Oxygen ion source with plasma cathode

An ion source with a plasma cathode has been developed for long lifetime use in ion implanters. In this ion source, a plasma cathode replaces the conventional metallic filament used in a Freeman-type ion source. This ion source consists of two compartments, namely a plasma generator and an ion source chambers interconnected by a tapered narrow duct. The pressure difference between the two parts, maintained by differential pumping, prevents the feed gas from flowing into the plasma generator. With any combination of an argon plasma cathode and a feed gas of either fluoride (AsF₅, PF₅) or oxygen, the lifetime was found to be more than 90 h with an extraction voltage of 40 kV and a correspoding ion current density of 20 mA/cm², and a considerable amount of As⁺, P⁺, O⁺, and O₂⁺ ions were observed in mass spectra.     

Targets and ion sources at the TISOL facility

The TISOL thick target, on-line isotope separator is now operational at the TRIUMF facility with an active experimental program. A series of newly developed, target materials coupled with two different ion sources can now produce a wide range of isotopes. Radioactive beams of isotopes of He, C, N, O, Ne, Cl, Ar, Kr and Xe are now available in significant amounts from the first ECR (electron cyclotron resonance) ion source directly coupled to a multipurpose ISOL device. In addition, a surface ionization source with good yields for radioactive isotopes of Li, Na, Al, Ga, Rb, In, Cs, Yb and Fr is also available. Special emphasis has been given to the development of target materials, in particular light mass powder or pellet targets such as SiC and MgO. In addition, a newly developed zeolite (NaSiAlO₄) target shows properties which make it an optimal choice for producing isotopes near stability for nuclear astrophysics experiments with accelerated radioactive beams. Source and target developments at the upgraded TISOL facility will be presented.     

BRISOL钠同位素放射性核束的产生

北京放射性核束装置在线同位素分离器（BRISOL）采用100 MeV、200 μA回旋加速器提供的质子束打靶产生中、短寿命放射性核束,在线分析后供物理用户使用,其质量分辨率好于20 000。为开展²⁰Na核的奇异衰变特性研究,研制了氧化镁靶,并采用100 MeV质子束轰击氧化镁靶在线产生了^20～26Na⁺的钠同位素放射性核束。当质子束流强为8 μA时,²⁰Na⁺离子束的最大产额为2×10⁵ s^-1,²¹Na⁺离子束的最大产额为4×10⁸ s^-1。完成了北京放射性核束装置首个放射性核束物理实验,累计供束近200 h。     

北京放射性核束装置在线同位素分离器的研制

北京放射性核束装置在线同位素分离器（BRISOL）采用100 MeV、200 μA回旋加速器提供的质子束打靶产生中、短寿命放射性核束,进行在线分析后供物理用户使用,其质量分辨率好于20 000。BRISOL装置现已建成,并开展了氧化镁、氧化钙靶的在线实验,在线产生了³⁷K⁺、³⁸K⁺、²⁰Na⁺、²¹Na⁺等多种放射性核束。本文详细介绍该装置的研制及运行情况。     

螯合剂对铀在小鼠体内分布的影响研究

铀在生物体内的化学形态及分布是评价铀毒性的基础。文章通过尾静脉注射给药方式研究螯合剂对染铀小鼠体内铀分布的影响。通过建立包含主要体液金属离子、小分子配体及UO₂²⁺与螯合剂的热力学平衡模型,采用数值模拟方法研究UO₂²⁺在血液中的形态。实验结果表明：DTPA易与UO₂²⁺形成［(UO₂)₂(OH)DTPA］^2-,对小鼠血液中的UO₂²⁺有明显的促排作用,但在促排的同时对小鼠的肾脏和骨骼有损伤;抗坏血酸对小鼠体内各组织器官的铀促排几乎无作用,但形成的［(UO₂)₂(OH)Ascorbate］²⁺会阻碍肾脏中U(Ⅵ)的代谢;NTA对小鼠体内各组织器官铀的促排作用小,并会促使体内出现固相(UO₂)₃(PO₄)₂·4H₂O,对骨骼有较强的损伤作用,不适合作为铀的促排剂。     

