Eu(Ⅲ)和Am(Ⅲ)在Th4(PO4)4P2O7上的吸附行为

通过静态法研究了Am(Ⅲ)和Eu(Ⅲ)在Th4(PO4)4P2O7上的吸附行为,主要包括吸附平衡时间、固液比、pH值、离子强度以及富里酸(FA)等因素对吸附的影响.实验结果表明,Am(Ⅲ)和Eu(Ⅲ)在Th4(PO4)4P2O7上的吸附具有相似的pH吸附曲线,pH值的变化对吸附的影响较大,吸附率在pH=2~5时出现剧增;在其他条件相同时,KNO3离子强度从0.01 mol/L增大到0.1 mol/L,吸附率随着离子强度的增大而减小.通过对比实验发现,FA对Am(Ⅲ)和Eu(Ⅲ)在Th4(PO4)4P2O7上的吸附具有促进作用.Am(Ⅲ)和Eu(Ⅲ)在Th4(PO4)4P2O7表面可能形成了表面络合物.吸附剂的表面特征及其吸附机理研究是进一步深入研究的重点.     

整合素素αⅤβ3受体显像剂18F标记RGD肽的研究进展

血管新生是肿瘤生长、转移过程中不可缺少的生物过程。整合素α_Ⅴβ₃受体在新生血管内皮细胞和多种肿瘤细胞表面高表达,在肿瘤血管新生中起着关键作用,目前已成为肿瘤诊断与治疗的一个重要靶点。精氨酸-甘氨酸-天冬氨酸（Arg-Gly-Asp, RGD）肽可特异性地与整合素α_Ⅴβ₃受体结合,¹⁸F标记的RGD肽类化合物PET显像可无创、动态地定量监测整合素α_Ⅴβ₃受体表达,在肿瘤早期诊断、疗效监测及抗血管新生评价上发挥着重要作用。本文就近年来国内外¹⁸F标记RGD 肽在肿瘤α_Ⅴβ₃受体显像中的研究进展作简要综述。     

乙异羟肟酸与Zr(Ⅳ),UO2+2配合物稳定常数的测定

对乙异羟肟酸(AHA)与Zr(Ⅳ), UO2 2的配位行为进行了初步研究,测定了AHA与Zr(Ⅳ), UO2 2配合物的稳定常数.结果表明,在HClO4体系中,AHA与Zr(Ⅳ), UO2 2分别发生三、二级配位,其稳定常数分别为:β1(Zr(Ⅳ))=(6.7±0.1)×1013,β2(Zr(Ⅳ)) =(1.8±0.1)×1025,β3(Zr(Ⅳ))=(3.8±0.3)×1035;β1(UO2 2)=(8.6±0.4)×107,β2(UO2 2)=(3.8±0.1)×1014.     

Am(Ⅲ)在Al2O3和石英上的吸附行为

研究了Am(Ⅲ)在Al2O3和石英上的吸附行为,探讨了水相pH值、总CO2-3和SO2-4浓度(1.0×10-3～2.0×10-1 mol/L)、腐殖酸和Am(Ⅲ)浓度等因素对吸附的影响,并对可能的吸附机理进行了分析,同时以1.0 mol/L HCl做为解吸剂,对吸附平衡后的固相进行了解吸实验.结果表明,随着水相pH值的升高,Am(Ⅲ) 在Al2O3和石英上的吸附分配比增大,水相的化学组分及其相应浓度增大对Am(Ⅲ)在石英上的吸附影响较明显;Am(Ⅲ)在Al2O3和石英上以界面配合物的形式吸附,且可用Freundlich吸附等温式描述;水相中腐殖酸浓度增大,Am(Ⅲ)在Al2O3和石英上的吸附降低.     

