SCI和EI收录∣中国化工学会会刊

中国化学工程学报 ›› 2023, Vol. 63 ›› Issue (11): 130-139.DOI: 10.1016/j.cjche.2023.05.004

• Full Length Article • 上一篇    下一篇

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

Bolong Jiang1,2, Shunjie Shi3, Yanyan Cui3, Jiayou Li3, Nan Jiang1, Yanguang Chen2   

  1. 1. Innovation Institute for Sustainable Maritime Architecture Research and Technology, Qingdao University of Technology, Qingdao 266000, China;
    2. College of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing 163318, China;
    3. Institute of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266000, China
  • 收稿日期:2023-01-18 修回日期:2023-05-05 出版日期:2023-11-28 发布日期:2024-01-08
  • 通讯作者: Bolong Jiang,E-mail:jiangbolong@qut.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (22008134).

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

Bolong Jiang1,2, Shunjie Shi3, Yanyan Cui3, Jiayou Li3, Nan Jiang1, Yanguang Chen2   

  1. 1. Innovation Institute for Sustainable Maritime Architecture Research and Technology, Qingdao University of Technology, Qingdao 266000, China;
    2. College of Chemistry and Chemical Engineering, Northeast Petroleum University, Daqing 163318, China;
    3. Institute of Environmental and Municipal Engineering, Qingdao University of Technology, Qingdao 266000, China
  • Received:2023-01-18 Revised:2023-05-05 Online:2023-11-28 Published:2024-01-08
  • Contact: Bolong Jiang,E-mail:jiangbolong@qut.edu.cn
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (22008134).

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

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