高电荷态ECR离子源的设计与实验研究

本文详细论述了三种各具特色的高电荷态ECR离子源的设计与研制，它们分别是：14．SGHz全永磁高电荷态ECR离子源LAPEC咫、传统常温ECR离子源GTS、混和超导ECR离子源HECRIS。另外，还从理论与实验两个方面对ECR离子源多电荷态离子束流的引出进行了详细研究。设计研制了一台高性能14．SGHz全永磁ECR离子源LAPECRZ，该离子源的设计尺寸为杯50mm*560mm，重量可达9ookg以上，为目前世界上体积与重量最大、设计参数最高的全永磁ECR离子源。全永磁离子源的尺寸增大一些，其加工与研制所存在的难度将会有质的变化。研制LAPEC形所存在的技术难度大大超过了以往所有全永磁ECR离子源。LAPECR2的磁场参数为：注入磁场1 ．4T，如果加注入端辅助铁扼，磁场可达2．6T；引出磁场为1 ．1T；六极永磁体在弧腔内壁产生的最大径向磁场的设计值为1．22T，实际加工得到的磁场大小为1．2T，与计算结果基本一致。该离子源的设计采用了多种特殊技术与方法以提高引出高电荷态离子束流强度，如：双层含铝衬底的等离子体弧腔、铝制等离子体电极、冷阴极电子枪（注入端负偏压电极）、旁轴微波直接馈入与等离子体位置相对于磁场可调等等。目前，我们已开始源体的组装。GTS离子源为目前世界上运行性能最好的常温ECR离子源之一。它的设计指导思想是ECR离子源的经验结论scaling Laws，高磁场、高磁镜比，高磁场梯度是该离子源磁场设计的主要特点。设计时充分考虑了多频加热机制，允许多频功率同时馈入弧腔：IOGHz＋14GHz＋18GHz＋ZSGHz。良好的磁场约束、灵活的磁场结构设计、高频率大功率微波馈入、大体积弧腔、足够的冷二次电子注入、优良的真空抽气系统、以及有效的束流引出系统等等都是该离子源高性能表观的原因。经过近一年半的优化与调试，该离子源运行性能优良，能产生很多领先国际伺类ECR源的离子束流，如：1.95emAO6+，O·semAArll”，o．15e拜AArl犷，31Oe瘩建叙e，哪se拼A豁岁”与0.4eμAXe39+为18GHz时调试的结果：1.OemAAr8+，1.8eμAAr17+24OeμAXe20+ ，20eμAxe30+与0.3oe从Axe38＋为在14GHz调试的最好结果。该离子源已多次为原子物理实验提供了Ar17+与Ar18+等高电荷态离子束流。HECRIS是一台高性能混和超导ECR离子源，其各项设计参数均高于GTS源，以保证该离子源能具有比GTS更好的性能。它的最小B场型设计继续沿袭现在ECR离子源设计惯用的Scaling Laws设计思想。该离子源采用较高频率的微波馈入，设计运行范围为18GHz-24GHz。该离子源着重于在运行调试中实现对轴向最小磁场Bmin的调节与匹配，这里采用两组超导线包进行辅助调节。径向磁约束由一个能在弧腔内壁产生1．6T径向磁场的六极永磁体提供，它强磁场设计与部分磁块存在的退磁问题的解决也是该离子源的一大特点与难点。文中还详细讨论一个高性能的Halbach结构六极永磁体的设计方法。分别从永磁材料选取、物理尺寸优化、结构选择等角度，结合理论分析与PolssON，PERMAG和TOscA3D程序的模拟计算结果，对六极永磁体的性能进行了全面的分析，提出两种确定六极永磁体中存在退磁磁块的办法，并且提出了一种用高极化矫顽力永磁材料替代退磁磁块中所采用的永磁材料的解决办法。对多电荷态ECR离子源的引出进行了理论与实验两方面的研究。利用PBGUNS程序，对ECR离子源的引出系统进行了一定的理论分析。通过模拟计算，详细地论述了引出系统的各主要物理参数对ECR离子源引出离子束流品质的影响。这些得到的结果，对设计一套高性能的ECR离子源引出系统具有一定的指导意义。结合理论分析，我们还设计完成了一系列关于ECR离子源引出系统的实验，来研究多电荷态离子束流的引出与短距离传输。采用电扫描发射度测量系统（ESS）探测离子束流在x与y方向的发射度，用两个荧光靶分别在束运线不同位置探测束流的束斑形状，并利用一个亮度探测器对束斑相对亮度进行探测。通过多组实验结果的处理，分别分析了离子源的几个主要参数如磁场、微波、掺气、偏压等对引出束流品质的影响并结合相关理论给予了解释，通过对混合多电荷态离子束流的三电极引出实验结果的讨论，建立了一个关于高电荷态ECR离子源束流引出的较为清晰的物理图象。

