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α-Fe2O3/SiO2纳米颗粒混合体系表面的酸碱性质及其对重金属离子的吸附行为
引用本文:孙和云,樊佳妮,黄佩佩,孙中溪*. α-Fe2O3/SiO2纳米颗粒混合体系表面的酸碱性质及其对重金属离子的吸附行为[J]. 物理化学学报, 2012, 28(9): 2183-2190. DOI: 10.3866/PKU.WHXB201206072
作者姓名:孙和云  樊佳妮  黄佩佩  孙中溪*
作者单位:School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P. R. China
基金项目:国家自然科学基金(50874052, 20677022)和国家重大科学研究计划(2011CB933700)资助项目
摘    要:以Fe(NO3)3·9H2O和正硅酸乙酯(TEOS)为原料, 通过溶胶-凝胶法和辅助模板法分别制备了纳米α-Fe2O3和SiO2, 并对所合成样品进行了粉末X射线衍射(XRD)和BET表征. 使用自动电位滴定仪测定了α-Fe2O3/SiO2纳米颗粒混合体系的表面酸碱性质. 研究了在不同pH下α-Fe2O3/SiO2混合体系对Cu2+、Pb2+、Zn2+离子的吸附行为. 基于上述实验数据, 用WinSGW软件计算了α-Fe2O3/SiO2混合体系表面酸碱配位常数, 并得出结论: α-Fe2O3/SiO2混合体系表面反应为单一脱质子反应≡XOH ⇔ ≡XO-+ H+(lg K = -8.19±0.15), 明显区别于同时具有加质子和脱质子反应的α-Fe2O3/SiO2/γ-Al2O3, α-Fe2O3/γ-Al2O3和SiO2/γ-Al2O3等纳米颗粒混合体系. 在此基础上拟合得到α-Fe2O3/SiO2混合体系吸附重金属离子Cu2+、Pb2+、Zn2+的表面络合反应平衡常数分别为:
≡XOH + M2+ ⇔ ≡XOM++ H+ [lg K = -3.1, -3.6, -3.8 (M = Cu, Pb, Zn)].
≡XOH+M2++H2O ⇔≡XOMOH+2H+[lg K = -8.8, -8.0, -10.5 (M = Cu, Pb, Zn)]

关 键 词:α-Fe2O3/SiO2  表面酸碱性质  吸附  重金属离子  组分分布  
收稿时间:2012-04-26
修稿时间:2012-06-07

Acid-Base Properties and Adsorption Behaviors of Heavy Metal Ions at the Surface of α-Fe2O3/SiO2Nano-Mixed System
SUN He-Yun,FAN Jia-Ni,HUANG Pei-Pei,SUN Zhong-Xi. Acid-Base Properties and Adsorption Behaviors of Heavy Metal Ions at the Surface of α-Fe2O3/SiO2Nano-Mixed System[J]. Acta Physico-Chimica Sinica, 2012, 28(9): 2183-2190. DOI: 10.3866/PKU.WHXB201206072
Authors:SUN He-Yun  FAN Jia-Ni  HUANG Pei-Pei  SUN Zhong-Xi
Affiliation:School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, P. R. China
Abstract:α-Fe2O3and SiO2were prepared from ferric nitrate and TEOS by sol-gel method in combination with using templates. The synthetic samples were characterized by powder X-ray diffraction (XRD) and N2adsorption/desorption methods. We determined the surface acid-base properties of α-Fe2O3/SiO2nano-mixed system by potentiometric titration technique, and studied the adsorption behaviors of heavy metal ions on the solid surface of α-Fe2O3/SiO2nano-mixed system at different pH values. According to the above experimental data, we calculated the surface acid-base reaction equilibrium constants of the nano-mixed system using WinSGW software to be ≡XOH ⇔ ≡XO-+ H+(lg K = -8.19±0.15). The calculated result reveals that the single deprotonation surface of α-Fe2O3/SiO2nano-mixed system is obviously different from the surfaces of α-Fe2O3/SiO2/γ-Al2O3, α-Fe2O3/γ-Al2O3 and SiO2/γ-Al2O3nano-mixed system with surface protonation as well as deprotonation at the same time. Based on the above result, the surface complexation constants of Cu2+, Pb2+, Zn2+on the surface of α-Fe2O3/SiO2mixed systems were simulated respectively as follows:
≡XOH + M2+ ⇔ ≡XOM++ H+ [lg K =-3.1, -3.6, -3.8 (M = Cu, Pb, Zn)].
Keywords:α-Fe2O3/SiO2',')  "  >α-Fe2O3/SiO2  Surface acid-base property  Adsorption  Heavy metal ions  Speciation
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