性能階之核種。當進入鍺偵檢器的輻射線，在外加電場作用下產生電子--電洞對經兩端電極收集，再經過前置放大器可輸出與在鍺結晶中產生電荷量成比例高度的信號，經放大器使脈衝信號加強，再依脈衝高度值類別收集，如此便可以脈衝振幅大小與能量成比例關係來分析不同幅射能量之核種。 The analysis method of Cs-137 and Co-60 adopts the Gamma spectrum analyzer: the analysis of the addition spectrum of the horse is mainly to use the amplitude ray of the special performance when the nucleus decays, and to identify the characteristics of the distribution spectrum of the gamma to determine the release. The nuclear species of this special performance level. When entering the radiation of the 锗 detector, an electron is generated by the applied electric field--the hole is collected by the electrodes at both ends, and then the preamplifier can output a signal proportional to the amount of charge generated in the crystallization of the ruthenium. The amplifier boosts the pulse signal and collects it according to the pulse height value category, so that the pulse magnitude can be proportional to the energy to analyze the nuclear species of different radiation energies.
本發明之除污劑對放射性廢土(含Cs-137核種)除污效果測試步驟說明如下： The test procedure of the decontamination effect of the decontamination agent of the invention on the radioactive waste soil (including Cs-137 nuclear species) is as follows:
1.精稱放射性廢土(樣本編號WW-A)50克，污染核種為Cs-137。 1. Finely called radioactive waste soil (sample number WW-A) 50 grams, the contaminated nuclear species is Cs-137.
2.計測放射性污染廢土(樣本編號WW-A)之放射性活度。 2. Measure the radioactivity of radioactive contaminated waste soil (sample number WW-A).
3.取本發明除污劑100ml，將之與放射性廢土(樣本編號WW-A)混合， 並攪拌3分鐘。 3. Take 100 ml of the detergent of the present invention and mix it with radioactive waste soil (sample number WW-A). Stir for 3 minutes.
4.靜置72小時。 4. Let stand for 72 hours.
5.混合後之放射性廢土過濾分離。 5. The mixed radioactive waste soil is separated by filtration.
6.分別計測過濾液及固體之放射性活度。 6. Measure the radioactivity of the filtrate and solid separately.
取自於行政院原子能委員會核能研究所廢棄物處理廠之放射性污染廢土(樣本編號WW-A)，污染核種為Cs-137，污染比活度為13.7Bq/g，放射性污染廢土共50克，故放射性總活度為685Bq，經添加本發明之除污劑100ml於放射性污染廢土，混合攪3分鐘，並靜置72小時後，過濾之，得固體80克，液體70ml，計測固體之放射性比活度8.2Bq/g，固體之放射性總活度為656Bq，液體之放射性比活度為小於LLD值(儀器最低可測值)，液體之放射性總活度為小於LLD值(儀器最低可測值)。除污劑對放射性廢土除污效果測試結果如表二。 The radioactive contaminated waste soil (sample No. WW-A) from the Waste Treatment Plant of the Nuclear Energy Research Institute of the Atomic Energy Commission of the Executive Yuan, the pollution nuclear species is Cs-137, the specific activity of pollution is 13.7 Bq/g, and the radioactive waste waste soil is 50. Gram, the total activity of radioactivity is 685Bq, 100ml of the decontaminant of the invention is added to the radioactive contaminated waste soil, mixed and stirred for 3 minutes, and allowed to stand for 72 hours, then filtered to obtain 80 g of solid, 70 ml of liquid, and the solid is measured. The specific activity of radioactivity is 8.2Bq/g, the total activity of solid radioactivity is 656Bq, the specific activity of liquid radioactivity is less than LLD value (the lowest measurable value of the instrument), and the total activity of liquid radioactivity is less than LLD value (lowest instrument) Measurable value). The test results of the decontamination effect of the decontaminant on the radioactive waste soil are shown in Table 2.
由表二得知本發明之除污劑，加入放射性污染廢土後，由放射性總活度由685Bq降至656Bq，放射性活度消除約4%，另污染核種Cs-137在本發明之除污劑加入後，亦無自放射性污染廢土中將染核種Cs-137淬取出來，由過濾之濾液無法檢測出核種Cs-137得以驗證。 It is known from Table 2 that the detergent of the present invention is added to the radioactive contaminated waste soil, and the total activity of the radioactivity is reduced from 685 Bq to 656 Bq, the activity is eliminated by about 4%, and the contaminated nuclear species Cs-137 is decontaminated in the present invention. After the addition of the agent, the Cs-137 was not extracted from the radioactive contaminated waste soil, and the nuclear Cs-137 could not be detected by the filtered filtrate.
