关于压水堆产武器级钚的模拟计算

防止核扩散是国际社会共同努力的目标,其中武器级核材料的防扩散是重中之重.钚是反应堆的副产品,如果不计较经济效益,利用铀为核燃料的反应堆都可以生产武器级钚.本文基于日本Takahama-3压水堆建立了五个模型,并进行中子和燃耗计算,得到两种燃料棒产武器级钚的条件、燃料棒轴向的燃耗分布、组件内燃料棒燃耗的变化区间和全堆芯燃料棒径向燃耗分布.基于上述模型和计算数据给出压水堆堆芯内含有武器级钚的准确位置和UO_2燃料棒中武器级钚的产量.这种低燃耗的乏燃料给国际核不扩散带来了巨大风险,国际社会应该加强对此类乏燃料的监管.     

压水堆不同燃耗完整和破损棒燃料芯块氧化特征拉曼光谱研究

为研究压水堆不同燃耗完整和破损燃料棒燃料芯块氧化过程和物相变化,采用拉曼光谱分析技术对燃耗为14 GW·d·t^-1和45 GW·d·t^-1的完整燃料棒及燃耗为14 GW·d·t^-1和41 GW·d·t^-1的破损燃料棒燃料芯块的氧化特征进行了分析。结果表明：14 GW·d·t^-1和45 GW·d·t^-1的完整燃料棒燃料芯块由UO₂、U₄O₉和U₃O₈组成,相比于燃料芯块的内部区域,芯块边缘显示出更强的氧化性;14 GW·d·t^-1和41 GW·d·t^-1破损燃料棒燃料芯块发生了重结构,形成柱状晶粒,主要物相为UO₂和U₃O₈。燃耗的加深和燃料棒的破损均促进了燃料芯块的氧化过程,但并不会改变燃料芯块的主要相结构。     

乏燃料中Pu同位素含量数值模拟

利用燃耗计算程序MCORGS模拟反应堆燃耗与乏燃料中Pu同位素含量之间的关系,通过对轴向上分为20段的重复栅元模型和组件模型进行的燃耗计算,得到压水堆中乏燃料中轴向不同位置燃耗的分布和Pu-239同位素含量的变化,模拟发现Pu-239同位素含量随着燃料棒在堆芯中的位置不同变化很大。同时,对VVER1000组件和压水堆1717组件也进行了燃耗计算,计算发现组件径向不同位置的燃耗有一定差别。轴向上和径向上不同位置的燃耗差别会导致同一批卸载的乏燃料中含有很多低燃耗的燃料区间,这种乏燃料给国际核不扩散带来了巨大的风险,应该加强监管。     

HPR1000堆芯装载50%MOX组件的燃料管理方案北大核心CSCD

针对HPR1000压水堆堆芯,开展了应用MOX(混合氧化物燃料)组件的燃料管理方案初步研究。对MOX燃料组件进行设计,研究了MOX燃料成分及燃料棒在组件内的布置。在此基础上,开展了1/4堆芯年换料、18个月长周期换料,并装载50%MOX组件这两种燃料管理方案研究。通过与UO2堆芯的对比,分析了装载50%MOX组件堆芯的核特性。分析结果表明,两种50%堆芯装载MOX组件的燃料管理方案,其堆芯主要物理参数均满足核设计准则要求。     

超临界水堆燃料组件选型论证研究

开展SCWR燃料组件性能分析及设计论证,分析研究SCWR组件设计目标,对比分析各类组件设计理念的物理热工性能与结构可实现性,论证选取综合性能优化的SCWR燃料组件方案。组件选型论证研究表明,大水棒方形组件方案采用结构设计较为简单的单水棒、组合式方形燃料组件,能够为燃料元件提供充分、均匀的慢化,而且慢化剂和冷却剂分流简单,具备良好的物理热工性能与结构可实现性,满足SCWR组件设计目标。     

压水堆核电站燃料组件弯曲对堆芯中子学的影响分析计算

在压水堆核电站中,由于燃料组件装配的压紧力、冷却剂流动、辐射蠕变、燃耗等因素会导致燃料组件的弯曲,燃料组件的弯曲对组件间的水隙分布产生影响,从而影响中子的慢化行为及堆芯的传热性能,进而对反应堆堆芯的运行参数造成影响。本文分析了组件弯曲的成因及机理、影响及后果（包括对堆芯功率分布、径向功率倾斜、焓升因子、热点因子等参数的影响）,并使用蒙特卡罗软件JMCT,对组件弯曲的确定论计算程序的正确性进行了验证。最后通过确定论的计算程序模块,对CPR1000核电站的组件弯曲情况进行了模拟分析,计算结果表明:在某一燃耗下,随着水隙增加或减小,燃料组件功率会随之增加或减小,使堆芯的功率分布发生倾斜,影响核电站的安全运行。     

