UiO-66-(COOH)2的合成及其对锂同位素吸附分离性能研究

为研究金属有机骨架材料对⁷Li的吸附分离性能,本研以水作为溶剂,四氯化锆和均苯四甲酸为起始原料,采用水热法合成金属有机骨架材料UiO-66-(COOH)₂,对合成材料的形貌、孔径、热稳定性等进行表征与分析;通过静态吸附实验探讨吸附时间、反应温度、溶液浓度对UiO-66-(COOH)₂锂离子吸附性能及同位素分离因子的影响;并对Li⁺浓度、⁶Li/⁷Li同位素丰度进行测定。结果表明,UiO-66-(COOH)₂可实现对锂的吸附以及⁷Li的分离,且在293 K Li₂CO₃溶液中,每0.05 g UiO-66-(COOH)₂对10 mL 0.05 mol/L Li₂CO₃进行4 h的静态吸附,最大吸附量Q为9.53 mg/g,分离因子S（⁷Li/⁶Li）为1.019 54。研究结果为⁷Li的分离提供了新途径。     

Measurement of the cross sections for the reactions Cr(n,2n)Cr, Zn(n,2n)Zn, Y(n,2n)Y and Zr(n,2n)Zr from 13.5 to 14.8 MeV

Cross section measurements for the reactions ⁵²Cr(n,2n)⁵¹Cr, ⁶⁶Zn(n,2n)⁶⁵Zn, ⁸⁹Y(n,2n)⁸⁸Y and ⁹⁶Zr(n,2n)⁹⁵Zr were carried out in the neutron energy range 13.47–14.79 MeV applying the activation technique. Neutrons were produced via the T(d,n)⁴He reaction, making use of the variation of neutron energy with the emission angle. The neutron fluences incident on the samples were determined relative to the well-evaluated cross section for the reaction ⁹³Nb(n,2n)^92mNb.

The induced γ-ray activities of the irradiated Zn, Zr and Y₂O₃ samples and their monitor foils were measured by means of a calibrated Ge(Li) γ-ray detector at the KFI, Debrecen. At the IRK, Vienna, relative γ-ray measurements using a high-purity Ge detector were combined with integral γ-ray counting by means of a NaI(TI) well-type detector on the Cr, Zn and Zr foils of highest activity and on some Nb monitor foils; integral γ-ray counting only was applied in the case of the Y₂O₃ samples. All necessary corrections were taken into account.

The results are compared to the corresponding results of cross section measurements published in the literature. The uncertainties obtained in this work are considerably smaller in most cases than the uncertainties given by other authors.     

离子液体/苯并15-冠-5浸渍XAD-7树脂萃取分离锂同位素

以XAD-7树脂为支撑担体制备了含有三种不同咪唑型离子液体([C_8mim][BF_4]、[C_8mim][PF_6]、[C_8mim][(SO_2CF_3)_2N])和萃取剂(苯并15-冠-5)的浸渍树脂,并用于锂同位素的萃取分离。浸渍树脂的红外和扫描电镜表征表明,离子液体成功负载到了树脂上;热重分析表明,该浸渍树脂具有良好的热稳定性。在水相初始pH=5.55时,浸渍树脂具有最佳萃取率。浸渍树脂在LiSCN溶液中具有较高的萃取率,而在CF_3COOLi溶液中呈现较大的单级分离因子,最大单级分离因子达到1.045±0.002。浸渍树脂的萃取平衡时间为2.5~3h。萃取热力学研究表明,该反应为自发过程,温度对体系的影响较小。~6Li富集于固相,~7Li富集在水相。该系列浸渍树脂易于再生,可循环使用。     

应用可调谐外腔半导体激光器测量锂同位素比率

采用中心波长固定的可调谐外腔半导体激光器作为光源,通过激光吸收光谱法对锂原子同位素比率进行测量。该方法利用PID温控器实现锂金属蒸发温度的控制和测量。采用激光斜入射的方式消除光路调试过程中产生的标准具效应。实验测量给出了6组不同腔体温度下⁶Li和⁷Li在671 nm附近的吸收光谱,通过对⁶LiD₁和⁷LiD₂吸收峰进行积分吸收计算,得到⁶Li/⁷Li同位素比率测量精度可达2.5%。     

Investigation of neutron converters for production of optically stimulated luminescence (OSL) neutron dosimeters using Al2O3:C