本發明之除污劑對放射性廢水(含Cs-137 & Co-60核種)除污效果測試步驟說明如下： The test procedure of the decontamination effect of the decontamination agent of the invention on the radioactive waste water (including Cs-137 & Co-60 nuclear species) is as follows:
1.取放射性廢水(樣本編號WW-B)25ml，污染核種Cs-137、Co-60。 1. Take 25ml of radioactive wastewater (sample No. WW-B), polluting nuclear species Cs-137, Co-60.
2.計測放射性污染廢水(樣本編號WW-B)之放射性活度。 2. Measure the radioactivity of radioactive contaminated wastewater (sample No. WW-B).
3.取本發明除污劑25ml，將之與放射性廢水(樣本編號WW-B)25ml混合，並攪拌30秒。 3. 25 ml of the detergent of the present invention was taken, mixed with 25 ml of radioactive waste water (sample No. WW-B), and stirred for 30 seconds.
4.靜置24小時。 4. Let stand for 24 hours.
5.計測混合液之放射性活度。 5. Measure the radioactivity of the mixture.
取自於行政院原子能委員會核能研究所廢棄物處理廠之放射性污染廢水(樣本編號WW-B)，污染核種為Cs-137、Co-60，其中Cs-137污染比活度為7.02Bq/g，Co-60污染比活度為32.4Bq/g，量取上述放射性污 染廢水(樣本編號WW-B)25ml，並添加本發明之除污劑25ml，混合攪拌30秒，靜置24小時，計測總體積為50ml之廢水活度，Co-60污染比活度為14.1Bq/g，Cs-137污染比活度為3.11Bq/g。除污劑對放射性廢水Cs-137及Co-60除污效果測試結果如表三。 Radioactive contaminated wastewater (sample No. WW-B) from the Waste Treatment Plant of the Nuclear Energy Research Institute of the Atomic Energy Commission of the Executive Yuan. The contaminated nuclear species are Cs-137 and Co-60, and the specific activity of Cs-137 is 7.02 Bq/g. , Co-60 pollution specific activity is 32.4Bq / g, the above radioactive contamination Dyeing wastewater (sample No. WW-B) 25ml, and adding 25ml of the decontaminating agent of the present invention, mixing and stirring for 30 seconds, standing for 24 hours, measuring the total volume of wastewater of 50 ml, the specific activity of Co-60 pollution is 14.1. The specific activity of Bq/g and Cs-137 was 3.11 Bq/g. The test results of the decontamination effect of the decontaminant on the radioactive waste water Cs-137 and Co-60 are shown in Table 3.
由表三得知本發明之除污劑，消除放射性污染廢水之污染核種Cs-137及Co-60活度具有貢獻，Co-60放射性總活度由810Bq降至705Bq，去除約13%之放射性污染，Cs-137放射性總活度由175.5Bq降至155.5Bq，去除約11%之放射性污染。 It is known from Table 3 that the decontaminant of the present invention contributes to the elimination of the contaminated nuclear species Cs-137 and Co-60 activities of the radioactive contaminated wastewater, and the total activity of the Co-60 radioactivity is reduced from 810 Bq to 705 Bq, and about 13% of the radioactivity is removed. Pollution, the total activity of Cs-137 radioactivity decreased from 175.5Bq to 155.5Bq, removing about 11% of radioactive contamination.
本發明之除污劑對放射性廢水(含Cs-137 & Sr-90核種)除污效果測試步驟說明如下： The test procedure of the decontamination effect of the decontamination agent of the invention on the radioactive waste water (including Cs-137 & Sr-90 nuclear species) is as follows:
1.取放射性廢水(樣本編號WW-C)25ml，污染核種Cs-137、Sr-90。 1. Take 25ml of radioactive wastewater (sample No. WW-C) and contaminate nuclear species Cs-137 and Sr-90.
2.計測放射性污染廢水(樣本編號WW-C)之放射性活度。 2. Measure the radioactivity of radioactive contaminated wastewater (sample No. WW-C).
