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Kafe 바로가기주관연구기관 | 한국원자력연구원 Korea Atomic Energy Research Institute |
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보고서유형 | 2단계보고서 |
발행국가 | 대한민국 |
언어 | 한국어 |
발행년월 | 2015-10 |
과제시작연도 | 2014 |
주관부처 | 미래창조과학부 Ministry of Science, ICT and Future Planning |
과제관리전문기관 | 한국연구재단 National Research Foundation of Korea |
등록번호 | TRKO201600010248 |
과제고유번호 | 1711013750 |
사업명 | 방사선기술개발사업 |
DB 구축일자 | 2016-10-08 |
키워드 | 발생장치.Ga-68.Ge-68.사이클로트론.방사성의약품.Generator.Ga-68.Ge-68.Cyclotron.Radiopharmaceutical. |
DOI | https://doi.org/10.23000/TRKO201600010248 |
30 MeV 사이클로트론을 활용해 모핵종인 68Ge를 생산하고 이를 지지체에 흡착시켜 일정시간 후에 딸핵종인 68Ga를 용출하여 PET용 방사성의약품의 개발에 활용할수 있는 68Ge/68Ga 발생장치의 개발과 용출된 68Ga 동위원소를 활용하는 기술 개발을 목표로 다음의 연구를 수행하였다.
○ 30MeV 사이클로트론용 68Ge 생산 표적 설계/제작 및 68Ge 생산
○ 표적으로부터
30 MeV 사이클로트론을 활용해 모핵종인 68Ge를 생산하고 이를 지지체에 흡착시켜 일정시간 후에 딸핵종인 68Ga를 용출하여 PET용 방사성의약품의 개발에 활용할수 있는 68Ge/68Ga 발생장치의 개발과 용출된 68Ga 동위원소를 활용하는 기술 개발을 목표로 다음의 연구를 수행하였다.
○ 30MeV 사이클로트론용 68Ge 생산 표적 설계/제작 및 68Ge 생산
○ 표적으로부터 68Ge 분리/정제 화학처리법 확립 (생산수율:1.26×10-2mCi/㎂h)
○ 68Ge 일상 생산을 위한 표적시스템 및 자동화기기 설계/제작
○ 68Ge/68Ga 발생장치 흡착제 후보물질 12종 개발 및 물성 분석
○ 안정동위원소 및 방사성동위원소(68Ge, 68Ga) 이용 흡착제 흡착/탈착능 평가
○ 4종 흡착제에 대한 누설평가(breakthrough) : 7.4×10-3 % ~ 2×10-4 %
○ 68Ga표지 흑색종 진단용 Benzamide 유도체 및 덴드리머 혼성체와 친수성 복합체의 합성/분석 및 생물학적 평가
Ⅳ. Result
1. Target development for 68Ge production and the production and the separation of 68Ge
natGa(p,xn)68Ge was selected as a nuclear reaction for the production of 68Ge.Based on the result of SRIM code simulation, proton energy was
Ⅳ. Result
1. Target development for 68Ge production and the production and the separation of 68Ge
natGa(p,xn)68Ge was selected as a nuclear reaction for the production of 68Ge.Based on the result of SRIM code simulation, proton energy was determined as 29 MeV at the first stage of research. Target for the test production was designed and fabricated according to this energy, and then, 68Ge was produced by using MC-50 cyclotron of KIRAMS and RFT-30 cyclotron of ARTI. According to the analysis result of test production, proton energy was changed to 26 ~ 27 MeV for the integrity of target. In addition, exclusive target irradiation station, transport system, and target treatment device were developed for the capsuled target. The property evaluation of various metals was also performed for the application to Ga encapsulation. Ti, Nb, and Mo foils were heated in the liquid Ga environment for 2 weeks. According to the result of scanning electron microscopy, a Nb foil showed the least amount of Ga adhesion while a Ti foil exhibited the most amount of Ga adhesion. Results of energy dispersive X-ray spectroscopy and X-ray diffraction analysis displayed that Ga just physically adhered to metal foils without any chemical bonding. Finally, result of X-ray photoelectron spectroscopy revealed that Nb was oxidized by heating in the liquid Ga while Mo was rather partially reduced. Both Nb and Mo can be candidates for the Ga encapsulation, but it is considered that Mo is better for the development of high-energy target for 68Ge production.
