载体法高效驱杀蚊整理模型的建立及其应用研究
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摘要
蚊子是与人类生活和健康关系极为密切的昆虫之一,除了直接叮刺、骚扰外,还可传播多种疾病。研究表明有60多种疾病可通过蚊虫传播,如疟疾、丝虫病、黄热病和登革热等。如今在发展中国家,尤其是在非洲国家,每年大约有一亿多的疟疾新发病例,大约有100多万人死于疟疾,而且大多数是儿童和孕妇；中国地处亚热带地区虽未遭受因蚊虫传染带来的大规模伤害,但人们也深受蚊虫的困扰。因此,驱杀蚊整理是目前最需迫切解决的问题之一,本论文就驱杀蚊试剂在纺织品中的应用及理论模型的建立进行研究。
本论文首先研究了驱杀蚊试剂的实际应用情况,根据其物化性质选用载体法制备高效驱杀蚊织物。比较了不同驱杀蚊试剂和载体对制备高效驱杀蚊织物的影响,发现OP为最佳载体,ZX-1(主要成分为2,2-双(4-氯苯基)-1,1,1-三氯乙烷)为最佳驱杀蚊试剂。制备过程首先以萃取分离法对ZX-1的原料预处理,通过两步法分离提纯ZX-1原料,并以驱杀蚊试剂ZX-1、环己烷、载体OP、分散剂NNO为原料处理涤纶织物,获得载体整理最佳工艺为：ZX-10.6g/L(3%,o.w.f),Mzx-1：M环己烷为1：1.6,载体OP3g/L,分散剂NNO0.5g/L,90℃处理90min,浴比为1：50。通过对经ZX-1载体整理后驱杀蚊涤纶织物的结构分析得出如下结论：ZX-1附着于纤维表面,并且进入涤纶纤维内部无定形区；涤纶织物的结晶度随着整理剂ZX-1浓度的增加而增加,同时驱杀蚊实际ZX-1不会影响纤维的晶形结构和涤纶织物的热稳定性；从而获得长期有效驱杀蚊涤纶织物。
本论文还研究了涤纶纤维对ZX-1的吸附性能及扩散机理研究。ZX-1不溶于水,涤纶纤维在常温常压下很难吸附ZX-1,选用载体法可有效吸附ZX-1。载体小分子较快地向纤维内部扩散并以范德华力或氢键的方式与纤维结合,减弱了纤维间的结合力,增大了大空穴产生的几率,提高ZX-1的扩散速度。吸附过程中ZX-1向纤维表面的扩散属于在湍流层中的扩散,其扩散边界层很薄；ZX-1在纤维中的扩散属于自由容积扩散,扩散系数随着涤纶纤维的自由容积变化而变化,遵循逐个孔穴“跳跃”扩散,最终提高ZX-1的扩散速率。
目前针对防蚊织物的研究主要集中在织物防蚊性能表征方面,而对其理论研究比较少,本论文探讨并建立了涤纶纤维吸附ZX-1过程中吸附模型。研究发现,涤纶纤维吸附ZX-1的吸附量随着温度的升高而增加；吸附时间的延长而吸附量增加速度减缓,直至达到饱和吸附。动力学(一级吸附动力学、二级吸附动力学和粒子间扩散吸附模型)和热力学模型(能斯特、朗格缪尔、弗里德利胥和D-R模型)研究表明,涤纶对ZX-1的吸附动力学模型符合二级动力学吸附模型,吸附热力学模型符合Langmuir等温吸附模型。涤纶吸附ZX-1的热力学参数吉布斯自由能变△G°和吸附活化能Ea同时说明涤纶纤维对zx-1的吸附过程属于较易发生的自发进行的过程；吸附焓△H°和吸附熵△S°表明涤纶纤维对ZX-1的吸附过程为放热,被纤维吸附的ZX-1较难从纤维上解吸。
本论文选用实验室驯化饲养的92代淡色库蚊作为实验对象,在实验室环境内对库蚊在织物上的行为学进行研究。实验结果表明,最佳测试条件为：羽化时间为3天的雌性库蚊,测试时间为晚上6-9点,引诱剂为浓度5%的C02气体,室内无自然光。通过对经过ZX-1载体整理后的驱杀蚊涤纶织物的实际驱蚊效果的测试得出如下结论：随着ZX-1浓度的增加,羽化天数为3天的雌性库蚊的活力最强,雌蚊对防蚊织物的趋避效应最明显；且测试时间的延长使得雌蚊对ZX-1的耐受度降低,活动力降低。随着水洗次数的增加,其驱蚊效果略微下降,但整体降低幅度不大；随着处理织物中ZX-1浓度的增加,雌蚊停留在水洗后织物的数目也随之降低,与未水洗的防蚊织物测试效果相比仍呈现一定的线性规律。
Mosquitoes are one of insects affecting humans'life and health significantly. Mosquito not only has direct barbed bite and harassment, but also transmits more than60diseases, such as malaria, dengue fever, filariasis, yellow fever et al. Now, in developing country, especially African country, almost one hundred million malaria diseases erupt, about one million people died because of malaria, most of children and pregnant women. Although, China haven't suffer for mass harm for mosquito transmission, people also puzzle for mosquito biting. Therefore, anti-mosquito finishing is one of the most urgent and critical problems to solve. This thesis is focus on researching the application of anti-mosquito textile and their theory.
