大粒径疏水催化剂的制备及氧化氚氢(HT)的性能研究

用两段聚合法及溶出致孔剂法分别制备了多孔大粒径苯乙烯－二乙烯基苯和聚四氟乙烯疏水担体;在此基础上,用浸渍法制备了２种大粒径铂疏水催化剂,在室温下研究了它们催化氧化ＨＴ（Ｈ２）的动力学和疏水性能。     

空气除氚系统中氚氧化催化剂的研究进展

在大型氚设施中空气除氚系统必不可少,通过气-水转换除去气态氚是目前应用最广泛也是最有效的工艺,过程中氧化催化剂至关重要。总结了气态氚的催化氧化研究进展、催化剂的催化性能及影响催化性能的主要因素。贵金属Pt和Pd在室温下对氚的转化效率接近100%,因而被广泛用于氚的催化氧化。通过负载分散载体、添加催化助剂、使用规整结构催化剂、设计新型的催化反应器能够进一步提高催化剂性能。以蜂窝状催化剂为研究热点的规整结构催化剂以其高比表面积和低压力降而显示出良好的催化性能,将它用于氚的催化氧化,是该领域的一个研究方向。氢、氘、氚在氧化过程中的同位素效应会影响除氚效率,需进行深入研究。     

催化加成氚代苯乙烯制备研究

以林德拉催化剂替代普通钯碳催化剂,利用氘气替代氚气模拟研究搅拌程度、温度、投料比对氚代苯乙烯加成反应转化率和选择性的影响。结果表明,较高的搅拌速度和温度可以提高催化加成反应的转化率,但对选择性影响较小;氘气加入量对转化率和选择性影响较大,不足或过量都会影响氘代苯乙烯的纯度;林德拉催化剂对苯乙烯的选择性高于钯碳催化剂。     

强流中子发生器除氚净化装置的研制

本文在研究、确定除氚工艺参数的基础上,研制成强流中子发生器除氚净化装置。该装置采用两级串接方式,在200℃温度下净化因子不低于10~4。     

疏水催化剂用于水中氚回收的实验研究

本文简要介绍采用自制的几种疏水催化剂进行的室温Ｈ－Ｔ同位素交换实验，初步考察了氢气流速对催化活性的影响。实验表明，催化剂的催化活性较高，能够用于室温下从氚水中回收氚。     

Ni基催化剂的氢-水汽相催化交换性能

汽相催化交换(VPCE)是水除氚的重要手段之一,本研究采用金属Ni替代常用的贵金属Pt作为逆流型VPCE工艺的催化剂,研究了其在多种实验条件下HDO-H2反应体系中的静态及动态催化交换性能。实验结果表明:静态实验时,催化剂在温度大于200℃、压力和反应物浓度的摩尔比值(HDO∶H2)越大的条件下,催化交换反应向正方向移动,催化性能更好;在Ni高负载率的情况下,其催化性能优于Pt基催化剂。动态实验时,产物平衡氘浓度与静态实验一致,H2中氘摩尔浓度均为1%左右;且进料比例对结果的影响规律与静态实验一致,反应物HDO越多,产物氘浓度越大。本研究表明了纯Ni催化剂在HDO-H2催化交换反应体系中有着较为明显的催化作用,可以替代传统贵金属Pt作为逆流型VPCE工艺的催化剂。     

可移动式除氚器的现场应用试验

在现场闭路循环工作模式下，采用中国辐射防护研究院研制的小型可移动式除氚器对微量(（0.5~1）×10^-6)气态氚进行脱氚试验。试验结果表明：催化床在450℃工作温度下，空气闭路循环流量为3.8m³/h时，除氚器可在114min内将1m³密封不锈钢罐空气中的氚浓度由4.62×10⁶Bq/L降至4.62×10³Bq/L。同时，论证了除氚器在现场使用的适应性与安全性，并对其研制和现场性能试验中发现的技术问题进行了论述。     

