Fujian Provincial Engineering Research Center of Rural Waste Recycling Technology, College of Environment & Resources, Fuzhou University, Fuzhou, 350116, China.
School of Civil and Environmental Engineering, University of Washington, Seattle, 98195, USA.
Environ Res. 2021 Mar;194:110652. doi: 10.1016/j.envres.2020.110652. Epub 2021 Jan 5.
In this work, a novel cellulose aerogel (CNC-PVAm/rGO) was fabricated using cellulose nanocrystalline (CNC) modified with polyvinylamine (PVAm) and reduced graphene oxide (rGO). The resultant CNC-PVAm/rGO was then applied for the adsorption of diclofenac sodium (DCF), a typical non-steroidal anti-inflammatory drug. Characterization using ultra-high-resolution field emission scanning electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and the Brunauer-Emmett-Teller surface area revealed that the obtained CNC-PVAm/rGO displayed an evident 3D porous structure, which had an ultralight weight, good recovery, abundant surface functional groups (e.g., -NH and -OH), and rGO nanosheets. In addition, the material presented a stable crystal structure and large specific surface area (105.73 m g). During the adsorption of DCF, the CNC-PVAm/rGO aerogel showed a rather excellent adsorption performance, with a maximum adsorption capacity (q) of 605.87 mg g, which was approximately 53 times larger than that of the bare CNC aerogel (11.45 mg g). The adsorption performance of CNC-PVAm/rGO was also better than that of other reported adsorbents. The adsorption of DCF to CNC-PVAm/rGO obeyed the Langmuir isotherm and pseudo-second-order kinetic models, and underwent a spontaneous exothermic process. Moreover, DCF was easily desorbed from CNC-PVAm/rGO with sodium hydroxide solution (0.1 mol L), and the absorbent could be reused four times. The introduction of PVAm and rGO to the CNC-PVAm/rGO aerogel also greatly enhanced electrostatic interactions, π-π interactions, and hydrophobic effects. These enhancements significantly promoted the hydrogen bonding interactions between the DCF molecules and CNC-PVAm/rGO, thus resulting in a large improvement in the adsorption performance of the aerogel.
在这项工作中,使用纤维素纳米晶(CNC)与聚乙烯亚胺(PVAm)和还原氧化石墨烯(rGO)改性,制备了一种新型纤维素气凝胶(CNC-PVAm/rGO)。然后,将所得的 CNC-PVAm/rGO 用于吸附典型的非甾体抗炎药双氯芬酸钠(DCF)。使用超高分辨率场发射扫描电子显微镜、傅里叶变换红外光谱、X 射线衍射、X 射线光电子能谱和 Brunauer-Emmett-Teller 比表面积对其进行了表征,结果表明,所得的 CNC-PVAm/rGO 显示出明显的 3D 多孔结构,具有超轻的重量、良好的可回收性、丰富的表面官能团(如-NH 和-OH)和 rGO 纳米片。此外,该材料具有稳定的晶体结构和大的比表面积(105.73 m²/g)。在吸附 DCF 时,CNC-PVAm/rGO 气凝胶表现出相当优异的吸附性能,最大吸附容量(q)为 605.87 mg/g,约为裸 CNC 气凝胶(11.45 mg/g)的 53 倍。CNC-PVAm/rGO 的吸附性能也优于其他报道的吸附剂。DCF 对 CNC-PVAm/rGO 的吸附符合 Langmuir 等温线和准二级动力学模型,并且是一个自发的放热过程。此外,DCF 可以很容易地从 CNC-PVAm/rGO 用氢氧化钠溶液(0.1 mol/L)解吸,并且该吸附剂可以重复使用四次。将 PVAm 和 rGO 引入到 CNC-PVAm/rGO 气凝胶中也极大地增强了静电相互作用、π-π 相互作用和疏水作用。这些增强显著促进了 DCF 分子与 CNC-PVAm/rGO 之间的氢键相互作用,从而导致气凝胶吸附性能的显著提高。