This paper presents the optically stimulated luminescence (OSL) properties of neutron dosimeters in powder and in the form of pellets prepared with a mixture of Al₂O₃:C and neutron converters. The neutron converters investigated were high density polyethylene (HDPE), lithium fluoride (LiF), lithium fluoride 95% enriched with ⁶Li (⁶LiF), lithium carbonate 95% enriched with ⁶Li (⁶Li₂CO₃), boric acid enriched with 99% of ¹⁰B and gadolinium oxide (Gd₂O₃). The proportion of Al₂O₃:C and neutron converter in the mixture was varied to optimize the total OSL signal and neutron sensitivity. The neutron sensitivity and dose-response were determined for the OSL dosimeters using a bare ²⁵²Cf source and compared to the response of Harshaw TLD-600 and TLD-700 dosimeters (⁶LiF:Mg,Ti and ⁷LiF:Mg,Ti). The results demonstrate the possibility of developing an OSL dosimeter made of Al₂O₃:C powder and neutron converter with a neutron sensitivity (defined as the ratio between the ⁶⁰Co equivalent gamma dose and the reference neutron absorbed dose) and neutron–gamma discrimination comparable to the TLD-600/TLD-700 combination. It was shown that the shape of the OSL decay curves varied with the type of the neutron converter, demonstrating the influence of the energy deposition mechanism and ionization density on the OSL process in Al₂O₃:C.     

压水堆主冷却剂中氚源项计算分析

压水堆主回路冷却剂流经堆芯时,水中固有及特加核素受中子辐照后会产生氚,氚几乎全部以气体和液体的形式排入环境,造成氚污染。因此,氚是压水堆辐射环境影响评价的主要关注内容之一。本文以AP1000为例,根据压水堆主回路冷却剂中氚的产生途径及其随时间的变化情况建立详细的计算模型,计算压水堆主回路冷却剂中的氚活度并分析各产氚途径对氚产生量的贡献。计算结果表明：主回路冷却剂中的氚主要来源于可溶性硼的中子活化和铀裂变,对氚产生量的贡献达80%以上;在⁷Li纯度为99.9%时,AP1000主回路中的年产氚量为5.23×10¹³ Bq,锂产氚量占总量的14.01%,随⁷Li纯度的增加,锂产氚量的贡献呈线性减小,在⁷Li纯度为99.99%时,锂产氚量占总量的3.18%。其他途径对氚的产生量贡献很小,可忽略。根据以上结果,可通过控制主回路冷却剂中添加的初始硼浓度、提高燃料包壳质量、增加LiOH中⁷Li的纯度等多种途径来降低主冷却剂中氚的产生量,从而减少氚对环境的放射性污染。     

Study of space-dependent fast-neutron spectra and tritium breeding ratio in different assemblies of Li, Li and natural Li

Using diffusion theory and the eigenfunction expansion method, a detailed space-dependent study of fast neutron spectra has been carried out in ⁷Li, ⁶Li and natural Li assemblies of dimensions 100 × 60 × 60 cm³ and 30 × 60 × 60 cm³. Values of total (space-averaged) tritium breeding ratio (TBR) have been obtained for these assemblies. BARC-892, a 27-group data-set was used for these calculations.

The results of TBR for the smaller assembly have been compared with the corresponding experimental and calculated values of Takahashi et al. (1984). We find that the present values of TBR are in reasonably good agreement with the above experimental results.     

The new nuclear reaction analysis facility at the Lund Nuclear Microprobe

A versatile system for the analysis of the light elements at a Nuclear Microprobe has been constructed. Special reactions for analysis of H (H(p,p)H), Li (⁷Li(p,)), B (¹¹B(p,)2) and F (¹⁹F(p,₁e⁻e⁺)¹⁶O)as well as the general techniques pNRA, PIXE and STIM are employed simultaneously. The set-up is mainly, but not only, intended for thin samples.     

Determination of sulphur and copper depth distribution in patina layers using nuclear reaction techniques

A method for Cu and S profiling in patina layers was developed by applying a combination of nuclear reaction analysis (NRA) and Rutherford backscattering spectroscopy (RBS). The copper profiling was performed by using the 1327 keV γ-ray deexciting the third excited state to the ground state of ⁶³Cu produced by the reaction ⁶³Cu(p,p^′γ)⁶³Cu. For the determination of sulphur the 2230 keV γ-ray was used deexciting the first excited state to the ground state of ³²S formed through the reaction ³²S(p,p^′γ)³²S, which exhibits three sharp resonances at projectile energies 3.094, 3.195 and 3.379 MeV. The relevant cross-sections were measured in the energy range between 3.0 and 3.7 MeV in steps of 20 keV at 125° to the incident proton beam direction. The technique was tested using artificially produced and natural copper patina layers. Supporting information on the depth distribution of the constituent elements of the patina samples was obtained by p-RBS (E_p: 1.5 MeV, θ: 160°).     