带自动控制功能的除氚系统

针对氚工艺尾气处理的需求和源项实际情况,根据化工原理和氚特性设计含自动控制功能除氚系统的主要部件、自动控制功能和初步性能测试,得出催化反应器、氚水吸附床等部件的结构尺寸,催化剂、干燥吸附剂的装填量等参数及控制软件界面;通过除氘和除氚实验初步测试了除氚系统的处理性能。结果表明,在循环处理模式下,1m3密闭容器中氘体积比6.0×10–4–2.8×10–2范围内时,35min内氘气浓度降低两个量级;5次对30L密闭容器内不同浓度的含氚气体处理,60min内对氚的去除效率均达到95%以上。     

环境样品中自由氚和组织结合氚的收集

本文介绍了所建立的环境样品中的自由氚和组织结合氚的分别采样装置和方法。对于样品中的自由氚,用低真空干燥回收法,回收率可达98％;对于样品中的组织结合氚,用连续加样催化氧化冷凝收集法,回收率为93％。两法都能一次收集足够制两个并行测量样的水量。     

氚标记八厘麻毒素的制备

一、问题的提出据统计,我国成年人中有5%—10%的高血压病患者。严重高血压患者可导致脑溢血、心力衰竭、肾功能衰竭等严重后果而构成我国人口中死亡率最高的疾病之一。然而,对这大量的危重高血压患者却缺少理想的降压药物。八厘麻是我国民间常用的中草药,是主要用于治疗跌打损伤的外用药。1977年武汉医     

Deactivation of Hydrophobic Pt/SDBC Catalyst in the WTRF LPCE Column for Tritium Separation

The styrene divinylbenzene copolymer (SDBC) supported platinum catalyst and the liquid phase catalytic exchange (LPCE) column have been developed to be applicable to the Wolsong tritium removal facility (WTRF) in Korea. The catalyst deactivation subject to both reversible uniform poisoning and permanent loss by impurity poisoning was investigated using a time-on-stream theory and a simplified shell progressive poisoning scenario in special case of higher internal diffusion resistance. Experimental data from fixed bed reactors with the Pt/SDBC catalysts have been used to establish the deactivation model and to estimate key parameters to be used in the WTRF LPCE column design. It was found that an impurity control in the streams would be critical to the WTRF LPCE column operation since the impurity poisoning played a very important role in the overall catalytic exchange reaction. Except for the case of the severe impurity poisoning of the whole catalysts, the LPCE column can be in operation over 10 years without any regeneration of the catalysts.     

Design Study of Feasible Water Detritiation Systems for Fusion Reactor of ITER Scale

Two types of water detritiation systems have been designed for fusion reactors of ITER scale. One of the systems is a combination of WD (Water Distillation) and VPCE(vapor phase catalytic exchange) columns. The other is a combination of a WD column and a CECE(combined electrolysis catalytic exchange) column. Three water distillation columns are needed for the former system. The total height of the three columns is 106 m. The height of the water distillation and CECE columns for the latter system are 20 and 24m, respectively. These large water distillation columns result in the larger tritium inventory of the former system than for the latter system. However, there have been the results for the operation of the actual scale of the water distillation and VPCE columns. No demonstration test has been carried out for the CECE column. From these reasons, the WD+VPCE system should be the first candidate for the fusion reactor. The WD+CECE system is superior to the WD+VPCE system for the flexibility in design as well as the tritium inventory. It is desired to demonstrate the CECE column to develop the water detritiation system best suited to the fusion reactors.     