Structural study on uranyl ion in 1-butyl-3-methylimidazolium nonafluorobutanesulfonate ionic liquid

The structure of uranyl ion in 1-butyl-3-methylimidazolium nonafluorobutanesulfonate ionic liquid (BMINfO) has been studied with ¹H- and ³⁵Cl-NMR, Raman, and UV-visible spectroscopy. In the ¹H-NMR spectrum of the BMINfO solution prepared by dissolving UO₂(ClO₄)₂·5 6H₂O, the signal of H₂O coordinated to UO₂²⁺ was observed at 6.64 ppm at 50°C (free H₂O in BMINfO: 3.1 ppm at 50°C), suggesting that the uranyl species exists as the aquo complex, [UO₂(H₂O)_n]²⁺. The signal of the coordinated H₂O disappears with heating at 120°C for 3 h under vacuum. This indicates the dehydration from [UO₂(H₂O)_n]²⁺. On the other hand, the ³⁵Cl-NMR signal of ClO₄⁻ as the counter anion of UO₂²⁺ was observed at 1011 ppm (vs. Cl⁻ in D₂O) regardless of heating. This indicates that no ClO₄⁻ ion is in the first coordination sphere of UO₂²⁺. Furthermore, the UV-visible absorption spectra showed that the characteristic absorption bands due to UO₂²⁺ were sharpened with the dehydration. This means the simplification of the structure around UO₂²⁺. These results described above suggest that UO₂²⁺ in BMINfO has no ligand in its equatorial plane after the dehydration, i.e. UO₂²⁺ exists as a bare cation in this system.     

Synthesis of carbon-nitride films using a fast-switched dual-source low energy ion beam deposition system

Thin C_xN_y films were deposited in UHV using alternating low energy ion beams of C⁺ and N⁺ or N₂⁺ in the energy range of 5 to 100 eV. The ion beam deposition system is equipped with two Freeman ion sources, mass analysis and fast automated beam switching, allowing perpendicular bombardment of the target with a single ion beam at a time. The composition and density of the films were studied by ARS (in situ), XPS and RBS. The dependence of the film properties and growth mechanisms on ion energy, beam switching rate, and C-to-N arrival ratio have been investigated. The influence of the deposition parameters on the film stoichiometry is discussed. Exposure of the film to atmosphere leads to oxygen incorporation, resulting in a lowered surface concentration of nitrogen. The XPS N 1s and C Is binding energies vary in a relatively broad range indicating that several bond states may be present. The influence of the substrate material on film growth has also been studied. On Si{100}, film growth commences with the formation of an interfacial silicon nitride. No film growth was observed on gold, however deposition was possible on tantalum and molybdenum.     

Production, acceleration and use of radioactive ion beams at Louvain-la-Neuve

The production and acceleration of radioactive beams using two cyclotrons coupled by an electron cyclotron resonance ion source is described. Pure beams of ¹³N(T1/2 = 9.96 min) and ¹⁹Ne(T1/2 = 17 s) with an energy around 1 MeV/amu are obtained with intensities larger than 50 ppA. As an example, cross section measurements using a ¹³N beam on hydrogen and deuteron targets are presented. Finally, the ARENAS³ project, a future plan for the production of radioactive beams in Belgium, is described.     

Effect of N_2 and O_2 on OH radical production in an atmospheric helium microwave plasma jet