177堆芯24个月换料可行性研究

与18个月换料相比,压水堆核电站24个月换料能减少大修次数,提高机组负荷因子,增加发电量。基于装载177组件的堆芯,通过提高新燃料组件富集度和增加批换料组件数使堆芯循环长度达到24个月换料周期要求,考虑实际24个月换料和名义24个月换料高低两种电厂可利用因子。考虑燃料组件费用、大修费用、乏燃料处理费用和发电收益等进行换料方案经济性分析评估,并和典型18个月换料经济性作比较。177堆芯平衡循环装载88组富集度为4.95%的燃料组件,能满足名义24个月换料循环长度的需要,组件平均卸料燃耗约48 GWd/tU;装载104个燃料组件的堆芯能满足实际24个换料循环长度的要求,堆芯参数满足相关安全限值要求。结果表明,177堆芯24个月换料具有可行性,其高负荷因子下的经济性与18个月换料相当。     

基于JMCT-JBURN的燃料棒径向功率分布计算北大核心CSCD

研究给出基于蒙特卡罗粒子输运软件JMCT耦合燃耗分析软件JBURN计算燃料棒径向功率分布的方法。介绍了计算模型的建立、输运及燃耗计算的相关设置以及裂变功率、俘获功率的统计方法。UO_(2)燃料棒径向功率分布的计算结果表明,采用JMCT-JBURN软件的结果与工程常用软件符合较好,最大偏差不超过3%,证明了计算方法和计算软件的适用性。该方法可用于工程设计。     

基于JMCT-JBURN的燃料棒径向功率分布计算

研究给出基于蒙特卡罗粒子输运软件JMCT耦合燃耗分析软件JBURN计算燃料棒径向功率分布的方法。介绍了计算模型的建立、输运及燃耗计算的相关设置以及裂变功率、俘获功率的统计方法。UO₂燃料棒径向功率分布的计算结果表明,采用JMCT-JBURN软件的结果与工程常用软件符合较好,最大偏差不超过3%,证明了计算方法和计算软件的适用性。该方法可用于工程设计。     

基于短半衰期核素的γ谱燃耗测量方法

提出了一种基于短半衰期核素平衡浓度求解燃耗的谱法。该方法通过将待测燃料在恒定中子通量条件下辐照一段时间,使得短半衰期标识核素建立浓度平衡,并基于核素平衡浓度与燃料中剩余235U含量之间的关系求解得到燃耗值。理论模拟结果与LR-0实验堆上的燃料辐照实验均表明,当燃料经过短期辐照后,短半衰期标识核素88Kr,92Sr能在谱中出现明显可分辨的特征峰,从而证实了88Kr,92Sr作为燃耗测量的标识核素的可行性。模拟了不同实验条件下测量富集度为20%的乏燃料的燃耗情况,实验表明标识核素88Kr,92Sr与其相应的干扰核素的特征峰在相应能量段均可分辨出来,且谱的测量宜选在乏燃料卸料冷却11 h内进行。最后通过88Kr,92Sr计算获得了与理论值相吻合的燃耗值。相比于其他方法,该方法测量燃耗不受辐照历史、燃料富集度、再次辐照前冷却时间的影响。     

Total Cross Sections for Electron Scattering from CF4, CF3H,CF2H2, and CFH3 Molecules in Energy Range from 100 to 3000 eV

The additivity rule has been employed to calculate the total cross sections for electron scattering by CF4,CF3 H, CF2 H2, and CFH3 molecules over an incident energy range from 100 to 3000 e V. Compared with other calculations and experimental data for CF4, excellent agreement has been obtained. Above 1000 eV, there are no experimental data for CF3H, CF2H2, and CFH3, so the present results can provide comparison and prediction for experimental research.     

Argon ion stimulated conversion between CFx (x = 0–3) chemical states and fluorine depletion in fluorocarbon films studied by X-ray photoelectron spectroscopy

Surface chemical composition of fluorocarbon films deposited onto indium-tin-oxide (ITO) substrates was modified by 2.0 keV Ar⁺ irradiation with doses of up to 2.6×10¹³ ions/cm². The effect of ion irradiation on the chemical composition and bonding configuration of the upper-surface and sub-surface regions were monitored by high-resolution angle-resolved X-ray photoelectron spectroscopy (AR-XPS). It was found that the as-deposited films compose of a distribution of CF, CF₂, CF₃ and C–C chemical states. C 1s line-shape analysis of XPS spectra measured at grazing and normal emission angles shows that as a result of the irradiation, the population of the CF₃ and CF₂ chemical states were preferentially depleted from the film’s surface resulting in an increased population of the CF and C–C chemical states in the upper-surface region of the film. It is suggested that low energy ion irradiation can be used to chemically modify the surface of fluorocarbon films.     