3.取本發明除污劑25ml，將之與放射性廢水(樣本編號WW-C)25ml混合，並攪拌30秒。 3. Take 25 ml of the detergent of the present invention, mix it with 25 ml of radioactive waste water (sample No. WW-C), and stir for 30 seconds.
4.靜置24小時。 4. Let stand for 24 hours.
5.計測混合液之放射性活度。 5. Measure the radioactivity of the mixture.
取自於行政院原子能委員會核能研究所廢棄物處理廠之放 射性污染廢水(樣本編號WW-C)，污染核種為Cs-137、Sr-90，其中Cs-137污染比活渡為170Bq/ml，Sr-90污染比活度為4,060Bq/ml，量取上述放射性污染廢水25ml，並添加本發明之除污劑25ml，混合攪伴30秒，靜置24小時，計測總體積為50ml之廢水活度，Cs-137污染比活渡為83.6Bq/ml，Sr-90污染比活度為2,000Bq/ml。除污劑對放射性廢水Cs-137及Sr-90除污效果測試結果如表四。 Taken from the Waste Treatment Plant of the Nuclear Energy Research Institute of the Atomic Energy Commission of the Executive Yuan The radioactive wastewater (sample No. WW-C), the polluted nuclear species are Cs-137, Sr-90, wherein the Cs-137 pollution ratio is 170 Bq/ml, and the Sr-90 pollution specific activity is 4,060 Bq/ml. Take 25 ml of the above radioactive contaminated wastewater, add 25 ml of the decontaminant of the present invention, mix and stir for 30 seconds, let stand for 24 hours, measure the wastewater activity with a total volume of 50 ml, and the Cs-137 pollution ratio is 83.6 Bq/ml. The specific activity of Sr-90 contamination is 2,000 Bq/ml. The test results of the decontamination effect of the decontaminant on the radioactive wastewater Cs-137 and Sr-90 are shown in Table 4.
由表四得知本發明之除污劑，可消除放射性污染廢水之污染核種Cs-137及Sr-90的活度，Sr-90由101,500Bq降至100,000Bq，去除約1%之放射性污染，Cs-137由4,250Bq降至4,180Bq，去除約2%之放射性污染。 It is known from Table 4 that the decontaminant of the present invention can eliminate the activity of polluting nuclear species Cs-137 and Sr-90 of radioactive contaminated wastewater, and Sr-90 is reduced from 101,500 Bq to 100,000 Bq, and about 1% of radioactive contamination is removed. Cs-137 was reduced from 4,250 Bq to 4,180 Bq, removing about 2% of the radioactive contamination.
由前述具體實施例可知，本發明之除污劑，加入待處理之放射性污染廢土中，廢土經處理後之放射性核種污染活度消除4%，且過濾後之濾液無放射性污染。又本發明之除污劑，加入待處理之放射性污染廢水中，廢水經處理後之放射性核種污染活度消除1~13%。 It can be seen from the foregoing specific examples that the decontaminating agent of the present invention is added to the radioactive contaminated waste soil to be treated, and the radioactive nuclear species pollution activity of the treated waste soil is eliminated by 4%, and the filtrate after filtration is free from radioactive contamination. Further, the decontaminant of the present invention is added to the radioactive contaminated wastewater to be treated, and the radioactive nuclear pollution activity of the treated wastewater is eliminated by 1 to 13%.
雖然本發明已以較佳實例揭露如上，但並非用以限定本發明，任何熟習此項技藝者，在不脫離本發明之精神和範圍內，當可做更動 與潤飾，因此本發明之保護範圍當視申請專利範圍所界定者為準。 The present invention has been described above by way of a preferred example, and is not intended to limit the invention, and may be modified by those skilled in the art without departing from the spirit and scope of the invention. And the scope of protection of the present invention is subject to the definition of the scope of the patent application.
