Comparative study of the adsorption performance of NH2-functionalized metal organic frameworks with activated carbon composites for the treatment of phenolic wastewaters

doi:10.1016/j.cjche.2023.05.004

Abstract

Abstract: To better understand the role of the —NH₂ group in adsorption process of phenolic wastewaters, NH₂-functionalized MIL-53(Al) composites with activated carbon (NH₂-M(Al)@(B)AC) were prepared. The results showed that the NH₂ group could increase the mesopore volume for composites, which promotes mass transfer and full utilization of active sites, because hierarchical mesopore structure makes the adsorbent easier to enter the internal adsorption sites. Furthermore, the introduction of the NH₂ group can improve the adsorption capacity, decrease the activation energy, and enhance the interaction between the adsorbent and p-nitrophenol, demonstrating that the NH₂ group plays a crucial role in the adsorption of p-nitrophenol. The density functional theory calculation results show that the H-bond interaction between the —NH₂ group in the adsorbent and the NO₂ in the p-nitrophenol (adsorption energy of -35.5 kJ·mol^-1), and base-acid interaction between the primary —NH₂ group in the adsorbent and the acidic OH group in the p-nitrophenol (adsorption energy of -27.3 kJ·mol^-1) are predominant mechanisms for adsorption in terms of the NH₂-functionalized adsorbent. Both NH₂-functionalized M(Al)@AC and M(Al)@BAC composites exhibited higher p-nitrophenol adsorption capacity than corresponding nonfunctionalized composites. Among the composites, the NH₂-M(Al)@BAC had the highest p-nitrophenol adsorption capacity of 474 mg·g^-1.

Key words: NH₂-functionalized adsorbent, Phenolic wastewaters, Adsorption, Mechanism, Density functional theory

摘要： To better understand the role of the —NH₂ group in adsorption process of phenolic wastewaters, NH₂-functionalized MIL-53(Al) composites with activated carbon (NH₂-M(Al)@(B)AC) were prepared. The results showed that the NH₂ group could increase the mesopore volume for composites, which promotes mass transfer and full utilization of active sites, because hierarchical mesopore structure makes the adsorbent easier to enter the internal adsorption sites. Furthermore, the introduction of the NH₂ group can improve the adsorption capacity, decrease the activation energy, and enhance the interaction between the adsorbent and p-nitrophenol, demonstrating that the NH₂ group plays a crucial role in the adsorption of p-nitrophenol. The density functional theory calculation results show that the H-bond interaction between the —NH₂ group in the adsorbent and the NO₂ in the p-nitrophenol (adsorption energy of -35.5 kJ·mol^-1), and base-acid interaction between the primary —NH₂ group in the adsorbent and the acidic OH group in the p-nitrophenol (adsorption energy of -27.3 kJ·mol^-1) are predominant mechanisms for adsorption in terms of the NH₂-functionalized adsorbent. Both NH₂-functionalized M(Al)@AC and M(Al)@BAC composites exhibited higher p-nitrophenol adsorption capacity than corresponding nonfunctionalized composites. Among the composites, the NH₂-M(Al)@BAC had the highest p-nitrophenol adsorption capacity of 474 mg·g^-1.

关键词: NH₂-functionalized adsorbent, Phenolic wastewaters, Adsorption, Mechanism, Density functional theory

Bolong Jiang, Shunjie Shi, Yanyan Cui, Jiayou Li, Nan Jiang, Yanguang Chen. Comparative study of the adsorption performance of NH₂-functionalized metal organic frameworks with activated carbon composites for the treatment of phenolic wastewaters[J]. Chinese Journal of Chemical Engineering, 2023, 63(11): 130-139.

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Comparative study of the adsorption performance of NH₂-functionalized metal organic frameworks with activated carbon composites for the treatment of phenolic wastewaters

Comparative study of the adsorption performance of NH₂-functionalized metal organic frameworks with activated carbon composites for the treatment of phenolic wastewaters

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