The effect of fluorocarbon gases on sonoluminescence: a failure of the electrical hypothesis

Ultrasonic irradiation of solutions containing volatile organometallic complexes results in intense emission from excited-state metal atoms. We have determined the effect of dissolved gases (Xe, Kr, Ar, Ne, He, CF₄, C₂F₆, CO, N₂) on the intensity of the sonoluminescence resulting from ultrasonic irradiation of silicone oil solutions of Cr(CO)₆. This provides a well-defined, spectrally resolved probe of sonoluminescence with emission resulting from a single species, the chromium atom excited states. As predicted by the hot-spot, thermal mechanisms of sonoluminescence, the intensity of excited-state Cr emission decreases with increasing thermal conductivity of the noble gases. The intensity of sonoluminescence increases with increasing γ (i.e. C_p/C_v), which is also in accord with a thermal mechanism. Sonoluminescence is substantially diminished by the addition of even small amounts (≈ 1%) of CF₄ or C₂F₆, even though they are capable of supporting electrical discharge. This is in agreement with a thermal mechanism, but is in direct conflict with electrical theories of sonoluminescence.     

ArF laser-induced discharge interruption in a mixture of C2H3Cl/CF4/CH4, CF4/CH4, and C2H3Cl/He

The ArF-laser (193-nm)-induced discharge interruption is comparatively described in a mixture of C₂H₃Cl/CF ₄/CH₄, CF₄/CH₄, and C₂ H₃Cl/He using a hollow-cathode-type discharge tube. The unfocused ArF laser (typically 27 mJ/cm² and 10 ns duration) illuminated both the negative glow inside the hollow cathode and the column between the two electrodes. With a 1.8-torr mixture of C₂ H₃Cl/CF₄, the discharge current of 1 mA was decreased rapidly with a current-decay time constant of 1 μs and a current-decay rate of 1 kA/s. With a 1.5-torr mixture of CF₄/CH₄, 2.2 μs and 450 A/s were obtained. With a 1.5-torr mixture of CH₂H₃Cl/He, a time constant of over 3 μs and a rate of less than 300 A/s were obtained. An analysis of the discharge interruption induced by ArF-laser irradiation is given in terms of photon-plasma kinetics. The current peak induced by ArF irradiation is also explained for a mixture of C₂H₃ Cl/He in terms of photoionization and photodetachment processes     

A DFT/TD-DFT study of effect of different substituent on ESIPT fluorescence features of 2-(2'-hydroxyphenyl)-4-chloro- methylthiazole derivatives

Based on density functional theory (DFT) and time-dependent density functional theory (TD-DFT), the effects of substituent on the excited-state intramolecular proton transfer (ESIPT) process and photophysical properties of 2-(2'-hydroxyphenyl)-4-chloromethylthiazole (HCT) are studied. The electron-donating group (CH₃, OH) and electron-withdrawing group (CF₃, CHO) are introduced to analyze the changes of intramolecular H-bond, the frontier molecular orbitals, the absorption/fluorescence spectra, and the energy barrier of ESIPT process. The calculation results indicate that electron-donating group strengthens the intramolecular H-bond in the S₁ state, and leads to an easier ESIPT process. The electron-withdrawing group weakens the corresponding H-bond and makes ESIPT process a little harder. Different substituents also affect the photophysical properties of HCT. The electron-withdrawing group (CF₃, CHO) has a little effect on electronic spectra. The electron-donating group (CH₃, OH) red-shifts both the absorption and fluorescence emission peaks of HCT, respectively, which causes the Stokes shift to increase.     

Surface chemistry of alkyl and perfluoro ethers: a FTIR and ab initio study of adsorption and decomposition of CF3OCF3 on an Al2O3 surface

The adsorption and thermal decomposition of perfluorodimethyl ether, (CF₃)₂O, on a high-surface-area Al₂O₃ surface was investigated by FTIR under both vacuum and pressure conditions. IR spectra in the 4000-1050 cm⁻¹ range were collected and the spectral assignments were assisted by quantum chemical ab initio calculations. The spectral evidence indicated that (CF₃)₂O decomposed to form adsorbed fluoroformate, FCOO (ads). Increases of temperature (up to 525 K) caused the FCOO (ads) to convert to hydrogen formate, HCOO (ads). Surface hydroxyl groups participated in the decomposition of (CF₃)₂O and the conversion of FCOO (ads) to HCOO (ads). A decomposition mechanism is proposed.     