二氧化铀对CO和CO2的吸附热力学

采用静态吸附容量法,测定了温度273～303K、压力0～1kPa范围内,CO和CO₂在UO₂表面的吸附等温线,研究了CO和CO₂的吸附热力学性质。结果表明,Langmuir方程和Freundlich方程分别是描述CO和CO₂吸附的最优模型方程。CO₂的吸附强度明显高于CO的,实验条件下,CO和CO₂的最大吸附量分别为0.36和1.25μmol/g。CO的吸附热为26kJ/mol,表明吸附为物理吸附;CO₂的吸附热随吸附量增加而减小,当吸附量由0.3μmol/g增至0.8μmol/g时,吸附热由46kJ/mol降至37kJ/mol,表明吸附同时存在化学吸附和物理吸附。     

双羟基脲与HNO2的反应动力学及对Pu(Ⅲ)的稳定作用

研究了HClO4和HNO3体系中双羟基脲(DHU)与HNO2的反应动力学.结果表明,HClO4和HNO3体系下DHU与HNO2的反应动力学速率方程式均为-dc(HNO2)/dt=k·c(HNO2 )1·c(DHU )0·c(H+)-0.15,反应对DHU均呈零级.在HClO4体系下,θ=15 ℃, I=0.5 mol/kg时,反应速率常数k1=(2.37±0.04) mol0.15/(L0.15·min);在HNO3体系下,θ=10 ℃, I=0.5 mol/kg时,反应速率常数k2= (1.29±0.06) mol0.15/(L0.15·min)(n=8).同时考察了反应温度对反应速率的影响,结果表明,随着温度的升高, 反应速率均明显加快, HClO4和HNO3体系对应的反应活化能分别为68.2 kJ/mol和76.8 kJ/mol.在HClO4和HNO3体系中,随着离子强度的增加,氧化还原反应的表观速率常数k'均下降.过量的DHU在HNO3溶液中可以很好的稳定Pu(Ⅲ)48 h而不被氧化.     

Re/99Tcm(CO)3-EPBI与Aβ(1～40)结合能力的测定及生物分布

为发展锝-99m标记的阿尔茨海默病(Alzheimer's disease, AD)早期诊断显像药物,在荧光测定法基础上,建立了体外荧光法测定羰基铼配合物与Aβ_(1～40)淀粉样纤维结合的解离常数K_d的方法.同时,合成了配体2-(1-乙基苯并咪唑)吡啶(EPBI)及其铼的配合物Re(CO)_3Cl(EPBI),测定后者与体外缠结Aβ_(1～40)结合的解离常数Kd;采用直接标记法制备EPBI的[~(99)Tc~m(CO)_3]~+配合物,并研究配合物[~(99)Tc~m (CO)_3]~+-EPBI的理化性质及生物分布.结果表明,Re(CO)_3Cl(EPBI)与Aβ_(1～40)结合的解离常数K_d=13.3 μmol/L;正常小鼠体内生物分布研究表明,化合物[~(99)Tc~m (CO)_3]~+-EPBI的脑初始(2 min内)摄取值为(0.63±0.17)%ID/g(n=3),在脑内清除较快,120 min时,摄取值为(0.27±0.03)%ID/g(n=3).     

水溶液中新核心[99Tcm(CO)2(NO)]2+和[99Tcm(CO)2(NO)-L] (L=DTPA,EDTA,EHIDA)的制备

研究了水溶液中制备[99Tcm(CO)2(NO)-L](L=DTPA,EDTA,EHIDA)配合物的2种方法:(1) 由前体[99Tcm(CO)3-L]制备[99Tcm(CO)2(NO)-L];(2)由[99Tcm(CO)2(NO)(H2O)3]2+中间体制备[99Tcm(CO)2(NO)-L];并确定了最佳标记条件.TLC和HPLC结果表明,2种方法得到的配合物放化产率均在90%以上.初步建立了1套在水溶液中简单、高效制备新的[99Tcm(CO)2(NO)]2+类配合物的方法.+基团取代原三羰基锝配合物得到的[99Tcm (CO)2(NO)-L]配合物具有良好的体外稳定性,取代后的配合物脂溶性和电荷性质都发生了改变,为99Tcm放射性药物的研制开辟了新思路.     

