摘要
制备了不同阳离子掺杂改性的针铁矿,并采用XRD、红外、热重差热分析以及TEM等手段对其进行了表征,结果显示,掺入Mn^(2+)、Cr^(3+)、Al^(3+)后并未明显改变α-FeOOH的晶体结构类型,说明部分阳离子掺杂进入α-FeOOH晶格,从而分别形成因Fe^(3+)被Mn^(2+)、Cr^(3+)、Al^(3+)部分取代的固溶体;红外分析也得到类似结果;热重和差热分析以及TEM观察结果均表明几种金属阳离子没有形成氧化物相,可以确定这些离子已经进入针铁矿的晶格;紫外-可见漫反射光谱分析发现Mn^(2+)、Cr^(3+)掺杂者的能带隙较之纯相针铁矿的稍小,依次为2.18 e V和2.24 e V;而Al^(3+)掺杂者的能带隙与纯相针铁矿相比有所提高,增加至2.34 e V。此外还考查了不同阳离子掺杂及纯相针铁矿与Fe(Ⅱ)构成的复合系统对邻硝基苯酚(2-NP)的还原效果,研究表明,在溶液pH=6和25℃等的条件下,上述还原转化反应符合准一级动力学方程。其中,Fe(Ⅱ)/Al^(3+)掺杂针铁矿复合系统对2-NP的降解效果最好,在120 min时就达到了100%去除率,在一定浓度范围内,随着2-NP浓度的升高,2-NP的还原速率降低。而且,Fe(Ⅱ)/Al^(3+)-针铁矿复合系统速率常数(k)随着溶液的pH值增大而升高。
In this paper, modified goethite samples doped with different cations were prepared and characterized. XRD showed that doping cations Mn^2+, Cr^3+ and Al^3+ didn't significantly change the types of crystal structure for α-FeOOH, indicating that the cations were doped into the α-FeOOH lattice, and solid solutions were respectively formed when Fe3+ was partially replaced by Mn^2+, Cr^3+ and Al^3+. The infrared analysis also showed a similar result. The results of TGA-DTA and TEM exhibited that these metal cations had entered the goethite lattice. By UV-vis diffuse reflection spectrum analysis, it was found that the band gaps of goethite doped with Mn^2+ and Cr^3+ were 2.18 and 2.24 eV, respectively, lower than the band gap of pure goethite (2.28 eV); in contrast, the band gap of goethite doped with Al^3+ was increased to 2.34 eV. In addition, the reductive effects of different complex systems of Fe(Ⅱ) combined with pure goethite and its counterparts doped with above three different cations on 2-NP reduction were investigated, and it was found that the 2-nitrophenol (2-NP) reductive transformation followed the pseudo-first-order kinetics under the condition pH=6 and temperature 25℃. The system Fe(Ⅱ)/goethite doped with Al^3+ showed the best degradation of 2-NP with a removal efficiency of 100% within 120 min. However, the reductive rate of 2-NP transformation was clearly reduced with the initial concentrations of 2-NP increasing to a certain extent. Moreover, the rate constant (k) of the system doped with Al^3+ was increased with the increment of the solution pH value.
作者
杜可清
吴宏海
朱慧琳
魏西鹏
管玉峰
蓝冰燕
DU Ke-qing WU Hong-hai ZHU Hui-lin WEI Xi-peng GUAN Yu-feng LAN Bing-yan(School of Chemistry and Environment, South China Normal University, Guangzhou 510006, China)
出处
《岩石矿物学杂志》
CAS
CSCD
北大核心
2016年第6期1075-1084,共10页
Acta Petrologica et Mineralogica
基金
国家自然科学基金项目(41372050)~~
作者简介
杜可清(1992-),女,硕士研究生,环境工程与科学专业,E-mail:dkq9201@163.com
通讯作者:吴宏海,男,教授,博士生导师:E-mail:wuhonghai@scnu.edu.cn。