摘要
自从美国9/11事件之后,提高安全性和预防损伤的必要性比以往任何时候都重要。世界各地的恐怖主义威胁和数百万埋在地下未爆炸的地雷需要开发一种能够快速,可靠和紧凑的爆炸物检测设备,它应被纳入到手持设备或远程监控设备。考虑到普遍采用的爆炸装置大多数没有密封屏蔽,因此通过检测空气中的爆炸物分子来确定爆炸物的存在成为可能。但传感器设备进行检测的关键问题是环境条件下灵敏度低。这是由于常用的硝基炸药(TNT,硝酸甘油,DNT,黑索金,特屈儿等)本身的蒸汽压很低,而自然空气流动使浓度进一步稀释至更低的ppt或ppb级。在大型开放地域,如机场、火车站,即使是最好的传感器也很难检测这种经过稀释的低浓度爆炸物分子。一个简单而有效的解决方案是为传感器设计一个预浓缩装置,以提高检测灵敏度。
由于其孔道尺寸和吸附选择性,分子筛膜近几十年来被用于气体分离。其中的MFI结构的分子筛膜具有0.51-0.56nm的孔道直径,由于其孔道直径小于爆炸物分子而大于空气分子而被用作分子筛膜材料。而一层超薄的分子筛膜应该能够过滤掉空气分子而使爆炸物蒸汽浓缩。由于分子筛膜的通量足够大,使得其能在短时间内流过大量空气分子,快速浓缩爆炸物分子,从而使传感器能够检测超低浓度(ppt或更低)的爆炸物。
本课题采用二次生长法在多孔不锈钢,多孔镍和α-Alumina载体表面合成了无缺陷的薄沸石分子筛膜,经过热焙烧或紫外线处理后,表征其渗透速率和对爆炸性分子的浓缩效率。为了避免膜在高温焙烧时开裂,采用UV/Ozone处理方法在较低温度下脱除分子筛内的有机模板剂。选用1,3,5-三甲苯(TMB)分子作为模型化合物,通过分离氮气与TMB的混合气体检测膜的选择性。通过文献检索,这是首次采用分子筛膜进行TMB、氮气二元混合物分离的工作。
与分子筛膜在载体一侧的单侧膜相比,分子筛膜在载体两侧的样品测得的选择性和渗透率较高。采用较大孔径的载体制备的膜可减少载体阻力,从而增加渗透率。经UV处理的α-Alumina支撑的双层膜具有最高的氮气通量(13.5mmol/m2·s)和选择性(10600)。
有机官能化是一种对分子筛表面进行改性的有效方法。硅烷试剂与分子筛表面的羟基基团反应不仅能够提高分子筛膜的疏水性能,还能提高疏油性能。采用纯碳氟链的硅烷试剂有机官能化的分子筛膜比采用一般硅烷试剂拥有更高的疏水性能。疏水层的疏水角在130°-150°之间。由于ZSM-5有更强的羟基基团,其有机官能化后的疏水角高于同样条件下处理的Silicalite-1分子筛膜。且分子筛上的有机官能团具有较好的耐热性,能够耐300°C高温过程。有机官能化对分子筛膜分离渗透率或选择性影响不明显,但可增加膜分离含有强吸附有机物的混合气体或湿空气时的耐久性。另外,载体的性能也会影响分离层的耐久性,且烷基化α-Alumina支撑的分子筛膜的耐久性优于多孔镍支撑的分子筛膜。
After the tragic events of9/11in US, the need for increased security and damageprevention is now more sought out than ever. Terrorist threats and millions ofunexploded land mines buried around the world necessitate the development ofequipment for explosives detection that is rapid, reliable and compact enough to beincorporated into a hand-held device or a remote surveillance device. If can beconsidered the commonly employed devices, most are also not shielded hermetically,it is possible to detect the explosives molecular by a sensor. The critical problem fordetection by a sensor device is the low sensitivity caused by the low to ultra-lowconcentrations of nitro compounds under ambient conditions. The most commonlyused nitro-based explosives (TNT, NG, DNT, RDX, Tetryl, etc.) possess a smallvapor pressure. Furthermore, natural air movements dilute ppb level to ppt or evenlower. This problem is exacerbated in large and open areas, such as airports and trainstations, where even the best-engineered sensors will have a hard time detecting suchlow concentrations. A simple and effective solution is to design a preconcentrator forsensor device to improve sensitivity.
Zeolite membranes have been developed for use in gas separation in recentdecades according to their pore size and selective adsorption. MFI type zeolite isconsidered as a promising membrane material for explosives separation because itspore size (0.51-0.56nm) is smaller than explosives molecules but much larger than aircomponents. Consequently, an ultrathin molecular sieving zeolite membrane couldfilter an air sample and serve as an explosives vapor concentrator. The membraneswill allow a large flux of air, thus leading to a concentration of the explosives vaporsby a large factor in a short time and will allow the detection of ultra-lowconcentrations (ppt or lower).
The aim of this work is to synthesize continuous, pinhole-free, ultra thinmolecular sieving zeolite membranes with suitable pore sizes by a seeded growthmethod on porous stainless steel, porous nickel or α-Alumina substrates. Themembranes, after thermal calcination or UV-treatment, will be characterized in termsof their permeation rates and concentration efficiency for explosive molecules. Toavoid membrane cracking during high temperature calcination, an UV/ozone treatment method is employed as a low temperature alternative to remove the organictemplate. To examine the selectivity of the membrane,1,3,5-Trimethylbenzene (TMB)has been used as a surrogate of the explosive molecule. Toward that end, a mixture ofTMB/nitrogen feed will be used as the testing case for this desired application. To ourknowledge, this is the first application of zeolite membranes for TMB/nitrogen binarymixture separation.
Higher selectivity and permeance are observed for samples with zeolite film onboth sides of the support, as compared to those with zeolite film on only one side ofthe support. In addition, by varying the type of support with different pore structures,it is shown that the support with large pore size can reduce the support resistance, andthereby increasing permeance. UV-treated membranes on both sides of α-Aluminasupport has the highest flux (13.5mmol/m2·s) and selectivity (10600) among allsamples tested.
Furthermore, organic functionalization is a very common and efficient method tomodify the zeolite. Silane was reacted with hydroxyl group on the surface of zeolite,which not only can increase the hydrophobic properties but also the oleophobicproperties of zeolite. Meanwhile, the silane with fluorocarbon chain can furtherincrease the hydrophobic properties of zeolite. The contact angle to water of thehydrophobic coating is range from130to150°. At same condition, organicfunctionalized ZSM-5membranes can get higher contact angle than silicalite-1membranes, due to its stronger hydroxyl groups. Otherwise, the organic functionalgroups can surfer high temperature as high as300°C on the zeolite. Organicfunctionalization cannot dramatically increase the separation permeance or selectivityof zeolite, but can increase the durability of zeolite when separate organic mixture gasor moist air. In addition, the properties of substrate have a significant influence on thedurability of separation film. The durability of nitrogen permeance on silanizedα-Alumina supported zeolite is much better than that on silanized porous nickelsupported zeolite.
引文
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