X-ray damage characterization in BaLiF3,KMgF3 and LiCaAlF6 complex fluorides

Two-inch sized KMgF₃,BaLiF₃ and LiCaAlF₆ (LiCAF) single crystals were grown by the Czochralski method under a CF₄ atmosphere. X-ray irradiation was used to carry out a comparative study of induced optical absorption phenomena and colour centre creation in the ultra-violet and visible spectral regions. The integral of the induced absorption spectra is significantly lower in LiCAF with respect to the other studied materials. It is found that the amplitude of the F-absorption band is suppressed more than a factor of 3 by Mg-doping. For Mg-doped crystals, the optimum doping concentration is about 0.2 mol% of Mg²⁺.     

Effect of branching in base polymer on ionic conductivity in hyperbranched polymer electrolytes

Novel hyperbranched polymer, poly[bis(diethylene glycol)benzoate] capped with a 3,5-bis[(3′,6′,9′-trioxodecyl)oxy]benzoyl group (poly-Bz1a), was prepared, and its polymer electrolyte with LiN(CF₃SO₂)₂, poly-Bz1a/LiN(CF₃SO₂)₂ electrolyte, was all evaluated in thermal properties, ionic conductivity, and electrochemical stability window. The poly-Bz1a/LiN(CF₃SO₂)₂ electrolyte exhibited higher ionic conductivity compared with a polymer electrolyte based on poly[bis(diethylene glycol)benzoate] capped with an acetyl group (poly-Ac1a), and the ionic conductivity of poly-Bz1a/LiN(CF₃SO₂)₂ electrolyte was to be 7×10⁻⁴ S cm⁻¹ at 80 °C and 1×10⁻⁶ S cm⁻¹ at 30 °C, respectively. The existence of a 3,5-bis[(3′,6′,9′-trioxodecyl)oxy]benzoyl group as a branching unit present at ends in the base polymer improved significantly ionic conductivity of the hyperbranched polymer electrolytes. The polymer electrolyte exhibited the electrochemical stability window of 4.2 V at 70 °C and was stable until 300 °C.     

氟利昂F113分子在飞秒激光作用下的多光子电离解离动力学

大气臭氧层因吸收太阳紫外光, 是人类必不可少的保护伞. 氟利昂在太阳光辐射下解离生成破坏臭氧的游离态氯原子, 是破坏大气臭氧层的主要元凶之一. 本文利用飞行时间质谱技术和离子速度成像技术研究了氟利昂F113(三氟三氯乙烷)分子在800 nm 飞秒光作用下的多光子电离解离动力学. 利用飞行时间质谱探测技术, 得到了三氟三氯乙烷在该波长飞秒激光作用下发生多光子电离解离产生的碎片质谱. 通过荷质比对碎片质谱进行了详细的标定和分析. 在质谱上未发现母体离子, 所有观察到的离子都是由于激光脉冲作用下产生的碎片. 三个最主要的碎片离子是CFCl₂⁺, CF₂Cl⁺, C₂F₃Cl₂⁺. 通过飞行时间质谱标定, 发现并归属了多个解离通道. 三个主要的解离机理分别为: 1) C-Cl键断裂直接生产氯自由基的通道C₂F₃Cl₃⁺→C₂F₃Cl₂⁺+Cl; 2) C--C键断裂C₂F₃Cl₃⁺→CFCl₂⁺+CF₂Cl; 3) C--C键断裂C₂F₃Cl₃⁺→CF₂Cl⁺+CFCl₂. 利用离子速度成像技术对这三个主要通道产生的碎片离子进行成像, 得到了C₂F₃Cl₂⁺, CFCl₂⁺和CF₂Cl⁺离子的速度影像. 由C--Cl键断裂产生的碎片离子C₂F₃Cl₂^{+}的速度分布由两个高斯分布曲线拟合, 而由C--C键断裂产生的碎片离子CFCl₂⁺和CF₂Cl⁺可以用一个高斯曲线拟合. 通过影像分析得到了解离碎片的平动能分布和角向分布各向异性参数等详尽的动力学信息. 结合高精度密度泛函理论计算对解离动力学进行了进一步的分析和讨论.深入认识氟利昂的解离动力学可为进一步控制破坏臭氧层提供理论参考和实验依据.     

Phase transitions in physisorbed films on cadmium (0001): comparison with graphite (0001)

Physical adsorption of simple molecules has been studied experimentally on cadmium (0001). Adsorption isotherms of Kr and CF₄ at 77.3 K show a first-order phase transition in the first layer, characteristic of adsorption on uniform substrates.

The nature of the phase transition on cadmium (0001) in the first layer is investigated for Kr and CF₄ by a thermodynamic approach in comparison with results obtained earlier on graphite (0001).

From the comparison between the two uniform substrates, we show that (1) cadmium (0001) has a less attractive force field than graphite (0001); and (2) like graphite (0001), cadmium (0001) is a very uniform surface suitable for studying two-dimensional phases according to the Gibbsian formulation.