UV-pulsed laser cavity ringdown spectroscopy of the hydroxyl radical OH(A–X)(0–0)band in the wavelength range of 306–310 nm was employed to determine absolute number densities of OH in the atmospheric helium plasma jets generated by a 2.45 GHz microwave plasma source.The effect of the addition of molecular gases N_2 and O_2 to He plasma jets on OH generation was studied.Optical emission spectroscopy was simultaneously employed to monitor reactive plasma species.Stark broadening of the hydrogen Balmer emission line(H_β)was used to estimate the electron density nein the jets.For both He/N_2 and He/O_2 jets, newas estimated to be on the order of 10~(15)cm~(-3).The effects of plasma power and gas flow rate were also studied.With increase in N_2 and O_2 flow rates, netended to decrease.Gas temperature in the He/O_2 plasma jets was elevated compared to the temperatures in the pure He and He/N_2 plasma jets.The highest OH densities in the He/N_2 and He/O_2 plasma jets were determined to be 1.0?×10~(16)molecules/cm~3 at x?=?4 mm(from the jet orifice)and 1.8?×?10~(16)molecules/cm~3 at x=3 mm, respectively.Electron impact dissociation of water and water ion dissociative recombination were the dominant reaction pathways, respectively, for OH formation within the jet column and in the downstream and far downstream regions.The presence of strong emissions of the N_2~+ bands in both He/N_2 and He/O_2 plasma jets, as against the absence of the N_2~+ emissions in the Ar plasma jets, suggests that the Penning ionization process is a key reaction channel leading to the formation of N_2~+ in these He plasma jets.     

土壤中球孢枝孢对铀（Ⅵ）的吸附

从拟作为低放射性废物处置填埋场土壤中分离出一种霉菌,经过鉴定为链孢霉目黑霉科球孢枝孢,并考察该菌对UO₂²⁺的吸附行为。实验结果表明：铀初始质量浓度为10mg/L,加入5g/L的新鲜湿菌体,其吸附平衡时间约为24h,最终吸附率约94.1%,吸附符合准二级动力学模型;吸附最适宜pH=5～9,当pH≤2时,菌体几乎不吸附UO₂²⁺;铀初始质量浓度为2~10mg/L时,吸附率均在90%左右;吸附近似符合Langmuir吸附经验公式;菌体累积吸附6次吸附量可达6.6mg/g;Ca²⁺会降低微生物对铀的吸附;柠檬酸、硝酸和EDTA对吸附的铀均具有一定的解吸能力,其中柠檬酸最高为67%。采用红外吸收光谱分析,显示吸附后出现UO₂²⁺的吸收峰,表明铀主要以UO₂²⁺的形式被菌体吸附。     

Volume added surface barrier discharge plasma excited by bipolar nanosecond pulse power in atmospheric air: optical emission spectra influenced by gap distance

In this paper, volume barrier discharge with different gap distances is added on the discharge border of high-voltage electrode of annular surface barrier discharge for generating volume added surface barrier discharge (V-SBD) excited by bipolar nanosecond high-voltage pulse power in atmospheric air. The excited V-SBDs consist of surface barrier discharge (d=0 mm) and volume added surface barrier discharges (d=2 mm and 3 mm). The optical emission spectra are recorded for calculating emission intensities of N₂ (C ³Ⅱ_u →B³Π_g ) and N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ ), and simulating rotational and vibrational temperatures. The influences of gap distance of V-SBD on emission intensity and plasma temperature are also investigated and analyzed. The results show that d=0 mm structure can excite the largest emission intensity of N ₂ (C ³ Π_u →B ³Π_g ), while the existence of volume barrier discharge can delay the occurrence of the peak value of the emission intensity ratio of N₂⁺ (B ²Σ_u⁺ → X ²Σ_g⁺ )/N ₂(C³Π_u →B³Π_g ) during the rising period of the applied voltage pulse and weaken it during the end period. The increasing factor of emission intensity is effected by the pulse repetition rate. The d=3 mm structure has the highest threshold voltage while it can maintain more emission intensity of N₂(C³ Π _u →B ³Π_g ) than that of d=2 mm structure. The structure of d=2 mm can maintain more increasing factor than that of the d=3 mm structure with varying pulse repetition rate. Besides, the rotational temperatures of three V-SBD structures are slightly affected when the gap distance and pulse repetition rate vary. The vibrational temperatures have decaying tendencies of all three structures with the increasing pulse repetition rate.     