Selective formation of aromatic amines by selenium-catalyzed reduction of aromatic nitro compounds with CO/H2O under atmospheric pressure

An efficient method for the catalytic reduction of aromatic nitro compounds to the corresponding aromatic amines is reported. In the presence of selenium as a catalyst, the aromatic nitro compounds are quantitively reduced by CO/H2O to form the corresponding amines under atmospheric pressure. The reduction occurs in high selectivity regardless of other reducible functionalities present on the aromatic ring. There exists a phase transfer process of the catalyst selenium in the reaction. (C) 2004 Elsevier B.V. All rights reserved.

CO selective oxidation in a microchannel reactor for PEM fuel cell

It is indispensable to remove CO at the level of less than 50ppm in H-2-rich feed gas for the proton exchange membrane (PEM) fuel cells. In this paper, catalyst with high activity and selectivity, and a microchannel reactor for CO preferential oxidation (PROX) have been developed. The results indicated that potassium on supported Rh metal catalysts had a promoting effect in the CO selective catalytic oxidation under H-2-rich stream, and microchannel reactor has an excellent ability to use in on-board hydrogen generation system. CO conversion keeps at high levels even at a very high GHSV as 500 000 h(-1), so, miniaturization of hydrogen generation system can be achieved by using the microchannel reactor. (C) 2004 Elsevier B.V. All rights reserved.

Cluster assistant generation of C2+ and C3+ ions in nanosecond laser ionization of seeded benzene beam

Cluster assisted photoionization processes of benzene, which was seeded in argon, induced by an intense 25 ns Nd-YAG laser has been studied by means of time-of-flight mass spectrometry. At the laser intensity of 10(11) W/cm(2), multicharged ions Cq+ (q = 2-3) with kinetic energy up to 150 eV were observed in the mass spectra. Strong evidences Support that these ions are formed in the Coulomb explosion of multicharged benzene cluster ions. (C) 2004 Elsevier B.V. All rights reserved.

Determination of organophosphate and carbamate pesticides based on enzyme inhibition using a pH-sensitive fluorescence probe

A flow injection system for the determination of organophosphate and carbamate pesticides is described. A sensitive fluorescence probe was synthesized and used as the pH indicator to detect the inhibition of the enzyme acetylcholinesterase (ACNE). The percentage inhibition of enzyme activity is correlated to the pesticide concentration. Several parameters influencing the performance of the system are discussed. The detection limits of 3.5, 50, 12 and 25 mug/l for carbofuran, carbaryl, paraoxon and dichlorvos, in pure water, respectively were achieved with an incubation time of 10 min. A complete cycle of analysis, including incubation time, took 14 min. The detection system has been applied to the determination of carbofuran in spiked vegetable juices (Chinese cabbage and cole), achieving recovery values between 93.2 and 107% for Chinese cabbage juice and 108 and 118% for cole juice at the different concentration levels assayed. (C) 2004 Elsevier B.V. All rights reserved.

