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冀钟1,2(), 赵彦玲2,3, 陈雨濛1,2, 高林霞1, 王翼鹏4, 刘欢2,3()
收稿日期:
2024-01-09
修回日期:
2024-03-25
出版日期:
2024-03-29
通讯作者:
刘欢
作者简介:
冀钟(1998—),男,硕士研究生,102110852@hbut.edu.cn
基金资助:
Zhong JI1,2(), Yanling ZHAO2,3, Yumeng CHEN1,2, Linxia GAO1, Yipeng WANG4, Huan LIU2,3()
Received:
2024-01-09
Revised:
2024-03-25
Online:
2024-03-29
Contact:
Huan LIU
摘要:
通过水热法成功合成了一系列宽硅铝比(50、100、150、300、500、800、1500、3000)的ZSM-5分子筛,旨在研究其对涂装行业典型挥发性有机物(volatile organic compounds, VOCs)的吸附规律。同时,结合分子筛表面的酸性位点,以解析硅铝比对分子筛吸附性能的影响机制。实验结果表明,丙酮的吸附能力主要受自身极性、支链结构和分子筛表面酸位点的影响。而乙酸丁酯、苯乙烯、对二甲苯、苯、甲苯的吸附性能会同时受到自身的分子量、分子直径、极性、分子结构和官能团的影响,分子量和分子直径大、极性强且具有支链结构的VOCs更容易被ZSM-5分子筛吸附。这6种VOCs中,ZSM-5分子筛对丙酮的吸附效果最好,硅铝比对其吸附性能的影响也最大,这是因为丙酮比其他VOCs更容易吸附在路易斯酸位点上,硅铝比的改变会影响酸位点的数量。低硅铝比的分子筛由于具有较多的酸位点,更适用于丙酮的吸附。
中图分类号:
冀钟, 赵彦玲, 陈雨濛, 高林霞, 王翼鹏, 刘欢. ZSM-5分子筛对典型涂装VOCs的吸附性能及机理研究[J]. 化工学报, DOI: 10.11949/0438-1157.20240042.
Zhong JI, Yanling ZHAO, Yumeng CHEN, Linxia GAO, Yipeng WANG, Huan LIU. Adsorption performance and mechanism of ZSM-5 molecular sieves on typical coating VOCs[J]. CIESC Journal, DOI: 10.11949/0438-1157.20240042.
图 5 不同硅铝比分子筛的氮气脱附曲线(a)和孔径分布图(b)
Fig. 5 Nitrogen desorption curves (a) and pore size distribution (b) of molecular sieves with different silicon-aluminum ratios
样品 | 理论Si/Al | 实际Si/Al | 总比表面积(m2/g)① | 微孔表面积(m2/g)② | 外比表面积(m2/g) | 总孔容(m3/g)③ | 平均孔径(nm)④ |
---|---|---|---|---|---|---|---|
1 | 50 | 48.49 | 420.59 | 360.74 | 59.85 | 0.36 | 3.47 |
2 | 100 | 91.84 | 471.92 | 396.42 | 75.50 | 0.54 | 4.54 |
3 | 150 | 129.88 | 468.11 | 407.82 | 60.29 | 0.62 | 5.32 |
4 | 300 | 245.05 | 402.45 | 335.09 | 67.36 | 0.24 | 2.43 |
5 | 500 | 350.98 | 416.94 | 369.04 | 47.90 | 0.26 | 2.46 |
6 | 800 | 547.63 | 438.67 | 391.86 | 46.81 | 0.24 | 2.42 |
7 | 1500 | 730.17 | 465.56 | 373.01 | 92.43 | 0.38 | 3.23 |
8 | 3000 | 933.74 | 437.19 | 372.81 | 64.37 | 0.33 | 3.01 |
表1 合成不同硅铝比分子筛的基本参数
Table 1 Basic parameters for the synthesis of molecular sieves with different Si/Al ratios
样品 | 理论Si/Al | 实际Si/Al | 总比表面积(m2/g)① | 微孔表面积(m2/g)② | 外比表面积(m2/g) | 总孔容(m3/g)③ | 平均孔径(nm)④ |
---|---|---|---|---|---|---|---|
1 | 50 | 48.49 | 420.59 | 360.74 | 59.85 | 0.36 | 3.47 |
2 | 100 | 91.84 | 471.92 | 396.42 | 75.50 | 0.54 | 4.54 |
3 | 150 | 129.88 | 468.11 | 407.82 | 60.29 | 0.62 | 5.32 |
4 | 300 | 245.05 | 402.45 | 335.09 | 67.36 | 0.24 | 2.43 |
5 | 500 | 350.98 | 416.94 | 369.04 | 47.90 | 0.26 | 2.46 |
6 | 800 | 547.63 | 438.67 | 391.86 | 46.81 | 0.24 | 2.42 |
7 | 1500 | 730.17 | 465.56 | 373.01 | 92.43 | 0.38 | 3.23 |
8 | 3000 | 933.74 | 437.19 | 372.81 | 64.37 | 0.33 | 3.01 |
图6 不同分子量VOCs在ZSM-5分子筛上吸附的饱和吸附量(a)和穿透时间(b)
Fig.6 Saturation adsorption (a) and penetration time (b) of different molecular weight VOCs adsorbed on ZSM-5 molecular sieves
图7 不同分子直径VOCs在ZSM-5分子筛上吸附的饱和吸附量(a)和穿透时间(b)
Fig. 7 Saturation adsorption (a) and penetration time (b) of VOCs with different molecular diameters adsorbed on ZSM-5 molecular sieves
图8 不同结构VOCs在ZSM-5分子筛上吸附的饱和吸附量(a)和穿透时间(b)
Fig.8 Saturation adsorption (a) and penetration time (b) of VOCs with different structures adsorbed on ZSM-5 molecular sieves
图 9 不同偶极矩VOCs在ZSM-5分子筛上吸附的饱和吸附量(a)和穿透时间(b)
Fig. 9 Saturation adsorption (a) and penetration time (b) of VOCs with different dipole moments adsorbed on ZSM-5 molecular sieves
图10 不同硅铝比ZSM-5分子筛吸附丙酮和乙酸丁酯的饱和吸附量(a)和穿透时间(b)
Fig. 10 Saturation adsorption (a) and penetration time (b) of acetone and butyl acetate adsorbed on ZSM-5 molecular sieves with different silica-to-aluminum ratios
图12 硅铝比100、500分子筛对丙酮、乙酸丁酯吸附前后NH3-TPD测试图(a~d)和质谱测试图(e~h)注:(Ⅰ、Ⅱ、Ⅲ 分别为分子筛吸附VOCs前后弱、中、强酸变化量)
Fig. 12 NH3-TPD test graphs (a~d) and mass spectrometry test graphs (e~h) before and after adsorption of acetone and butyl acetate on silica-aluminium ratios of 100 and 500 molecular sieves
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