中子俘获反应截面在线测量技术研究

利用γ全吸收型4π BaF₂探测装置,对中子俘获反应截面进行了在线测量。基于HI-13串列加速器提供的脉冲化质子束,通过⁷Li(p,n) ⁷Be反应产生中子,构建了keV能区中子源实验条件,经屏蔽准直后的中子轰击样品,应用4π BaF₂装置在线测量(n,γ)反应复合核退激时释放的瞬发γ射线级联,测量了Au、C、Nb、空白等样品。通过计算⁹³Nb(n,γ)⁹⁴Nb和¹⁹⁷Au(n,γ)¹⁹⁸Au两个反应的截面数据比值并与文献数据比对,检验了4π BaF₂探测装置和(n,γ)反应截面在线测量技术,为在中国散裂中子源（CSNS）上顺利开展(n,γ)反应截面数据测量工作提供了技术支持。     

The cross section for the K(n,p)Ar reaction between 14.2 and 17.2 MeV

Activation techniques have been used to measure the cross section for the ⁴¹K(n,p)⁴¹Ar reaction between 14.2 and 17.2 MeV. Neutrons were produced by the ³H(d,n)⁴He reaction, and the mixed-power method was used to measure the neutron flux through the ²⁷Al(n,)²⁴Na reaction. The activated samples were counted for the 1294 keV, 1.827 h γ-activity of ⁴¹Ar and the 1369 keV, 15.03 h γ-activity of ²⁴Na using a 16% Ge(Li) detector and a 4096-channel analyzer. The cross sections for the ⁴¹K(n,p)⁴¹Ar reaction using the mixed-power method were found to be 53 ± 3 mbarn at 14.2 ± 0.2 MeV, 47 ± 3 mbarn at 15.2 ± 0.2 MeV, 41 ± 3 mbarn at 16.2 ± 0.2 MeV and 36 ± 4 mbarn at 17.2 ± 0.2 MeV. The associated-particle method was also used for measuring the neutron flux in order to check the mixed-powder result at 14.2 MeV. The average cross section for three associated-particle runs at 14.2 MeV was found to be 50 ± 3 mbarn which, within experimental error, agrees with the mixed-powder value.     

细胞尺度10B不均匀分布对细胞微剂量影响的计算与分析

硼中子俘获治疗已经成为当前治疗恶性黑色素瘤、头颈部肿瘤等恶性肿瘤的有效手段之一。¹⁰B在细胞尺度上不均匀分布将直接影响到对肿瘤细胞失活剂量的控制。为研究含硼化合物在细胞内空间上分布不同对靶区细胞微剂量的影响,本工作利用Monte-Carlo工具包开发了用于计算¹⁰B（n,α）⁷Li产生的α与⁷Li对靶区剂量的模拟程序α-Li Version 1.0。通过此程序,计算了2种细胞尺寸、8种α粒子能量、3种源分布方式的细胞S值,并与MIRD委员会解析算法的计算结果进行对比,两者差异在1%以内;对不同细胞核半径、不同细胞半径及不同源位置等条件下的3 420种模型进行了模拟计算,证明了α粒子和⁷Li粒子在细胞内的S值存在差异性;最终获得的¹⁰B（n,α）⁷Li反应的细胞S值数据库,可用于细胞尺度¹⁰B不均匀分布情况下的高精度微剂量学计算。     

Range distribution of fluorine in F-implanted LiNbO3

Depth profiles of fluorine in ¹⁹F⁺implanted LiNbO³ have been accurately measured using the ₁₉F(p, γ)¹⁶O resonant nuclear reaction at E_R = 872.1 keV, with Γ = 4.2 keV. A proper convolution calculation method was used to extract the true distribution of fluorine from the experimental excitation yield curves. The experimental range distribution parameters, R_p and ΔR_p, were compared with those obtained by Monte Carlo simulation using a computer code developed recently in this group and with results obtained using the TRIM90 code. It shows that the experimental R_p values agree with the Monte Carlo simulation values very well, while the experimental ΔR_p values are larger than those obtained from the simulations. The simulation with our computer code improves the agreement between the experimental and calculated range straggling, ΔR_p.     

The Stuttgart positron beam, its performance and recent experiments

A monoenergetic MeV positron (e⁺) beam, with a flux at present of 6 × 10⁴ e⁺/s in the energy range of 0.5 to 6.5 MeV, has been installed at the Stuttgart Pelletron accelerator. The stabilization and the absolute calibration of the energy E is monitored by a Ge detector with real-time feedback; a relative energy stability of ΔE/E 10⁻⁴ is obtained. So far, e⁺e⁻ scattering and annihilation-in-flight experiments for investigating the low-energy e⁺e⁻ interaction as well as β⁺ γ positron lifetime measurements in condensed matter have been performed. The advantages of the β⁺ γ method compared to the conventional γγ coincidence technique have been demonstrated. Recently, triple-coincidence positron “age-momentum correlation” measurements have been carried out on fused quartz. A brief account is given on the development of a “positron clock” aiming at a substantial improvement of the time resolution of the β⁺ γ positron lifetime measurements.     