Synthesis and characterization of carbon black supported Pt-Ru alloy as a model catalyst for fuel cells

A set of bimetallic Pt-Ru catalysts prepared by co-impregnation of carbon black with ruthenium(III) chloride hydrate and hydrogen hexachloroplatinate(IV) hydrate were investigated by temperature-programmed reduction (TPR), chemisorption of hydrogen, transmission electron microscopy (TEM), microcalorimetry of adsorbed CO and a structure-sensitive reaction (n-hexane conversion). The results showed that the volumetric capacities for CO and H-2 adsorption is influenced in the bimetallic Pt-Ru catalysts by the formation of a Pt-Ru alloy. The n-hexane reaction revealed that the reaction mechanism for the pure Pt catalyst mainly occurs via cyclic isomerization and aromatization due to the presence of bigger Pt surface ensembles, whereas the Pt-Ru catalysts exhibited predominantly bond-shift isomerization by the diluting effect of Ru metal addition. The differential heats of CO chemisorption on Pt-Ru catalysts fell between the two monometallic Pt and Ru catalysts extremes. (C) 2004 Elsevier B.V. All rights reserved.

The PPh3 ligand modified Rh/SiO2 catalyst for hydroformylation of olefins

A novel family of hybrid catalyst with high turnover frequency (TOF) and high selectivity towards aldehydes for hydroformylation of olefins could be successfully approached through direct coordination with the PPh3 ligand to the highly dispersed Rh metal particle precursors. A further advantage is that the catalyst is easily prepared and recyclable. The results revealed that hydroformylation of olefins to aldehydes dominantly took place on the surface of PPh3 ligand modified Rh metal particles of the hybrid catalyst. It was found that the formation of chemical coordination bond between the Rh metal particles and the lone-pair electron of PPh3 was evident through the TG and P-31 NMR measurement. Moreover, the addition of PPh3 onto the Rh/SiO2 exert a significant influence on the adsorption state of reactant CO, H-2 and C2H4 on the PPh3-Rh/SiO2 sample, which probably lead to good catalytic performances for hydroformylation of olefins. (C) 2004 Elsevier B.V. All rights reserved.

Preparation and characterization of microencapsulated hexadecane used for thermal energy storage

Polyurea microcapsules about 2.5 mum in diameter containing phase change material for thermal energy storage application were synthesized and characterized by interfacial polycondensation method with toluene-2,4-diisocyanate and ethylenediamine as monomers in an emulsion system. Hexadecane was used as a phase change material and OP, which is nonionic surfactant, and used as an emulsifier. The chemical structure and thermal behavior of the microcapsules were investigated by FTIR and thermal analysis respectively. The results show encapsulated hexadecane has a good potential as a solar energy storage material.

Microencapsulation of n-eicosane as energy storage material

For heat energy storage application, polyurea. microcapsules containing phase change material, n-eicosane, were synthesized by using interfacial polymerization method with toluene- 2,4-diisocyanate (TDI) and diethylenetriamine (DETA) as monomers in an emulsion system. Poly(ethylene glycol)octyl-phenyl ether (OP), a nonionic surfactant, was the emulsifier for the system. The experimental result indicates that TDI was reacted with DETA in a mass ratio of 3 to 1. FT-IR spectra confirm the formation of wall material, polyurea, from the two monomers, TDI and DETA. Encapsulation efficiency of n-eicosane is about 75%. Microcapsule of n-eicosane melts at a temperature close to that of n-eicosane, while its stored heat energy varies with core material n-eicosane when wall material fixed. Thermo-gravimetric analysis shows that core material n-eicosane, micro-n-eicosane and wall material polyurea can withstand temperatures up to 130, 170 and 250 degreesC, respectively.

Preparation of stir bars for sorptive extraction using sol-gel technology

A sol-gel coating method for the preparation of extractive phase on bars used in sorptive microextraction is described. The extraction phase of poly(dimethylsiloxane) is partially crosslinked with the sol-gel network, and the most part is physically incorporated in the network. Three aging steps at different temperatures are applied to complete the crosslinking process. Thirty-micrometer-thick coating layer is obtained by one coating process. The improved coating shows good thermal stability up to 300degreesC. Spiked aqueous samples containing n-alkanes, polycyclic aromatic hydrocarbons and organophosphorus pesticides were analyzed by using the sorptive bars and GC. The results demonstrate that it is suitable for both aploar and polar analytes. The detection limit for chrysene is 7.44 ng/L, 0.74 ng/L for C-19 and 0.9 ng/L for phorate. The extraction equilibration can be reached in less than 15 min by supersonic extraction with the bars of 30 mum coating layer. (C) 2004 Elsevier B.V. All rights reserved.