2. Separation and purification of 68Ge
Using stable isotopes (72Ge, 69Ga), condtion of 68Ge production was indirectly realized. As a result of back extraction method using acid solution, erupted solution was composed of Ge higher than 90% and Ga lower than 0.1%. It means that Ge was successfully separated. Based on this result, 68Ge separation process was performed. Proton-irradiated target was put in beaker, and then, heated. After irradiated solid target (natGa + 68Ge) was liquified, 68Ge was extracted by using 5 ml of 4 N HCl and 2 ml of 30% H2O2. 510 keV peak, corresponding to the annhilation energy of β+ produced for the decay of 68Ge, was observed.
3. Development of adsorbent for 68Ge/68Ga generator
In column adsorbent of 68Ge/68Ga generator, a long-lived parent radionuclide(t1/2=271 d) and its short-lived daughter radionuclide (t1/2=68min) make radiative equilibrium. In order to find much more suitable generator adsorbents, we carried out various adsorbents experiment. The ability of the adsorbent to adsorb various metal oxides, mineral and metal phosphate was investigated in order to evaluate the possibility of its use in germanium adsorption and gallium desorption. The adsorbents were fully characterized by spectroscopic analysis equipments. The plastic syringe (volume: 1.8 ㎖, height: 56 mm) chromatographic column fitted with polyethylene frit (polyethylene, pore: 20μm) at the bottom was packed with 200 mg of adsorbents. Germanium-68 solution (6 μCi/㎕) containing germanium and gallium impurities were passed through the metal oxide column at a flow rate of 1 ㎖/min and the effluent was collected. All radioactivity was measured by dosimeter. The selective TiO2, CeO2, Al/W/Ti and Zr(HPO4)2 based 68Ge/68Ga generator has been composed and evaluation. High purity of 68Ga elution was obtained with in 1 minute as a 1.0 ㎖ volume of 0.1N and 0.4 N HCl fractions. We were successfully achieved a high radio chemical purity and low breakthrough of 68Ge using the various adsorbents as the column material. These 68Ga/68Ga generator adsorbents have high potential for use in sources of PET radioisotopes.
4. Development of shield case for 68Ge/68Ga generator
For the shielding the 68Ge/68Ga generator, Pb and W were chosen and the generator was designed and fabricated. According to the results of MCNP analysis, 25mm(Pb) and 15mm(W) are enough for the legal transport regulation. In this research, shield case for the generator was design and manufactured with 40mm(Pb) and 30mm(W) conservatively.
5. Development of 68Ga labelled radiopharmaceuticals
68Ga-SCN-DOTA/NOTA-PCA (68Ga labelled benzamide derivative) was synthesized with a radiochemical yield of ~80% and a radiochemical purity of >97% by analytical HPLC. It showed stability with higher thatn 95% during the in vitro stability test of 2 h. The in vitro binding of 68Ga-benzamide derivatives to melanin and its cellular uptake demonstrated the selective uptake in melanin. In addition, the biodistribution and micro–PET imaging of benzamide derivatives in B16F10 tumor models showed the specific accumulation in melanoma. These results suggest that68Ga-SCN-DOTA-PCA would be a promising agent for melanoma diagnosis.
[ 68Ga ]nanocomposites were synthesized using Ga-68 after preparing nanocoreshell with DOTA-PAMAM dendrimer complex and NOTA-ctiric acid on the surface of Fe3O4 nanoparticles (NPs). The fabricated nanocomposites were characterized by NMR, XRD, MS, TEM, Zeta sizer etc. Radio-TLC and HPLC confirmed the formation of 68Ga-DOTA/NOTA complex. The size of as synthesized nanocomposites was 11.5 nm and after surface modification progresses, the size of NPs was gradually increased to 15.3 nm. The nanocomposites with stable gallium isotope showed excellent biocompatibility and [ 68Ga ]nanocomposites have high uptake on CT-26, SKBR-3, KB and A 549 cell line. The values of cellular uptake was attained a maximum of 9.764 % at 60 min for CT-26, 13.591 % at 120 min for SK-BR-3 cell line, 9.6133 % at 60 min for KB and 10.861 % at 120 min for A549. These detailed studies established that 68GaNHFCNP exhibits potential application for cancer contrast.
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