联合电解催化交换系统的动态模型及理论计算

为探求联合电解催化交换系统各单元中氚浓度空间分布和动态变化的内在规律，建立了D／T体系的气-液两元模型。根据不同的催化剂传质性能，计算了为达到特定脱氚率和电解池浓缩倍数所要求的交换床总高度和进液位置。理论计算得到的氚在交换床上的空间分布趋势与文献报道的中试结果一致，电解池中的氚浓度随时间呈线性增长。     

Catalytic Oxidation of Tritium in Wet Gas

Use of precious metal catalyst is recommended in the tritium recovery system because it can oxidize tritium at ambient temperature. The ability to operate at the ambient temperature without preheating and past cooling is a large advantage in the ease of system operation. It is observed in this study, however, that the catalytic oxidation characteristics of the precious metal catalysts are largely affected by the water vapor to such extent that almost no oxidation rate of tritium is expected in the wet gas. Effect of the water vapor on the oxidation rate is quantitatively discussed based on data obtained in this study and an emergency cleanup system from the room air with pre-adsorption bed is proposed.     

Detritiation of Glovebox Atmosphere by Using Compact Tritium Removal Equipment

A compact tritium removal equipment (TRE), assembled in a console with casters, has been developed for detritiation of air in a glovebox used for handling of several curies of tritium. The TRE was designed to remove gaseous tritium in the form of T₂, HT and CH₃T through oxidation with precious metal/alumina catalysts followed by adsorption on zeolite pellets.

From the detritiation experiments with hydrogen tritide (HT, 2–20 mCi), the TRE was confirmed to have sufficient performance for the practical use. The tritium concentration in the test gas (total volume –32l; 1%H₂, 5%O₂, 94%N₂) decreased from 0.64 to 6.4 ×10-⁷ Ci.m³ within 155 min when the TRE was operated under the recirculation mode with the flow rate of 200 l-h¹ at the catalyst temperature of 200°C. In addition, the HT-to-HTO fractional conversion was determined at various catalyst temperatures (25–200°C) and flow rates (100–360 lh-¹).     

φ6mm Pt-PTFE疏水催化剂的研制

在研制粒径为6mm的多孔PTFE疏水担体基础上,采用浸渍法研制了可在工程上应用的Pt PTFE疏水催化剂。室温下,在并流催化床上考察了该疏水催化剂的催化活性、疏水性能和催化剂上活性粒子的稳定性。结果表明:当氚浓度为153Bq/mL,氢气线速度为5.31cm/s和15.93cm/s时,水中氚的催化转化率分别为73.7%和69.6%。在用普通水浸泡并淋洗145d后,该疏水催化剂的催化活性和活性粒子(Pt)的含量无明显变化。     

用于LPCE的有序床催化剂催化活性研究

采用气-液逆流方式研究了Pt/C/PTFE有序床疏水催化剂对H_2(g)/HDO(l)体系中同位素交换的催化性能。结果表明:Pt/C/PTFE有序床催化剂不仅具有较高的催化活性和良好的疏水性,而且能够达到很高的气体流速;实验所用的两种Pt/C/PTFE的体积传质系数(K_(ya))均达1.12m~3(STP)/(s·m~3)(50mol/(m~3·s))以上,且用水浸泡35d后其催化活性无明显变化;在气液摩尔比为1∶1的条件下,气体空塔线速率达到1.0m/s时,两种填装的有序床Pt/C/PTFE均未发生液泛。     

Recovery of Tritium in Room Air by Precious Metal Catalyst with Hydrophilic Substrate

The catalytic oxidation and adsorption method is considered to be a potential and reliable measure to recover tritium released into room air in fusion power plants. The activity of precious metal catalysts that are expected to be useful in recovery of tritium released into the room air is affected by moisture in the air, and tritium in the gas phase can be captured into the catalyst substrate not only through adsorption but also through isotopic exchange reaction. The simulation study on tritium behavior in the catalyst bed was carried out quantitatively on the basis of experimental results. It is confirmed by the simulation study that the installation of the preadsorption bed decreases water vapor before the gas is passed through the precious metal catalyst bed; this is an effective countermeasure against the deterioration of the catalytic oxidizing performance caused by moisture. It is also shown that large amounts of tritium can be captured by the catalyst itself when the preadsorption bed is introduced.