Volatile Organic Compounds Adsorption Capacities of Zeolite/Activated Carbon Composites Formed by Electrostatic Self-Assembly.

ACS applied materials & interfaces(2023)

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摘要
Activated carbon (AC) is a broad-spectrum adsorbent but is flammable and has low adsorption capacities for polar and/or high-boiling volatile organic compounds (VOCs), while zeolites exhibit high thermal stability but poor adsorption of macromolecular and nonpolar VOCs. In this study, zeolite/AC composites were synthesized with the aim of obtaining broad-spectrum, efficient, and safe adsorbents for VOCs. Dimethyldiallylammonium chloride (DDA)-modified AC was used as a carrier for an in situ hydrothermal reaction enabling assembly with zeolites due to electrostatic attraction. Interface models were constructed for their phases, which revealed the binding force and simulated the binding process. The adsorption and flame resistance of the composites were evaluated. The results showed that DDA effectively modified AC to give it a long-lasting positive charge in solutions. High-silicon and pure-silicon zeolites exhibited low negative charges or were even neutral; it was difficult to combine with the modified AC via electrostatic attractions. Instead, LTA zeolites with high aluminum contents and negative charges were used, and the seed-induction method was used. Ethanol and ultrasonic dispersion were used to prevent agglomeration of the seeds and modified AC powder, so they were self-assembled electrostatically. Moreover, the crystallization time was extended and composites with high zeolite loadings were successfully prepared. According to the model calculation, the binding energy between the zeolite and AC before and after the DDA modification were 324.97 and 1076.46 kcal mol, respectively, and the distance between them was shortened by 2.7 Å after DDA treatment. As a result, AC and zeolite combined more closely and exhibited a stronger binding energy. The adsorption capacity for highly polar dichloromethane was improved by zeolite loading on the AC, and the bed penetration time was doubled. However, impregnation with inorganic sodium enhanced the reactivities of the organic components in the composite, and the ignition point was slightly reduced. Furthermore, the electrostatic self-assembly method can expand to prepare the LTA zeolite/columnar AC composite from shaped AC, greatly improving its application prospects.
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关键词
zeolite, activated carbon, composites, interface model, volatile organic compounds, adsorption
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