物理化学学报 >> 2010, Vol. 26 >> Issue (09): 2437-2442.doi: 10.3866/PKU.WHXB20100910

催化和表面结构 上一篇    下一篇

仿生光催化剂的优化制备、介孔特性表征及其在催化降解苯酚废水中的应用

高冠道, 李婧, 张爱勇, 安晓红, 周蕾   

  1. 南开大学环境科学与工程学院,环境污染过程与基准教育部重点实验室,天津300071
  • 收稿日期:2010-02-01 修回日期:2010-05-12 发布日期:2010-09-02
  • 通讯作者: 高冠道 E-mail:gaoguandao@163.com
  • 基金资助:

    国家自然科学基金项目(20803036),科技人员服务企业行动(2009GJA10014)和水体污染控制与治理科技重大专项(2008ZX07314-003-2)基金资助

Optimizational Preparation and Mesoporous Material Characteristics of a Novel Biomimetic Photocatalyst and Its Application to the Photocatalytic Degradation of Phenol

GAO Guan-Dao, LI Jing, ZHANG Ai-Yong, AN Xiao-Hong, ZHOU Lei   

  1. Key Laboratory of Pollution Processes and Environmental Criteria, Ministry of Education, College of Environmental Science and Engineering, Nankai University, Tianjin 300071, P. R. China
  • Received:2010-02-01 Revised:2010-05-12 Published:2010-09-02
  • Contact: GAO Guan-Dao E-mail:gaoguandao@163.com
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20803036), Plan on Scientific and Technological Personnel Serving Enterprise (2009GJA10014), Major Scientific and Technological Projects of Water Pollution Control and Treatment (2008ZX07314-003-2).

摘要:

以十二胺(DDA)或十八胺(ODA)为模板剂, 采用焙烧或萃洗法去除模板剂制备中孔分子筛(HMS). X射 线粉末衍射(XRD)及氮吸附表征结果说明, 以十二胺为模板剂且采用焙烧法去除模板剂制备的分子筛具有明显 的XRD 介孔衍射峰, 而且其氮吸附曲线具有典型的IV 类等温线特征及H1 型脱附滞后环, 这属于典型的介孔 材料特征. 以此分子筛为载体, 通过F—C 反应将磺酸铁酞菁(FePcS)修饰在HMS上, 得到新型光催化剂. 催化剂 的BET 比表面积为675.1 m2·g-1, 平均孔径为5.78 nm, 孔容为0.587 cm3·g-1, 且仍保持着鲜明的介孔特征. 最后 在模拟可见光照射下应用催化剂处理浓度高达1000 mg·L-1的模拟苯酚废水, 反应400 min 后, 苯酚的转化率达 到85%以上, 反应溶液pH 值也由4.52 降到2.65, 表明有酸类降解中间产物生成, 反应最终苯酚转化率接近 100%, 总有机碳(TOC)的去除率达81%以上. 催化剂表现出了良好的催化降解有机废水的性能.

关键词: 中孔分子筛, 磺酸铁酞菁, 孔特性, 优化制备, 光催化

Abstract:

Hexagonal mesoporous silica (HMS) was synthesized using dodecylamine (DDA) or octadecylamine (ODA) as templates which were then removed by calcination or extraction. Characterization data of HMS from XRD and N2 adsorption-desorption proved that the optimized material were typical mesoporous materials based on the facts that the XRDdiffraction peak displayed apparently the feature of mesoporous materials and the N2 adsorption-desorption curve was typical of a type IV isothermand contained a type H1 desorption hysteresis loop. These novel photocatalysts had a BET surface area of 675.1 m2·g-1, an average pore diameter of 5.78 nm and a BJH pore volume of 0.587 cm3·g-1, and were prepared by the F—C reaction between functionalized HMS and iron sulfophthalocyanine (FePcS). Additionally, the catalysts preserved an undamaged heavy mesoporous structure. Upon the irradiation of the simulated visible light, these novel catalysts were applied to the degradation of simulated phenol wastewater at a concentration of 1000 mg·L-1. The conversion of phenol reached 85%and the pH decreased from the original 4.52 to 2.65 after reaction time of 400 min, which indicated that acid intermediates were produced during the photocatalysis of phenol. Finally, the conversion rate of phenol was nearly 100% and the total organic carbon (TOC) removal rate exceeded 81%. The novel catalyst is, therefore, highly effective for the degradation of phenol.

Key words: Hexagonal mesoporous silica, Iron sulfophthalocyanine, Pore characteristics, Optimizing preparation, Photocatalysis

MSC2000: 

  • O643