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通过 Box-Behnken 优化制备 CS/β-CD/Nano-ZnO 复合多孔膜及其对刚果红的吸附性能研究

Preparation and characterization of CS/β-CD/Nano-ZnO composite porous membrane optimized by Box-Behnken for the adsorption of Congo red.

机构信息

School of Environment and Energy, Guangzhou Higher Education Mega Centre, South China University of Technology, Guangzhou, 510006, People's Republic of China.

The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters of Ministry of Education, Guangzhou, 510006, People's Republic of China.

出版信息

Environ Sci Pollut Res Int. 2018 Aug;25(22):22244-22258. doi: 10.1007/s11356-018-2110-3. Epub 2018 May 26.

Abstract

In this paper, an effective chitosan/beta-cyclodextrin/nanometer zinc oxide (CS/β-CD/Nano-ZnO) composite porous membrane was synthesized by sol-gel and polymer-assisted inverting method. Preparation conditions of CS/β-CD/Nano-ZnO were investigated by single-factor and Box-Behnken response surface methodology optimizing triethoxyvinylsilane (JH-V151), beta-cyclodextrin (β-CD), and nanometer zinc oxide (Nano-ZnO), and applied to study the adsorption characteristics of Cong red (CR) from aqueous solution using batch experiments. The optimum preparation conditions were determined that the volume fraction of JH-V151 alcohol solution was 11%, the ratio of β-CD to CS was 5.35, and the ratio of Nano-ZnO's mass to solution's volume was 0.36%. Different characterization methods including field-emission scanning electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, UV-visible spectroscopy, and Universal Materials Tester were used to prove the appearance, crystallinity, functional groups, swelling degree, transmittance, and tensile property of CS/β-CD/Nano-ZnO. The optimized batch experimental parameters were 50 mg L, 4 h, 7.0, 0.5 g L, and 55.0 °C as initial concentration, contact time, pH, adsorbent dose, and temperature, respectively. The maximum adsorption capacity on CR reached 96.33 mg g, which is 4.34 times with respect to CS. The batch experimental data were best described by a pseudo-second-order kinetics model and Langmuir isotherm model (R = 0.9965, theoretical saturated adsorption capacity 147.28 mg g). The values ∆G were - 2.09, - 4.73, and - 7.37 kJ mol at 298, 308, and 318 K temperatures, respectively. The ∆H value was 76.68 kJ mol, indicating the endothermic and spontaneous adsorption in nature. The ∆S value was 0.26 kJ mol K, a signal of entropy increase during adsorption. The adsorption capacity decreased only by 5.8% after six recycling runs, which indicated the reusability of CS/β-CD/Nano-ZnO. Therefore, the CS/β-CD/Nano-ZnO composite porous membrane is a promising membrane material for the efficient removal of CR from any water at large and economic scales at moderate concentration.

摘要

本文采用溶胶-凝胶和聚合物辅助反转法合成了一种有效的壳聚糖/β-环糊精/纳米氧化锌(CS/β-CD/Nano-ZnO)复合多孔膜。通过单因素和 Box-Behnken 响应面法优化了三乙氧基乙烯基硅烷(JH-V151)、β-环糊精(β-CD)和纳米氧化锌(Nano-ZnO)的制备条件,并应用于批实验研究从水溶液中吸附刚果红(CR)的吸附特性。确定的最佳制备条件为:JH-V151 醇溶液体积分数为 11%,β-CD 与 CS 的比例为 5.35,纳米 ZnO 质量与溶液体积的比例为 0.36%。采用场发射扫描电子显微镜、X 射线衍射、傅里叶变换红外光谱、紫外可见光谱和通用材料试验机等不同表征方法证明了 CS/β-CD/Nano-ZnO 的外观、结晶度、官能团、溶胀度、透光率和拉伸性能。优化后的批实验参数为初始浓度 50mg/L、接触时间 4h、pH 值 7.0、吸附剂用量 0.5g/L 和温度 55.0°C。对 CR 的最大吸附容量达到 96.33mg/g,是 CS 的 4.34 倍。批实验数据最符合准二级动力学模型和 Langmuir 等温线模型(R=0.9965,理论饱和吸附容量 147.28mg/g)。在 298、308 和 318K 温度下,∆G 值分别为-2.09、-4.73 和-7.37kJ/mol。∆H 值为 76.68kJ/mol,表明吸附为吸热和自发过程。∆S 值为 0.26kJ/mol/K,表明吸附过程中熵增加。经过六次循环回收后,吸附容量仅下降了 5.8%,表明 CS/β-CD/Nano-ZnO 具有良好的可重复使用性。因此,CS/β-CD/Nano-ZnO 复合多孔膜是一种很有前途的膜材料,可用于在较大规模和经济规模下,从任何水中去除 CR,尤其是在中浓度下。

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