Structure and kinetic studies of U(VI)-benzamidoxime complex in non-aqueous solutions by H- and C-NMR

The structural and kinetic studies of U(VI) complex with benzamidoxime(Hba) as ligand in CD₃COCD₃ have been studied by means of ¹H and ¹³C NMR. The Hba molecule was found to coordinate to UO₂²⁺ in the form of anionic benzamidoximate (ba), and the number of ba coordinated to UO₂²⁺ was determined to be 3 by analyzing the chemical shift of ¹³C NMR signal for Hba in the presence of UO₂²⁺. The exchange rate constants(k_ex) of ba in [UO₂(ba)₃] were determined by the NMR line-broadening method. The kinetic parameters were obtained as follows: k_ex(25°C) = 3.1 × 10³s⁻¹, ΔH^≠ = 35.8 ± 3.5 KJ mol⁻¹, and ΔS^≠ = −65 ± 13.7 J K⁻¹ mol⁻¹. The UV-visible absorption spectra of solutions containing UO₂²⁺ and Hba were also measured. The molar extinction coefficient of the complex was found to be extremely large compared with those of UO₂(L)₅²⁺ (L = unidentate oxygen donor ligands) complexes. This is due to the strong electron withdrawing of UO₂²⁺ from Hba and suggests that an interaction between UO₂²⁺ and Hba is very strong. Such a high affinity of monomeric amidoxime to UO₂²⁺ reasonably explains the high adsorptibility of amidoxime resin to U(VI) species, and is considered to result in the high recovery of U(VI) species from sea water using amidoxime resin.     

铀在北山地下水中的种态分布及溶解度分析

为了解铀酰离子在北山地下水中的吸附、扩散和迁移行为,利用地球化学计算软件PHREEQC,采用由OECD/NEA发布的最新铀的热力学数据,计算了铀在我国高放废物地质处置库重点研究区甘肃北山地下水中的种态分布,并分析了围岩中存在的方解石对铀溶解度的影响。计算结果表明,在北山地下水组成不变的前提下,在偏酸性条件下,铀主要以UO₂F⁺、UO₂SO₄、UO₂²⁺、UO₂F₂和UO₂(SO₄)₂^2-的形式存在,而在中性至弱碱性条件下,主要以 UO₂(CO₃)^4-₃、UO₂(CO₃)₂^2-、UO₂(OH)₃^-和UO₂(OH)₄^2-的形式存在。我国计划建造的高放废物处置库的设计深度为地下500～1000m,其水岩体系一般呈弱碱性。在这样的弱碱性水岩体系中,以阴离子形式存在的铀酰配合物具有较强的可移动性。当地下水的pH=7.56时,在Eh<24mV的条件下,铀主要以沥青铀矿的形式存在,而在更高的Eh条件下,则主要以UO₂²⁺与CO₃^2-和OH^-形成的阴离子配合物的形式存在。当地下水与空气接触时,O₂的存在会使Eh升高,此时铀的主要存在种态为UO₂²⁺及其各种配合物。当围岩体系中存在方解石时,在pH<8.0的条件下,铀在地下水中的溶解度会显著提高,而在更高pH条件下,方解石对铀的溶解度无明显影响。     

赣杭构造带某铀矿区地下水中铀的存在形式研究北大核心CSCD

为研究铀矿区地下水化学性质对铀的存在形式的影响,本文以赣杭构造带某铀矿区地下水为研究对象,在对9个典型采样点地下水化学成分分析的基础上,采用数理统计软件SPSS 18.0和地球化学模拟软件PHREEQC及llnl.dat数据库,探究了研究区内地下水水化学特征及U的存在形式。结果表明:本研究区地下水水化学类型以HCO_(3)-Na与HCO_(3)-Na·Ca为主,U含量与Ca^(2+)和Mg^(2+)浓度体现出较强正相关性,与SO_(4)^(2-)的相关性次之;地下水中U元素主要以六价为主,几乎占100%,主要存在形式依次为UO_(2)(CO_(3))_(2)^(2-)、UO_(2)(CO_(3))_(3)^(4-)、UO_(2)CO_(3)、UO_(2)(OH)2、UO_(2)(OH)_(3)^(-)、UO_(2)OH^(+)等6种,其中UO_(2)(CO_(3))_(2)^(2-)占绝对优势,整体以碳酸铀酰形式为主,这也与研究区地下水酸碱性相对应。     

