碱土金属盐改性介孔硅材料降低卷烟烟气氨释放量
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摘要
通过浸渍法制备得到碱土金属盐(CaCl_2)改性介孔硅材料,可用于降低卷烟主流烟气中粒相氨和气相氨的释放量。采用X射线粉末衍射分析(XRD)、比表面积孔径分析(BET)、程序升温脱附分析(TPD)等,对制备的CaCl_2改性介孔硅材料进行了结构表征,优化了CaCl_2在介孔硅材料上的负载量,考察了其对卷烟烟气中氨的吸附去除性能,并探讨了该材料降低烟气中氨释放量的机理。结果表明:(1)CaCl_2在介孔硅材料上的较优负载量为25%;(2)在滤嘴中添加CaCl_2改性介孔硅材料,卷烟样品主流烟气中气相氨降低率达到50%以上,粒相氨降低率达到10%以上;(3)CaCl_2负载介孔硅材料降低氨释放量的机理是先利用材料的介孔孔道对氨进行物理捕捉,然后通过CaCl_2与氨发生络合作用实现化学吸附,并且孔道的存在加快了金属离子与NH_3发生物理作用与化学吸附的进程。
The mesoporous silica material modified by alkaline earth salt(CaCl_2) was synthesized by immersion process, which could reduce the ammonia emission from the mainstream smoke of cigarette. The structural characteristics of the CaCl_2-modified mesoporous silica material were analyzed by adopting XRD, BET and TPD analysis, and the loading quantity of CaCl_2 in mesoporous silica material was optimized. In addition, the adsorption removal property of this material to ammonia in cigarette smoke was investigated, and its mechanism of reducing the ammonia emission from cigarette smoke was explored. The results showed that:(1) the optimized loading quantity of CaCl_2 in mesoporous silica material was 25%;(2) after adding CaCl_2-modified mesoporous silica material into the filter tip of cigarettes, the gaseous-phase ammonia content in the mainstream smoke of cigarette samples was decreased by over 50%, and the particulate ammonia content was reduced by more than 10%. The mechanism which CaCl_2-modified mesoporous silica material reduces the ammonia emission from cigarette smoke is as follows: ammonia is physically captured by the pores of this material firstly, then ammonia is chemically adsorbed through the complexation of CaCl_2 with ammonia, and the existence of pore canals accelerates the physical and chemical adsorption process between metal ion and NH_3.
The mesoporous silica material modified by alkaline earth salt(CaCl_2) was synthesized by immersion process, which could reduce the ammonia emission from the mainstream smoke of cigarette. The structural characteristics of the CaCl_2-modified mesoporous silica material were analyzed by adopting XRD, BET and TPD analysis, and the loading quantity of CaCl_2 in mesoporous silica material was optimized. In addition, the adsorption removal property of this material to ammonia in cigarette smoke was investigated, and its mechanism of reducing the ammonia emission from cigarette smoke was explored. The results showed that:(1) the optimized loading quantity of CaCl_2 in mesoporous silica material was 25%;(2) after adding CaCl_2-modified mesoporous silica material into the filter tip of cigarettes, the gaseous-phase ammonia content in the mainstream smoke of cigarette samples was decreased by over 50%, and the particulate ammonia content was reduced by more than 10%. The mechanism which CaCl_2-modified mesoporous silica material reduces the ammonia emission from cigarette smoke is as follows: ammonia is physically captured by the pores of this material firstly, then ammonia is chemically adsorbed through the complexation of CaCl_2 with ammonia, and the existence of pore canals accelerates the physical and chemical adsorption process between metal ion and NH_3.
引文
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[3] 金勇,王诗太,李克,等.卷烟滤嘴在降焦减害中的研究进展[J].烟草科技,2016(11):98-106.
[4] 岳盈溢,朱保昆,黄艳,等.一种新的机械混合法制备Ag(Ⅰ)@β吸附剂及其吸附CO性能[J].中国烟草学报,2016,22(2):14-20.
[5] Kuoyan M A, Yu H J, Dai Y, et al. Synthesis of ZSM-5@ordered mesoporous silica composites by means of dodecylamine surfactant[J]. Journal of Wuhan University of Technology-Mater Sci Ed, 2014, 29(6): 1124-1128.
[6] Yu H J, Dai Y, Zhao D Y, et al. Synthesis of core-shell structured zeolite-A@ mesoporous silica composites for butyraldehyde adsorption[J]. J Colloid Interface Sci, 2014(428): 251-256.
[7] 戴亚,汪长国,朱立军,等.一种复合化生物制剂在卷烟减害中的应用[J].烟草科技,2008(5):5-8.
[8] Deng Q X, Chao Z H, Xie W, et al. Significant reduction of harmful compounds in tobacco smoke by the use of titanate nanosheets and nanotubes[J]. Chem Commun, 2011, 47(21): 6153-6155.
[9] 许峰,叶鸿宇,张建中,等.有机-无机杂化介孔膦酸钛材料降低卷烟烟气有害成分[J].中国烟草学报,2014,20(6):6-11.
[10] 杨智慧,佘世科,宁敏,等.磷酸酯淀粉的制备及其降低卷烟主流烟气中氨效果的研究[J].中国烟草学报,2017,23(3):19-27.
[11] 王俊骅.壳寡糖的化学改性及其对氨和苯酚吸附性能的研究[D].杭州:浙江大学,2017.
[12] 陈庆.直链淀粉的羧化和多孔改性及其对氨和苯酚的吸附性能研究[D].杭州:浙江大学,2017.
[13] 张伟东,胡子曼,唐猷成,等.氨复合吸附剂体系CaBr/硅胶与CaCl2/硅胶比较[J].四川大学学报:自然科学版,2009,46(6):1769-1774.
[14] 段琼,李彬,杨景昌,等.氯化钙在10X分子筛上的微波强化分散及其氨吸附的研究[J].离子交换与吸附,2007,23(1):24-31.
[15] 赖育挺,汤茂辉,刘瑾,等.MgCl2/硅胶氨复合吸附剂的制备研究[J].四川化工,2009,12(1):6-9.
[16] 李力,戴亚,李东亮,等.卷烟主流烟气中氨释放量离子色谱测定方法的改进[J].烟草科技,2016(4):45-52.
[17] Enibe S O, Iloeje O C. Heat and mass transfer in porous spherical pellets of CaCl2 for solar refrigeration[J]. Renewable Energy, 2000, 20(3): 305-324.