凹凸棒黏土负载纳米TiO2-Fe3O4吸附剂的制备及Cr(Ⅵ)的脱除

doi:10.11944/j.issn.1000-0518.2019.03.180112

摘要/Abstract

摘要：

采用溶胶-凝胶法、一锅反应法制备了负载纳米TiO₂和Fe₃O₄的凹凸棒黏土(TiO₂-Fe₃O₄-ATP)吸附剂,并进行了模拟废水中Cr(Ⅵ)的吸附及脱附性能的研究。通过扫描电子显微镜(SEM)、X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)和EDS等分析方法对ATP负载纳米TiO₂-Fe₃O₄前后结构进行了表征,考察了物料配比及吸附时间、pH值、温度、投加量和初始质量浓度对Cr(Ⅵ)吸附率的影响。结果表明,吸附剂在Ti元素含量与负载总量的摩尔比为3：4时吸附效果最佳。当吸附剂质量为0.6 g,Cr(Ⅵ)离子初始质量浓度小于0.8 mg/L时,pH=6,温度20 ℃,吸附剂对Cr(Ⅵ)的吸附率为79.8%。 TiO₂-Fe₃O₄-ATP吸附剂对Cr(Ⅵ)离子吸附满足Freundlich模型。在20~40 ℃ 条件下,吸附过程ΔG<0、ΔS=-43.55 J/(mol·K)、ΔH=-14.36 kJ/mol,表明该吸附是个自发、熵减、放热的过程。吸附过程符合准二级动力学模型,吸附速率控制步骤以表面化学反应为主。 TiO₂-Fe₃O₄-ATP吸附剂在循环使用4次后,吸附率仍能达到65%以上。

关键词: 凹凸棒黏土, TiO₂, Fe₃O₄, 吸附剂

Abstract:

Attapulgite clay(ATP) supported nano TiO₂-Fe₃O₄(TiO₂-Fe₃O₄-ATP) adsorbents were prepared by sol-gel method in one-pot, and its adsorption and desorption properties of Cr(Ⅵ) in simulated wastewater were studied. The structure and contents of the adsorbent were characterized by scanning electron microscopy(SEM), X-ray diffraction(XRD), Fourier transform infrared spectrometer(FT-IR) and EDS before and after nano TiO₂-Fe₃O₄ loading, The effects of the ratio of reactants, adsorption time, pH value, temperature, dosage and initial concentration on the adsorption rate of Cr(Ⅵ) were studied. The best performance of the adsorbents was observed when the molar fraction of Ti in the total loading is 75%. The attapulgite adsorbent loaded with nano TiO₂ and Fe₃O₄ has better adsorption effect on the removal of Cr(Ⅵ) when the mass of adsorbent is 0.6 g. When the initial concentration of Cr(Ⅵ) is less than 0.8 mg/L and the pH value is 6 at 20 ℃, the adsorption rate of Cr(Ⅵ) reached 79.8%. The adsorption of Cr(Ⅵ) by TiO₂-Fe₃O₄-ATP can be described by Freundlich equation. At 20~40 ℃, the free energy(ΔG), enthalpy(ΔH) and entropy(ΔS) changes of the adsorption process were calculated. The results show that ΔG<0, ΔS=-43.55 J/(mol·K), ΔH=-14.36 kJ/mol, indicating that the adsorption is spontaneous, exothermic and entropy reduction. Pseudo-first-order kinetic model, pseudo-second-order kinetic model and shell progressive model were studied for the kinetic data. The result shows that the adsorption process fits the quasi-second-order kinetic model. The rate control step of adsorption is mainly surface chemical reaction. The adsorption rate of TiO₂-Fe₃O₄-ATP adsorbent can reach more than 65% after 4 times of recycling.

Key words: attapulgite clay, TiO₂, Fe₃O₄, adsorbent

李静萍, 杨仕海, 刘洋, 柏文博. 凹凸棒黏土负载纳米TiO₂-Fe₃O₄吸附剂的制备及Cr(Ⅵ)的脱除[J]. 应用化学, 2019, 36(3): 324-334.

LI Jingping, YANG Shihai, LIU Yang, BO Wenbo. Preparation of Attapulgite Clay Supported Nano TiO₂-Fe₃O₄ Adsorbent and Removal of Cr(Ⅵ)[J]. Chinese Journal of Applied Chemistry, 2019, 36(3): 324-334.

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凹凸棒黏土负载纳米TiO₂-Fe₃O₄吸附剂的制备及Cr(Ⅵ)的脱除

Preparation of Attapulgite Clay Supported Nano TiO₂-Fe₃O₄ Adsorbent and Removal of Cr(Ⅵ)

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