Evaluation of trans-ferulic acid degradation by dielectric barrier discharge plasma combined with ozone in wastewater with different water quality conditions

In this study, dielectric barrier discharge plasma and ozone(O_3) were combined to synergistically degrade trans-ferulic acid(FA), and the effect of water quality on FA degradation was studied. The results showed that 96.9% of FA was degraded after 40 min treatment by the plasma/O_3 process. FA degradation efficiency increased with the p H values. The presence of suspended solid and humic acid inhibited FA degradation. FA degradation efficiency increased as the water temperature increased to 30 °C. However, the further increase in water temperature was adverse for FA degradation. Effects of common inorganic ions on FA degradation were also investigated. The addition of Cl~- inhibited the FA degradation, whileCO_3~(2-) had both negative and positive influences on FA degradation.NO_3~- andSO_4~(2-) did not have significant effect on FA degradation. Fe~(3+)and Cu~(2+)benefited FA degradation through the Fenton-like and catalytic ozonation reactions.     

Measurements of the erosion of stainless steel, carbon, and SiC by hydrogen bombardment in the energy range of 0.5 – 7.5 keV

Total erosion yields by sputtering and blistering for 1 to 15 keV H₂⁺ bombardment at normal incidence have been measured by weight loss of 304 stainless steel, pyrolytic graphite, carbon fibres, glassy carbon and SiC. The erosion yields are in the range of 3 × 10⁻³ to 2.6 × 10⁻² atoms per incident hydrogen atom. Observation in the scanning electron microscope shows that blisters occur in stainless steel and SiC at doses of 5 × 10¹⁸ particles/cm², but disappear at doses of 5 × 10 particles/cm² . The surface roughening observed depends largely on grain orientation. On carbon no blistering could be found. After bombardment the carbon surfaces are generally more smooth than before.     

北山地下水中可变价核素的溶解度和种态分布研究

北山28号钻孔(BS28)毗邻我国拟建高放废物处置库首座地下实验室场址。近期,基于现场动态连续测量,并结合地下水中溶解铁含量及围岩中Fe^2＋/Fe^3＋的比例推算,获得该钻孔365～690 m深处地下水在温度为18.4 ℃和pH值为(8.1±0.2)条件下,Eh值范围为-56至98 mV。基于此,本文利用PHREEQC程序及碳酸铀酰与Mg、Ca和Sr的三元配合物的热力学数据,计算了U、⁹⁹Tc、⁷⁹Se和Np在该地下水中的溶解度及种态分布情况。结果表明,地下水的pH值为8.1,Eh值在-56 mV到98 mV之间时,U、Tc和Se的溶解度范围分别为10^-9～10^-6 mol/L、10^-14～10^-4 mol/L和10^-14～10^-7 mol/L,而Np的溶解度始终低于10^-15 mol/L。在上述条件下,溶解态U、Se与Tc主要以Ca₂UO₂(CO₃)₃、CaUO₂(CO₃)₃^2-、HSeO₃^-、SeO₃^2-、TcO₄^-等中性分子或阴离子形式存在。在假定地下水氧气分压不变的情况下,在pH值为8.1时Eh值分别取-56 mV(最小值)、21 mV(中间值)和98 mV(最大值),本文也研究了pH 值在5～11范围内变化的影响。本工作仅针对均相溶液体系进行模拟,由于北山花岗岩围岩中富含二价铁,针对地下水-岩体系的实际情况,仍需进一步开展相关核素的还原固定实验研究。     

Environmentally acceptable nuclear fuel cycle development of a new reprocessing system

