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사용후핵연료의 연소도 변화에 따른 산화 및 OREOX 공정에서 핵분열기체 방출 특성
박근일,조광훈,이정원,박장진,양명승,송기찬,Park, Geun-Il,Cho, Kwang-Hun,Lee, Jung-Won,Park, Jang-Jin,Yang, Myung-Seung,Song, Kee-Chan 한국방사성폐기물학회 2007 방사성폐기물학회지 Vol.5 No.1
Quantitative analysis on release behavior of the $^{85}Kr\;and\;^{14}C$ fission gases from the spent fuel material during the voloxidation and OREOX process has been performed. This thermal treatment step in a remote fabrication process to fabricate the dry-processed fuel from spent fuel has been used to obtain a fine powder The fractional release percent of fission gases from spent fuel materials with burn-up ranges from 27,000 MWd/tU to 65,000 MWd/tU have been evaluated by comparing the measured data with these initial inventories calculated by ORIGEN code. The release characteristics of $^{85}Kr\;and\;^{14}C$ fission gases during the voloxidation process at $500^{\circ}C$ seem to be closely linked to the degree of conversion efficiency of $UO_2\;to\;U_3O_8$ powder, and it is thus interpreted that the release from grain-boundary would be dominated during this step. The high release fraction of the fission gas from an oxidized powder during the OREOX process would be due to increase both in the gas diffusion at a temperature of $500^{\circ}C$ in a reduction step and in U atom mobility by the reduction. Therefore, it is believed that the fission gases release inventories in the OREOX step come from the inter-grain and inter-grain on $UO_2$ matrix. It is shown that the release fraction of $^{85}Kr\;and\;^{14}C$ fission gases during the voloxidation step would be increased as fuel burn-up increases, ranging from 6 to 12%, and a residual fission gas would completely be removed during the OREOX step. It seems that more effective treatment conditions for a removal of volatile fission gas are of powder formation by the oxidation in advance than the reduction of spent fuel at the higher temperature.
고연소도 경수로 사용후핵연료의 열처리에 따른 세슘 방출거동
박근일,조광훈,이정원,박장진,양명승,송기찬,Park, Geun-Il,Cho, Kwang-Hun,Lee, Jung-Won,Park, Jang-Jin,Yang, Myung-Seung,Song, Kee-Chan 한국방사성폐기물학회 2007 방사성폐기물학회지 Vol.5 No.1
The dynamic release behavior of Cs from high burn-up spent PWR fuel was experimentally performed under the conditions of a thermal treatment process such as voloxidation and sintering conditions. In voloxidation process, influence of the oxidation and reduction atmosphere on the Cs release characteristic using fragment type of spent fuel heated up to $1,500^{\circ}C$ was compared. In sintering process, temperature history effect on Cs release behavior was evaluated using green pellet under 4% $H_2/Ar$ environment. Temperature range for complete Cs release from spent fuel fragment under voloxidation condition was about $800^{\circ}C{\sim}1,200^{\circ}C$, but that of green pellet under the reduction atmosphere was $1,100^{\circ}C{\sim}1,400^{\circ}C$. Key parameters on Cs release behavior from spent fuel was powder formation as well as the diffusion rate of Cs compound to grain boundary and fuel surface.