Firstly, this thesis research on actual applied condition of anti-mosquito reagents. According to physicochemical properties of anti-mosquito reagents, carrier finishing method is the optimal method to produce high effecient anti-mosquito textile. Having compared different reagents and carriers which affected anti-mosquito textile producing, we found that OP and ZX-1(main component was2,2-bis(4-Chlorophenyl)-1,1,1-trichloroethane) were the best carrier and reagent. Then, pretreated ZX-1raw material by using extraction separation with two method to purify ZX-1. Effects of the dosage of pesticide, ZX-1, the reactive temperature and time, and the dosage of additives on the anti-mosquito textile finishing were discussed. These data showed that, the optimal treatment process was the concentration of ZX-10.6g·L-1(3%, o.w.f), ZX-1to cyclohexane mass ratio1:1.6, the concentration of carrier3g· L-1, the concentration of dispersing agent NNO0.5g·L-1, bath ratio1:50, with1.5hour under90℃. Researching on Structural analysis of anti-mosquito textile after ZX-1by carrier finishing, these results showed that ZX-i were treated on the surface of polyester fiber, and entered into amorphous regions of polyester fibers'interior; the degrees of crystallinity of polyester fiber after ZX-1anti-mosquito treatment were increased with increasing ZX-1concentrations, simultaneously, ZX-1treatment did not particularly affect the size and shape of crystallites in the polyester fiber; ZX-1treatment also didn't influence thermostability of polyester fiber, finally, obtained long time high anti-mosquito textile.
Adsorption Properties of polyester fiber absorbing ZX-1and diffusion mechanism were studied. This study included that ZX-1was water-fast and could not come into fibers'interior under normal temperature and pressure, so we chose carrier method to effectively absorb ZX-1into polyester fibers' inner. We found carrier micromolecule quickly diffused into fibers'interior and combined with fiber by Van der waals'force or hydrogen bond, weakened the bond between fibers, increased odds of big cavities to appear and improved diffusion velocity of ZX-1. By the way, ZX-1diffusion on fibers' surface was belong to turbosphere diffusion, its diffusionboundarylayer was very thin; ZX-1diffusion on fibers'inner was belong to free volume diffusion, and its diffusion coefficient increased with free volumes of polyester fiber increasing, it followed with one by one cavity "jump" diffusion, finally improved diffusion rate of ZX-1.
At present, anti-mosquito textiles are focused on textile properties characterization, however, theoretical study rare dicusses. Thus, the thesis researched on adsorption thermodynamics and kinetics model when polyester fiber adsorbed ZX-1process. These results showed that ZX-1concentration on the fiber increased with increasing the ZX-1concentration in solution until it reached the saturation value. According to kinetics model (first-order adsorption kinetics, the pseudo-second-order adsorption kinetics and an intra-particle diffusion model) and thermodynamic model (Nernst, Langmuir, Freundlich and Dubinin-Radushkevich (D-R) isotherm model), the second-order-model was found most suitable to describe the kinetic diffusion process; Langmuir model appears to fit the adsorption of ZX-1on polyester fibers better than other adsorption models. In addition, thermodynamic parameters such as free energy (AG) and adsorption activation energy (Ea) were all showed that this adsorption process was geared to spontaneous adsorption process; enthalpy (△H°) and entropy (AS) were indicated that this adsorption process was exothermic process, and ZX-1which is absorbed by polyester fiber, was hard to desorb form polyester fiber inner.
Another important part of the thesis is to study on mosquito behavior on the anti-mosquito textile in the laboratory with92generation culex as experimental subject, which was naturalized. These data showed that the optimal test condition were female cluex with3emergence day, texting time6-9PM, the concentration of attractant5%CO2, non-natural light. Actual anti-mosquito effect experiments results with anti-mosquito textile after ZX-1finishing indicated that3emergence day female cluex's activity was the best, and its greater effect was more and more obvious with increasing concentration of ZX-1; however, its suffertibility and activities became lower with testing time extending. furthermore, anti-mosquito effect of textiles after washing was appreciably reduced when increasing washing time, but the reducing range was small; number of female cluex staying on the textiles after washing was appreciably reduced with the concentration of ZX-1on the anti-mosquitotextile increasing, compared with non-wash textile, there were also appeared with certain linear regular.