利用X射线衍射技术分析LaNi5氚老化效应

利用覆膜法对长期贮存氚的LaNi_5进行了XRD分析.经过实验发现,老化后的LaNi_5的谱峰比新鲜的LaNi_5存在明显的展宽,而经过高温除He处理后,又恢复到新鲜的LaNi_5水准,氚衰变形成的~3He在晶格中居留并在其中形成部分位错亚结构,这可能是导致LaNi_5 XRD衍射峰宽化的主要原因.     

13C呼吸试剂D-木糖-U-13C5的合成

以D-葡萄糖-U-¹³C₆为起始原料,采用减碳法经双丙酮保护、选择性酸水解、氧化、还原和碱水解五步合成D-木糖-U-¹³C₅,总产率为38.6%（以D-葡萄糖-U-¹³C₆计）。对每步产物使用相应的气相色谱（GC）、气质联用仪（GC-MS）、液相色谱（HPLC）和液质联用仪（LC-MS）进行表征。分析结果表明,每步反应中的产物均为目的产物,同位素丰度和纯度都符合要求,最后一步的产物为D-木糖-U-¹³C₅,其¹³C丰度为99.1 % ,化学纯度为99.9%,符合¹³C呼吸试验的要求。     

在Na2CO3溶液中季铵盐萃取Zr机理的研究

用红外光谱分析和季铵盐萃取研究了Zr—DBP界面物在碳酸钠溶液中的溶解机理。结果表明,Zr—DBP界面物在碳酸钠溶液中生成了能溶于水的配合阴离子Zr(CO3)4^4-或ZrO(CO3)3^4-,Zr—DBP界面物溶解前后与纯HDBP的红外谱图相比,溶解液中DBP的P—O键的特征峰与纯HDBP的更为接近。说明界面物在溶解Na2CO3过程中,破坏了原有界面物的配合,DBP不再与Zr配合,而以自由离子形式存在。     

Influence of Ionization Degrees on Conversion of CO and CO_2 in Atmospheric Plasma near the Ground

A zero-dimensional model is used to study the processes of physical and chemical reactions in atmospheric plasma with different ionization degrees near the ground （0 km）. The temporal evolutions of CO, C02 and other main reactants （namely OH and O2）, which affect the conversion of CO and C02, are obtained for afterglow plasma with different initial values. The results show that the consumption rate of CO is largest when the initiM electron number density neo=1012 cm-3, i.e. the ionization degree is 0.000004%. The number density of CO2 is relatively small when neo=1016 cm-3, i.e. the ionization degree is 0.04%, whereas they are very close under the condition of other ionization degrees. Considering the total number densities of CO and C02 and the consumption rate of CO comprehensively, the best condition is neo=1013 cm-3, i.e. the ionization degree is 0.00004% for reducing the densities of CO and CO2 in the atmospheric plasma. The temporal evolutions of N＋, Ar＋, CO＋ and CO＋ are also shown, and the influences on the temporal evolutions of CO and C02 are analyzed with increasing ionization degree.     

HNO3氧化去除Np-Pu反萃液中的H2C2O4

研究了用HNO3 氧化去除TRPO流程反萃Np Pu的H2 C2 O4反萃液中H2 C2 O4的条件。 7 5mol·L-1HNO3 0 .3mol·L-1H2 C2 O4混合液于 90℃下蒸发 1 3 0h和 1 0 0℃下蒸馏回流 6h ,H2 C2 O4可完全分解去除 ;混合液中添加适量催化剂MnCO3 ,于 1 0 0℃下蒸发或蒸馏回流 ,H2 C2 O4分解加速 ,1～ 1 5h内H2 C2 O4完全分解。蒸发或蒸馏回流过程中产生的HNO2 把Np(Ⅳ )氧化为Np(Ⅴ )和Np(Ⅵ ) ,95 %以上的Pu保持Pu(Ⅳ )。     

侧线反馈对H2/HD/D2低温精馏分离的影响

为研究带侧线反馈的低温精馏氢同位素分离规律性,建立了带侧线反馈的低温精馏氢同位素分离计算方法,并以H2/HD/D2体系进行了计算分析.计算结果表明,侧线反馈对分离性能影响显著,再沸器中以D2为主,氘丰度可达到0.90,而无侧线反馈情况下,再沸器中以HD为主,氘丰度不超过0.50;有侧线反馈条件下,系统运行约40 h HD向D2的转化达到峰值,而在无侧线情况下,HD浓缩在40 h已达到饱和;当侧线采出比为1时,脱氘率最高.     