유로퓸 고용(固溶) 우라늄산화물(酸化物)의 황화반응(黃化反應) 특성(特性)
이재원,박근일,이정원,Lee, Jae Won,Park, Geun Il,Lee, Jung Won 한국자원리싸이클링학회 2013 資源 리싸이클링 Vol.22 No.3
희토류산화물인 $Eu_2O_3$, 우라늄산화물인 $UO_2$ 및 $U_3O_8$, $Eu_2O_3$와 우라늄산화물의 혼합물에 대한 선택적 황화반응을 조사한 후에, $(U,Eu)O_2$ 및 $(U,Eu)_3O_8$와 같은 Eu 고용 우라늄산화물, Eu 고용 우라늄산화물의 고온 산화열처리 상분리 생성물인 Eu 농도가 높은 $(U,Eu)_4O_9$와 $U_3O_8$의 혼합상에 대한 황화반응 특성을 $400-800^{\circ}C$에서 조사하였다. $Eu_2O_3$ 및 우라늄산화물의 혼합물의 경우에는 $450^{\circ}C$에서 Eu와 우라늄 산화물간의 반응이 없이 $Eu_2O_3$만 $Eu_3S_4$로 전환되었다. $(U,Eu)_3O_8$ 및 $(U,Eu)O_2$에서는 반응온도 $600^{\circ}C$까지는 우라늄산화물과 동일한 황화반응 거동을 보였으며, $800^{\circ}C$에서는 Eu 농도가 높은 $(U,Eu)S_x$과 ${\alpha}-US_2$ 상이 생성되었다. 고온 산화열처리 상분리 생성물은 $600^{\circ}C$에서 $(U,Eu)S_x$과 UOS 상이 생성되었다. 상분리 생성물을 환원하여 얻은 Eu 농도가 높은 $(U,Eu)O_2$와 $UO_2$의 혼합상은 $450^{\circ}C$에서 $(U,Eu)O_2$은 산황화물인 (U,Eu)OS로 전환되고 $UO_2$는 반응하지 않았다. Sulfurization reaction characteristics of $Eu_2O_3$, uranium oxides($UO_2$, $U_3O_8$), mixture of $Eu_2O_3$ and uranium oxides, Eu-doped uranium oxides($(U,Eu)O_2$, $(U,Eu)_3O_8$), and phase-separated products prepared by HOX (High temperature OXidation) of $(U,Eu)O_2$ were investigated in the temperature range from 400 to $800^{\circ}C$. Only $Eu_2O_3$ in the mixture of $Eu_2O_3$ and uranium oxides was converted into $Eu_3S_4$ by sulfurization reaction at $450^{\circ}C$ without reaction between them. Sulfurization reaction behavior of $(U,Eu)_3O_8$ and $(U,Eu)O_2$ up to $600^{\circ}C$ was similar to $U_3O_8$ and $UO_2$, respectively, while they were sulfurized into Eu-rich $(U,Eu)S_x$ and ${\alpha}-US_2$ at $800^{\circ}C$. In the sulfurization of RE-rich $(U,Eu)_4O_9$ and $U_3O_8$ prepared by high temperature oxidation, it was confirmed that RE-rich $(U,Eu)S_x$ and UOS phases were formed at $600^{\circ}C$. For Eu-rich $(U,Eu)O_2$ and $UO_2$ prepared by reduction of HOX products, it was identified that Eu-rich (U,Eu)OS was formed at $450^{\circ}C$ by sulfurization of Eu-rich $(U,Eu)O_2$, while $UO_2$ remained unreacted.
단일 전해액 배출만을 가지는 pH조절용 연속식 이온 교환막 전해 시스템의 개발과 그 특성
김광욱,김인태,박근일,이일희,Kim Kwang-Wook,Kim In-Tae,Park Geun-Il,Lee Eil-Hee 한국방사성폐기물학회 2005 방사성폐기물학회지 Vol.3 No.4
In order to produce only a pH-controlled solution without discharging any unwanted solution, this work has developed a continuous electrolytic system with a pH-adjustment reservoir being placed before an ion exchange membrane-equipped electrolyzer, where as a target solution was fed into the pH-adjustment reservoir, some portion of the solution in the pH-adjustment reservoir was circulated through the cathodic or anodic chamber of the electrolyzer depending on the type of the ion exchange membrane used, and some other portion of the solution in the pH-adjustment reservoir was discharged from the electrolytic system through the other counter chamber with its pH being controlled. The internal circulation of the pH-adjustment reservoir solution through the anodic chamber in the case of using a cation exchange membrane and that through the cathodic chamber in the case of using an anion exchange membrane could make the solution discharged from the other counter chamber effectively acidic and basic, respectively. The phenomena of the pH being controlled in the system could be explained by the electro-migration of the ion species in the solution through the ion exchange membrane under a cell potential difference between anode and cathode and its consequently-occurring non-charge equilibriums and electrolytic water- split reactions in the anodic and cathodic chambers.