本论文首先研究了驱杀蚊试剂的实际应用情况,根据其物化性质选用载体法制备高效驱杀蚊织物。比较了不同驱杀蚊试剂和载体对制备高效驱杀蚊织物的影响,发现OP为最佳载体,ZX-1(主要成分为2,2-双(4-氯苯基)-1,1,1-三氯乙烷)为最佳驱杀蚊试剂。制备过程首先以萃取分离法对ZX-1的原料预处理,通过两步法分离提纯ZX-1原料,并以驱杀蚊试剂ZX-1、环己烷、载体OP、分散剂NNO为原料处理涤纶织物,获得载体整理最佳工艺为：ZX-10.6g/L(3%,o.w.f),Mzx-1：M环己烷为1：1.6,载体OP3g/L,分散剂NNO0.5g/L,90℃处理90min,浴比为1：50。通过对经ZX-1载体整理后驱杀蚊涤纶织物的结构分析得出如下结论：ZX-1附着于纤维表面,并且进入涤纶纤维内部无定形区；涤纶织物的结晶度随着整理剂ZX-1浓度的增加而增加,同时驱杀蚊实际ZX-1不会影响纤维的晶形结构和涤纶织物的热稳定性；从而获得长期有效驱杀蚊涤纶织物。
本论文还研究了涤纶纤维对ZX-1的吸附性能及扩散机理研究。ZX-1不溶于水,涤纶纤维在常温常压下很难吸附ZX-1,选用载体法可有效吸附ZX-1。载体小分子较快地向纤维内部扩散并以范德华力或氢键的方式与纤维结合,减弱了纤维间的结合力,增大了大空穴产生的几率,提高ZX-1的扩散速度。吸附过程中ZX-1向纤维表面的扩散属于在湍流层中的扩散,其扩散边界层很薄；ZX-1在纤维中的扩散属于自由容积扩散,扩散系数随着涤纶纤维的自由容积变化而变化,遵循逐个孔穴“跳跃”扩散,最终提高ZX-1的扩散速率。
目前针对防蚊织物的研究主要集中在织物防蚊性能表征方面,而对其理论研究比较少,本论文探讨并建立了涤纶纤维吸附ZX-1过程中吸附模型。研究发现,涤纶纤维吸附ZX-1的吸附量随着温度的升高而增加；吸附时间的延长而吸附量增加速度减缓,直至达到饱和吸附。动力学(一级吸附动力学、二级吸附动力学和粒子间扩散吸附模型)和热力学模型(能斯特、朗格缪尔、弗里德利胥和D-R模型)研究表明,涤纶对ZX-1的吸附动力学模型符合二级动力学吸附模型,吸附热力学模型符合Langmuir等温吸附模型。涤纶吸附ZX-1的热力学参数吉布斯自由能变△G°和吸附活化能Ea同时说明涤纶纤维对zx-1的吸附过程属于较易发生的自发进行的过程；吸附焓△H°和吸附熵△S°表明涤纶纤维对ZX-1的吸附过程为放热,被纤维吸附的ZX-1较难从纤维上解吸。
本论文选用实验室驯化饲养的92代淡色库蚊作为实验对象,在实验室环境内对库蚊在织物上的行为学进行研究。实验结果表明,最佳测试条件为：羽化时间为3天的雌性库蚊,测试时间为晚上6-9点,引诱剂为浓度5%的C02气体,室内无自然光。通过对经过ZX-1载体整理后的驱杀蚊涤纶织物的实际驱蚊效果的测试得出如下结论：随着ZX-1浓度的增加,羽化天数为3天的雌性库蚊的活力最强,雌蚊对防蚊织物的趋避效应最明显；且测试时间的延长使得雌蚊对ZX-1的耐受度降低,活动力降低。随着水洗次数的增加,其驱蚊效果略微下降,但整体降低幅度不大；随着处理织物中ZX-1浓度的增加,雌蚊停留在水洗后织物的数目也随之降低,与未水洗的防蚊织物测试效果相比仍呈现一定的线性规律。
Mosquitoes are one of insects affecting humans'life and health significantly. Mosquito not only has direct barbed bite and harassment, but also transmits more than60diseases, such as malaria, dengue fever, filariasis, yellow fever et al. Now, in developing country, especially African country, almost one hundred million malaria diseases erupt, about one million people died because of malaria, most of children and pregnant women. Although, China haven't suffer for mass harm for mosquito transmission, people also puzzle for mosquito biting. Therefore, anti-mosquito finishing is one of the most urgent and critical problems to solve. This thesis is focus on researching the application of anti-mosquito textile and their theory.