Study of an electroosmotic pump for liquid delivery and its application in capillary column liquid chromatography

A packed-bed electroosmotic pump (EOP) was constructed and evaluated. The EOP consisted of three capillary columns packed in parallel, a gas-releasing device, Pt electrodes and a high-voltage power supply. The EOP could generate output pressure above 5.0 MPa and constant flow rate in the range of nl/min to a few mul/min for pure water, pure methanol, 2 mM potassium dihydrogenphosphate buffer, the buffer-methanol mixture and the pure water-methanol mixture at applied potentials less than 20 W The composition of solvent before/after pumping was quantitatively determined by using a gas chromatograph equipped with both flame ionization detector and thermal conductivity detector. It was found that there were no apparent changes in composition and relative concentrations after pumping process for a methanol-ethanol-acetonitrile mixture and a methanol-water mixture. Theoretical aspect of the EOP was discussed in detail. An capillary HPLC system consisting of the EOP, an injection valve, a 15 cm x 320 mum i.d., 5 mum Spherigel C(18) stainless steel analytical column, and an on-column UV detector was connected to evaluate the performance of the EOP. A comparative study was also carried out with a mechanical capillary HPLC pump on the same system. The results demonstrated that the reproducibility of flow rate and the pulsation-free flow property of the EOP are superior to that of mechanical pump in capillary HPLC application. (C) 2004 Elsevier B.V. All rights reserved.

Preparation and characterization of long methacrylate monolithic column for capillary liquid chromatography

Long methacrylate monolithic columns (100 cm x 320 mum i.d.) were prepared from silanized fused-silica capillaries of 320 mum i.d. by in situ copolymerization of butyl methacrylate (BMA) with ethylene dimethacrylate (EDMA) in the presence of a suitable porogen. The separation performance and selectivity of the column were evaluated and compared with a 25 cm x 320 mum i.d. column prepared in the same way by capillary high-performance liquid chromatography (mu-HPLC) The results showed that the 1 m long monolithic column can generate 33 x 10(3) plate number and exhibited good permeability, higher sample loadability, and separation capability. (C) 2004 Elsevier B.V. All rights reserved.

Development of functionalized terbium fluorescent nanoparticles for antibody labeling and time-resolved fluoroimmunoassay application

Silica-based functionalized terbium fluorescent nanoparticles were prepared, characterized and developed as a fluorescence probe for antibody labeling and time-resolved fluoroimmunoassay. The nanoparticles were prepared in a water-in-oil (W/O) microemulsion containing a strongly fluorescent Tb3+ chelate. N,N.N-1,N-1-12,6-bis(3'-aminomethyl-1'-pyrazolyl)phenylpyridine] tetrakis(acetate)-Tb3+ (BPTA-Tb3+), Triton X-100, octanol, and cyclohexane by controlling copolymerization of tetraethyl orthosilicate (TEOS) and 3-[2-(2- aminoethylamino)-ethylamino]propyl-trimethoxysilane (AEPS) with ammonia water. The characterizations by transmission electron microscopy and fluorometric quantum methods show that the nanoparticles are spherical and uniform in size, 45 +/- 3 nm in diameter, strongly fluorescent with fluorescence yield of 10% and a long fluorescence lifetime of 2.0 ms. The amino groups directly introduced to the nanoparticle's surface by using AEPS in the preparation made the surface modification and bioconjugation of the nanoparticles easier. The nanoparticle-labeled anti-human alpha-fetoprotein antibody was prepared and used for time-resolved fluoroimmunoassay of (x-fetoprotein (AFP) in human serum samples. The assay response is linear from 0.10 ng ml(-1) to about 100 ng ml(-1) with the detection limit of 0.10 ng ml(-1). The coefficient variations (CVs) of the method are less than 9.0%. and the recoveries are in the range of 84-98% for human serum sample measurements. (C) 2004 Elsevier B.V. All rights reserved.