The aim of the present study is to establish a new reprocessing system for spent nuclear fuel, which would overcome the environmental problems in the nuclear fuel cycle. In order to achieve this, the following subjects have to be conquered: recoveries of high ratios of uranium and trans uranium elements from spent nuclear fuel, separations of strong radioactive elements, such as Sr and Cs, and assurance of the extreme safety during operation. The last subjects might be of particular importance in order to avoid any potential danger. Therefore, in the present system all processes were performed under mild aqueous conditions. Experiments were carried out for a simulated spent fuel solution, which was calculated from the ORIGEN CODE containing uranium and 17 major elements. The system consists of the following processes: 1. dissolution of spent UO₂ fuel involving off-gas treatment of I and Ru; 2. neutralization of the dissolved fuel solution with NaHCO₃---Na₂CO₃ mixed solution to be slightly basic at pH about 9 followed by the separation of precipitated fission products by centrifugation; 3. separation of Cs by a precipitation method using tetraphenylborate ion; 4. recovery of U, Np and Pu as precipitates of hydrolyzed compounds from alkaline solution; 5. separation of Am and Cm from lanthanide elements. The concentration of residual uranium in the final solution was measured to be ppm order, indicating that the decontamination factor of U was as large as 10⁴. Other hexa-valent actinide ions, NpO₂²⁺ and PuO₂²⁺, also have extremely large stability constants for the complex formation with carbonate ion, and are expected to behave similarly with UO₂²⁺. In conclusion, the present reprocessing system enables us to recover U, Pu and Np from spent nuclear fuel by means of a simple precipitation method in much higher ratios compared with other reprocessing methods, to separate hazardous Cs and Sr from high-level waste, and to exclude any potential danger owing to chemical processes under mild aqueous conditions.     

A new concept kinetic-ejection negative-ion source for rib generation

Chemically active radioactive species are often released from target-materials in a variety of molecular forms. For example, ¹⁷F, is principally released from Al₂O₃ target-material as Al¹⁷F. Because of the low probability of simultaneously dissociating such molecular carriers and efficiently ionizing their atomic constituents with conventional hot-cathode, electron-impact ion sources, species of interest are often distributed in several mass channels in the form of molecular side-band beams. Consequently, beam intensities of the desired radioactive species are diluted. The sputter negative-ion beam generation technique is particularly effective for simultaneously dissociating molecular carriers and efficiently ionizing highly electronegative atomic constituents. Therefore, a new concept kinetic-ejection negative-ion source (KENIS), based on this principle, was conceived to address this problem. The source has proven to be highly efficient for simultaneously dissociating and negatively ionizing sputter-ejected atomic fluorine from cesiated surfaces. The source has been successfully employed on-line to generate high intensity ¹⁷F⁻ beams for use in the astrophysics research program at the Holifield Radioactive Ion Beam Facility (HRIBF) using the ¹⁶O(d,n)¹⁷F reaction. The mechanical design features, principles of operation, operational parameters, beam quality information (emittance data) and efficiencies for forming intense beams of ¹⁷F⁻ during off-line and on-line operation of the source are presented in this report.     

Numerical analysis of thermal plasma scrubber for CF4 decomposition

CF₄ gas emitted in the semiconductor and display manufacturing process is a very harmful greenhouse gas. It must be removed or converted safely due to its extreme toxicity. Although a CF₄ decomposition system using a thermal plasma scrubber was commercialized, its removal efficiency is limited. In this work, a numerical analysis of CF₄ decomposition in the thermal plasma scrubber was carried out in order to propose an efficient decomposition environment. The decomposition and recombination temperatures of CF₄ were analyzed using thermodynamic equilibrium calculations. The chemical reaction of CF₄ decomposition into carbon and fluorine gas was considered in this numerical analysis. The injection position and angle of the CF₄ were controlled in order to enhance the decomposition rate. The vertical injection of CF₄ near the torch exit improved the mixing of the CF₄ with the thermal plasma flame. In addition, it was confirmed that the high temperature region expanded due to a vortex generated by strong turbulence in the bottleneck-shaped reactor. As a result, it is revealed that the CF₄ injection location and the reactor configuration are the most important factors in improving the decomposition rate.