綜上所述，本發明可供產業上利用，且經查相關前案，本發明揭露以中藥材原料組合而成之放射性廢料除污劑及其應用於放射性廢料之處理方法，於申請前均未見於刊物或已公開使用，屬於在放射性廢料處理領域之創新技術，又本發明具體實施後，可將原本活度較高之放射性廢 料處理至活度相對較低之放射性廢料，實非所屬技術領域中具有通常知識者依申請前之先前技術所能輕易完成，充分展現本發明具有新穎性及進步性；同時本發明之放射性廢料除污劑原料均取自價格便宜之中藥材，可大幅降低產業放射性廢料處理成本，增加產業競爭力，期望 貴局能早日准予專利，造福國內相關產業。 In summary, the present invention is available for industrial use, and the related inventions have been examined. The present invention discloses a radioactive waste decontaminating agent which is a combination of Chinese herbal medicine raw materials and a method for treating the same. It is not found in the publication or has been used publicly. It belongs to the innovative technology in the field of radioactive waste treatment, and after the specific implementation of the present invention, the radioactive waste with higher activity can be used. The treatment of the radioactive waste to a relatively low activity can be easily accomplished by those having ordinary knowledge in the prior art according to the prior art prior to the application, and fully demonstrates the novelty and progress of the present invention; Decontaminant raw materials are taken from cheaper intermediates, which can greatly reduce the cost of industrial radioactive waste treatment and increase industrial competitiveness. We hope that your company will grant patents as soon as possible to benefit domestic related industries.
60‧‧‧液狀放射性廢料除污劑 60‧‧‧ Liquid radioactive waste decontaminant
70‧‧‧待處理之放射性廢棄物 70‧‧‧ Radioactive waste to be disposed of
20‧‧‧摻配 20‧‧‧ blending
80‧‧‧攪拌混合 80‧‧‧ Mixing and mixing
90‧‧‧靜置 90‧‧‧Stay
50‧‧‧固液分離 50‧‧‧ Solid-liquid separation
95‧‧‧濾液 95‧‧‧ filtrate
97‧‧‧放射性活度削減後之廢棄物 97‧‧‧Recycling waste after radioactivity reduction
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| JP2014013540A JP5839624B2 (en) | 2013-04-08 | 2014-01-28 | Radioactive material adsorbent, method for producing the same, and treatment method using the same |
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| US5045273A (en) * | 1988-08-24 | 1991-09-03 | Siemens Aktiengesellschaft | Method for chemical decontamination of the surface of a metal component in a nuclear reactor |
| RU2428203C1 (en) * | 2010-05-13 | 2011-09-10 | Государственное образовательное учреждение высшего профессионального образования "Санкт-Петербургский государственный технологический институт (технический университет)" | Method of herbal crude drug decontamination |
| TW201131581A (en) * | 2009-12-04 | 2011-09-16 | Areva Np Gmbh | Method for surface-decontamination |
| CN102206918A (en) * | 2011-04-07 | 2011-10-05 | 安徽师范大学 | Multipurpose Chinese herbal medicine type ironing liquid and preparation method thereof |
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| JP2013130574A (en) * | 2011-11-22 | 2013-07-04 | Kunio Goto | Radioactive decontamination method and decontamination agent therefor |
| JP2013150962A (en) * | 2012-01-26 | 2013-08-08 | Series:Kk | Method for producing flocculation auxiliary agent for purifying contaminated water |
| JP2013221830A (en) * | 2012-04-16 | 2013-10-28 | Okayama Univ | Radioactive substance removing agent |
| JP6236608B2 (en) * | 2012-11-16 | 2017-11-29 | 国立大学法人佐賀大学 | Adsorption and removal of cesium from water |
| JP2014145718A (en) * | 2013-01-30 | 2014-08-14 | Asia Biosystems Kk | Decontamination liquid, decontamination method, and plaster for decontamination |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US5045273A (en) * | 1988-08-24 | 1991-09-03 | Siemens Aktiengesellschaft | Method for chemical decontamination of the surface of a metal component in a nuclear reactor |
| TW201131581A (en) * | 2009-12-04 | 2011-09-16 | Areva Np Gmbh | Method for surface-decontamination |
| RU2428203C1 (en) * | 2010-05-13 | 2011-09-10 | Государственное образовательное учреждение высшего профессионального образования "Санкт-Петербургский государственный технологический институт (технический университет)" | Method of herbal crude drug decontamination |
| CN102206918A (en) * | 2011-04-07 | 2011-10-05 | 安徽师范大学 | Multipurpose Chinese herbal medicine type ironing liquid and preparation method thereof |
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| JP5839624B2 (en) | 2016-01-06 |
| TW201440073A (en) | 2014-10-16 |
| JP2014202748A (en) | 2014-10-27 |
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