Analysis of Cu and O in high-Tc superconductors by 7–9 MeV protons

The use of proton-induced γ-ray emission for the simultaneous analysis of Cu and O in high-T_c superconductors is demonstrated. Utilizing 7–9 MeV protons, the ratio of O relative to Cu can be determined reliably to a few percent accuracy in homogeneous bulk samples and films thicker than 130 μm using standard bulk samples of O and Cu. Results of the present method are compared with those of the analysis of YBa₂Cu₃O_7xdone by the Rutherford scattering of particles and the non-Rutherford scattering through the ¹⁶O(p,p₀)¹⁶O reaction.     

基于光化学锂同位素分离条件的同位素比率测量

从光化学锂同位素分离实验研究的需求出发,基于其分离条件,提出了一种测量锂同位素比率的方法。该方法利用锂原子蒸气对探测光吸收峰的峰值来计算锂的同位素比率,避开了测量原子密度时所需的吸收信号频率定标与光强随频率变化积分中积分限的选择问题。该方法还根据锂同位素吸收谱的特殊性采用具有较强吸收效应的⁶Li的D₂线对应的吸收峰峰值,可在原子蒸气中⁶Li含量较低时提高对比率的测量精度。设计并搭建了实验装置,对该方法进行了测试。同一条件下所测得的同位素比率相对标准偏差小于1%,表明该方法对光化学分离方法中锂同位素比率相对变化是敏感的。这意味着该方法可作为以原子蒸气为分离介质的激光锂同位素分离研究的诊断手段。     

恒星中子源~(13)C(α,n)~(16)O反应的研究

13 C(α,n)16 O是渐进巨星支(AGB)星中慢速中子俘获(s)过程的主中子源反应,而17 O 6.356 MeV1/2+阈下共振对13 C(α,n)16 O反应影响很大。本文使用HI-13串列加速器和Q3D磁谱仪,首次测量了13C(11B,7Li)17 O转移反应角分布,确定了影响13C(α,n)16 O反应最关键、最不确定的17 O(Ex=6.356MeV)阈下共振态的α宽度,从而得出天体物理能区13 C(α,n)16 O反应的天体物理S因子和反应率,澄清了国际上已有S因子数据间高达25倍的巨大分歧。AGB星s过程核合成网络计算表明:新反应率数据导致恒星中铅的丰度增加了25%。     

Research of Si and GaAs diode structures by Ion Beam Induced Charge (IBIC) collection

A Si pn junction diode and a GaAs Schottky diode were prepared for studying the basic mechanism of charge collection followed by high energy charged particle incidence in order to improve the resistance against single event upset. A 2 μm wide and 20 μm long rectangular Al electrode attached to a circular Al electrode with a 50 μm diameter was made on a 2.5 μm thick epilayer (minority carrier density 2 × 10¹⁵ /cm³). Both a Schottky electrode of Al (5 μm × 110 μm) and two ohmic electrodes of AuGe/Ni (110 μm × 110 μm) were made on a 2 μm thick epilayer (7.3 × 10¹⁵ /cm³) grown on a semi insulator GaAs substrate (1 × 10⁷ Ω cm). The internal device structure was examined by the IBIC (Ion Beam Induced Charge) method using a 2 MeV He⁺ ion microbeam. IBIC images clearly show an Al electrode, the SiO₂, and an epilayer. These results were then used to improve the qualities of the test diodes.     

Micro-ERDA studies of hydrogen in polycrystalline CVD diamond windows

The incorporation of hydrogen in thick polycrystalline chemical vapour deposition diamond plates has been studied by elastic recoil detection with a 2.8 MeV He⁺ microbeam. Hydrogen-rich inclusions of lateral dimensions 50–100 μm have been found and analysed quantitatively by depth resolved hydrogen area maps and line scans. The laterally averaged hydrogen content and its depth profile were also characterized by the ¹H(¹⁵N, γ)¹²C reaction. The observed hydrogen-rich inclusions correlate with features visible in optical microscopy but not with the optically visible crystallite topography.     

GIC4117串列加速器外束PIXE/PIGE分析系统

本文介绍在北京师范大学GIC4117串列加速器上建立的外束PIXE/PIGE分析系统,和基于此系统的薄样品外束PIXE/PIGE定量分析方法。给出了2010年Teflon滤膜采集的361个气溶胶样品外束PIXE分析得到的各元素平均探测限和最低探测限,并同真空PIXE分析探测限进行了比较。利用标准样品给出了激发曲线不同坪区薄样品外束PIGE分析F和Na的探测限,通过测定¹⁹F(p, p′γ)¹⁹F激发的197 keV γ射线得到的F的探测限可达73.9 ng•cm^-2,Na的探测限可达198.9 ng•cm^-2。