Laser Welding of Seal Tube for Instrumented Irradiation Fuel Test
김수성,이철용,김웅기,박근일,고진현,서준석,Kim Soo-Sung,Lee Chul-Yong,Kim Woong-Ki,Park Geun-Il,Koh Jinh-Yun,Seo Jun-Seok The Korean Welding and Joining Society 2005 대한용접·접합학회지 Vol.23 No.6
This work was carried out to obtain sound welds and to select a most suitable binary metal joint among three different dissimilar binary metal combinations such as Zr-4/Ta, Mo/Ta and Ti/Ta(seal tube/sensor sheath) joints fur the instrumented nuclear fuel irradiation test. To do this, Taguchi experimental method was employed to optimize the experimental data. In addition, metallography, micro-focus x-ray radiography and hardness test were conducted to examine the welds. From the weld bead appearance, penetration depth and bead width as well as weld defects standpoint, Zr-4/Ta joint is suggested for the circumferential joining between a seal tube and a sensor sheath. The optimized welding parameters based on Zr-4/Ta joint are suggested as well.
Surface Analysis Study on ZIRLO Cladding Hulls Oxidized at Low Temperatures
전민구,최용택,이창화,강권호,박근일,Jeon, Min Ku,Choi, Yong Taek,Lee, Chang Hwa,Kang, Kweon Ho,Park, Geun Il Korean Radioactive Waste Society 2014 방사성폐기물학회지 Vol.12 No.3
본 논문에서는 X선 광전자 분광법(X-ray photoelectron spectroscopy, XPS)을 이용하여 ZIRLO (ZIRconium Low Oxidation) 피복관의 표면 산화 거동을 연구하였다. 산화 시간 (10-336 시간, $500^{\circ}C$) 및 산화 온도 ($400-700^{\circ}C$, 10 시간)에 따른 산화 특성변화를 관찰하였다. XPS peak 분석 결과, $500^{\circ}C$에서 산화된 피복관의 산화 시간이 24 시간이 될 때 $ZrO_2$ peak가 11.86% 관찰되었으며, 이후 산화 시간이 길어질수록 $ZrO_2$의 비율이 17.93%까지 (336 시간) 증가하는 것이 확인되었다. 반면, 10 시간 산화된 피복관에서 5.68% 존재하던 ZrO 상은 산화 시간이 24 시간으로 늘어남에 따라 사라지는 것이 관찰되었다. 산화 온도 증가에 의한 영향 분석 결과에서는 산화 온도가 $400^{\circ}C$에서 500, 600, $700^{\circ}C$로 증가할 때 ZrO 상의 비율이 0% 부터 5.68, 8.31, 9.16%로 증가하는 것이 확인되었다. 이 때, $ZrO_2$ 상은 $700^{\circ}C$에서 산화된 시료에서만 관찰되었다. ZrO 상의 형성 메커니즘은 불명확하지만, 고온에서 공기 중의 수분과 Zr의 반응으로 인해 $Zr(OH)_4$ 상의 형성이 가속되는 것으로 예상된다. 본 논문에는 $500^{\circ}C$에서 산화된 ZIRLO 피복관과 이들의 염소화 반응 특성에 대한 논의도 포함되었으며, 염소화 반응 진행 가능성에 있어서 산화막의 두께가 중요한 역할을 하는 것으로 보여진다. Surface oxidation behavior of ZIRLO (ZIRconium Low Oxidation) hulls was investigated using an X-ray photoelectron spectroscopy (XPS) technique. The effects of oxidation time (10-336 h at $500^{\circ}C$) and temperature ($400-700^{\circ}C$ for 10 h) were studied. Deconvolution results of the hulls oxidized at $500^{\circ}C$ revealed that a $ZrO_2$ phase appeared after 24 h (11.86%), and an increase in the $ZrO_2$ ratio was observed when the hulls were oxidized for 336 h (17.93%). On the other hand, the ZrO phase which employed 5.68% in the 10 h oxidized sample disappeared when the oxidation time increased to 24 h. The XPS results also showed that an increase in the oxidation temperature resulted in an increase in the ratio of ZrO, which increased from 0 to 5.68, 8.31, and 9.16% when the oxidation temperature increased from 400 to 500, 600, and $700^{\circ}C$, respectively. $ZrO_2$ phase was observed only in the sample that was oxidized at $700^{\circ}C$. The mechanism of ZrO formation was not conclusive, but it was suggested that a formation of hydroxide might have been accelerated at elevated temperatures leading to a formation of a $Zr(OH)_4$ phase. The relationship between the surface oxidation status of the hulls oxidized at $500^{\circ}C$ and their chlorination reaction feasibility was discussed, and it was suggested that the thickness of the oxide layer is an important parameter that determines the chlorination reaction feasibility.