Tritium Separation by CO2 Laser Multiphoton Dissociation of Trifluoromethane

Integral system tests with the Cylindrical Core Test Facility (CCTF) were performed to investigate the effect of the initial clad temperature on the reflood phenomena in a PWRLOCA. The initial peak clad temperatures in these three tests were 871, 968 and 1,047 K, respectively. The feedback of the system on the core inlet mass flow rate was estimated to be little influenced by the variation of the initial clad temperature except for the first 20 s in the transient. The observed temperature rise from the reflood initiation was lower with the higher initial clad temperature. This qualitatively agreed with the results of the small scale forced feed reflood experiments. However, the magnitude of the temperature rise in CCTF was significantly low due to the high initial core inlet mass flow rate. Also observed were the multi-dimensional thermal behaviors for the three cases in the CCTF wide core. The analysis codes REFLA and TRAC reasonably predicted the effect of the initial clad temperature on the core thermo-hydraulics under the simulated core inlet flow conditions. However, the calculated temperature rise of the maximum powered rod based on the one-dimensional core analysis was higher than that of the average powered rod, which contradicts the tendency observed in CCTF tests.     

Behavior of Nitrogen Compounds in Radiation Field and Nuclear Reactor Systems

Formation of nitrogen compounds in N₂-H₂O systems under radiation was studied. A reaction scheme with 24 species and 73 reactions was proposed. Two trigger reactions for nitrogen atom generation: N₂ → 2N (g-value of 1.6 μmol per 1 kJ absorbed energy in N₂ molecules), and N₂+H₂O^*→NH₂+NO (κ=3.0×10⁹ S^?1·M^?1 at 298 K with activation energy of 34.4kJ/mol) were included.

Calculated results with the reaction scheme agreed within an error factor of two with ammonium formation rates from an aqueous solution with dissolved nitrogen and hydrogen gasses under γ-irradiation at temperatures of 288~473 K. The reaction scheme was also verified with BWR plant observations on nitric acid formation from in-leaked air under hydrogen water chemistry and ammonium injection tests.     

Radiation Treatment of Exhaust Gases, (XII) NO Removal in Moist NO-SO2-O2-N2 Mixtures Containing NH3

The NO removal by electron beam irradiation was studied in the moist NO-SO₂-O₂-N₂ mixtures containing NH₃. The NO removal was promoted markedly by addition of NH₃ and at the same time, SO₂ was removed. The formations of NO₂, N₂O, NH₄NO₃ and (NH₄)₂SO₄ were observed in the mixtures containing NH₃. The NO removal increased with H₂O and SO₂ concentrations and was hardly affected by the presence of 3–19.5% O₂. The degree of the NO_x(NO+NO₂) removal became larger with decreasing temperature in the range of 80–150°°C. The NO removal was independent of dose rate in the range of 3.1×10⁴–2.4×10⁶ rad/s. The promotion of the NO removal by addition of NH₃ is attributable to the effective decomposition of NO by NH₂ radical formed by the reaction of NH₃ with OH radical. The NO₂ yield decreased by addition of NH₃ and the N₂O yield increased.     

Numerical Simulation for Chemical Reactions of Actinide Elements in Aqueous Nitric Acid Solution

A computer code REACT incorporating 30 rate equations of reactions, i.e. radiolytic formation and decomposition of HNO₂, redox and disproportionation reactions, was developed to simulate behavior of actinide elements in the aqueous nitric acid solution. Main aspects of REACT code were explained briefly and then calculated results were compared with reported data to evaluate the model in the systems of radiolytic accumulation of HNO₂, stabilization process of Pu solution. The study showed that some radiolytic products other than HNO₂ would play a significant role and should be taken into account for precise simulation of very slow valency change of Pu in the neat Pu solution particularly with high radiation power density. Some examples of calculation were also shown for systems of reduction of Pp and Np by uranous or HAN and oxidation of Np (V) to Np (VI).