Firstly, this thesis research on actual applied condition of anti-mosquito reagents. According to physicochemical properties of anti-mosquito reagents, carrier finishing method is the optimal method to produce high effecient anti-mosquito textile. Having compared different reagents and carriers which affected anti-mosquito textile producing, we found that OP and ZX-1(main component was2,2-bis(4-Chlorophenyl)-1,1,1-trichloroethane) were the best carrier and reagent. Then, pretreated ZX-1raw material by using extraction separation with two method to purify ZX-1. Effects of the dosage of pesticide, ZX-1, the reactive temperature and time, and the dosage of additives on the anti-mosquito textile finishing were discussed. These data showed that, the optimal treatment process was the concentration of ZX-10.6g·L-1(3%, o.w.f), ZX-1to cyclohexane mass ratio1:1.6, the concentration of carrier3g· L-1, the concentration of dispersing agent NNO0.5g·L-1, bath ratio1:50, with1.5hour under90℃. Researching on Structural analysis of anti-mosquito textile after ZX-1by carrier finishing, these results showed that ZX-i were treated on the surface of polyester fiber, and entered into amorphous regions of polyester fibers'interior; the degrees of crystallinity of polyester fiber after ZX-1anti-mosquito treatment were increased with increasing ZX-1concentrations, simultaneously, ZX-1treatment did not particularly affect the size and shape of crystallites in the polyester fiber; ZX-1treatment also didn't influence thermostability of polyester fiber, finally, obtained long time high anti-mosquito textile.
Adsorption Properties of polyester fiber absorbing ZX-1and diffusion mechanism were studied. This study included that ZX-1was water-fast and could not come into fibers'interior under normal temperature and pressure, so we chose carrier method to effectively absorb ZX-1into polyester fibers' inner. We found carrier micromolecule quickly diffused into fibers'interior and combined with fiber by Van der waals'force or hydrogen bond, weakened the bond between fibers, increased odds of big cavities to appear and improved diffusion velocity of ZX-1. By the way, ZX-1diffusion on fibers' surface was belong to turbosphere diffusion, its diffusionboundarylayer was very thin; ZX-1diffusion on fibers'inner was belong to free volume diffusion, and its diffusion coefficient increased with free volumes of polyester fiber increasing, it followed with one by one cavity "jump" diffusion, finally improved diffusion rate of ZX-1.
At present, anti-mosquito textiles are focused on textile properties characterization, however, theoretical study rare dicusses. Thus, the thesis researched on adsorption thermodynamics and kinetics model when polyester fiber adsorbed ZX-1process. These results showed that ZX-1concentration on the fiber increased with increasing the ZX-1concentration in solution until it reached the saturation value. According to kinetics model (first-order adsorption kinetics, the pseudo-second-order adsorption kinetics and an intra-particle diffusion model) and thermodynamic model (Nernst, Langmuir, Freundlich and Dubinin-Radushkevich (D-R) isotherm model), the second-order-model was found most suitable to describe the kinetic diffusion process; Langmuir model appears to fit the adsorption of ZX-1on polyester fibers better than other adsorption models. In addition, thermodynamic parameters such as free energy (AG) and adsorption activation energy (Ea) were all showed that this adsorption process was geared to spontaneous adsorption process; enthalpy (△H°) and entropy (AS) were indicated that this adsorption process was exothermic process, and ZX-1which is absorbed by polyester fiber, was hard to desorb form polyester fiber inner.
Another important part of the thesis is to study on mosquito behavior on the anti-mosquito textile in the laboratory with92generation culex as experimental subject, which was naturalized. These data showed that the optimal test condition were female cluex with3emergence day, texting time6-9PM, the concentration of attractant5%CO2, non-natural light. Actual anti-mosquito effect experiments results with anti-mosquito textile after ZX-1finishing indicated that3emergence day female cluex's activity was the best, and its greater effect was more and more obvious with increasing concentration of ZX-1; however, its suffertibility and activities became lower with testing time extending. furthermore, anti-mosquito effect of textiles after washing was appreciably reduced when increasing washing time, but the reducing range was small; number of female cluex staying on the textiles after washing was appreciably reduced with the concentration of ZX-1on the anti-mosquitotextile increasing, compared with non-wash textile, there were also appeared with certain linear regular.
引文
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