催化学报 ›› 2018, Vol. 39 ›› Issue (1): 8-15.DOI: 10.1016/S1872-2067(17)62933-4

• 论文 • 上一篇    下一篇

金负载氧化石墨烯/PDPB复合材料用于同步去除六价铬离子和苯酚

刘俊, 方文章, 王宇航, 邢明阳, 张金龙   

  1. 华东理工大学精细化工研究所, 上海 200237
  • 收稿日期:2017-08-21 修回日期:2017-10-08 出版日期:2018-01-18 发布日期:2018-01-19
  • 通讯作者: 邢明阳, 张金龙
  • 基金资助:

    国家自然科学基金(21577036,21377038,21237003,21677048);国家重点基础研究发展规划(973计划,2013CB632403);中国国家重点研究发展计划(2016YFA0204200);中央高校基本科研业务费专项基金(22A201514021).

Gold-loaded graphene oxide/PDPB composites for the synchronous removal of Cr(VI) and phenol

Jun Liu, Wenzhang Fang, Yuhang Wang, Mingyang Xing, Jinlong Zhang   

  1. Key Laboratory for Advanced Materials and Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China
  • Received:2017-08-21 Revised:2017-10-08 Online:2018-01-18 Published:2018-01-19
  • Contact: 10.1016/S1872-2067(17)62933-4
  • Supported by:

    This work was supported by the National Natural Science Foundation of China (21577036, 21377038, 21237003, 21677048), the National Basic Research Program of China (973 Program, 2013CB632403), State Key Research Development Program of China (2016YFA0204200), the Fundamental Research Funds for the Central Universities (22A201514021).

摘要:

近年来,电镀和染料行业工业废水中排放的有机污染物和重金属离子严重危害着环境.构建无机-有机新型纳米材料用于光催化去除重金属离子和有机污染物受到了广泛的关注.共轭聚合物因其低廉的制造成本,快速的电子传送能力,优秀的电化学性能和高的机械性能,它们作为一类新能源材料已经快速发展起来.Remita等使用软模板方法制备的一种共轭聚合物聚1,4-二苯基丁二炔(PDPB)在可见光下对苯酚表现出较好的去除率.然而,聚合物PDPB的一些缺陷限制了其应用,比如高的疏水特性和快速的光生电子-空穴复合.因此,我们引入氧化石墨烯(GO)和金纳米粒子来提高PDPB的光催化活性.通过简单的机械搅拌和光还原方法制备了Au-GO/PDPB复合材料.通过TEM,XRD,XPS,固体紫外和光电流测试等技术对催化剂进行了一系列表征,结果发现氧化石墨烯作为优秀的电子传送基地,金纳米粒子作为电子捕获剂,在空间上实现了电子空穴的空间隔离,从而大大提高了Au-GO/PDPB复合材料对于六价铬离子和苯酚的同步光去除的光催化活性.
XPS表征和TEM图像表明了GO和Au纳米粒子的存在.其PDPB有着纳米纤维的结构,宽度在20nm左右,长度在几个微米.当复合了氧化石墨烯后,可以明显看出氧化石墨烯的形态,进一步光还原负载金纳米粒子,同样可以在TEM图中观察到金纳米粒子的存在,其直径在10nm左右.之后通过光催化同步去除六价铬离子和苯酚来探究Au-GO/PDPB复合材料的活性,结果表明所制备的Au-GO/PDPB比纯的PDPB有着增强的光催化活性在同步光去除六价铬离子(Cr (VI))和苯酚中.更进一步地是,我们同样确定了GO和Au纳米离子的最佳负载量,结果发现,Au1-GO2/PDPB复合材料(金的负载量为1wt%,氧化石墨烯的负载量为2wt%)在所有催化剂中有着最好的光催化活性,其在4 h内对苯酚的去除率达到49.4%,相应的对于六价铬离子的还原率达到了77.4%.我们的研究提供了一种构建有机-无机杂化复合材料的方法,其在太阳光下对于有机污染物和重金属离子的同步去除有着高的光催化活性.

关键词: 光催化, 重金属离子, 有机污染物, 聚合物1,4-二苯基丁二炔(PDPB), 同步去除

Abstract:

The construction of novel inorganic-organic hybrid nanomaterials for synchronous photocatalytic removal of heavy metal ions and organic pollutants has received significant attention. We successfully synthesized gold-loaded graphene oxide/PDPB (polymer poly(diphenylbutadiyne)) composites (Au-GO/PDPB) through a facile mechanical agitation and photoreduction method. The composites were characterized by XPS and TEM images, which confirmed the presence of GO and Au nanoparticles on the PDPB. The as-prepared Au-GO/PDPB composites displayed enhanced photocatalytic activity compared with that of pure PDPB for the synchronous photoreduction of hexavalent chromium (Cr(VI)) and photo-oxidation of phenol. We also determined the optimal loading mass of GO and Au nanoparticles on the PDPB; the Au1-GO2/PDPB (2.0 wt% GO and 1.0 wt% Au) composite displayed the best photocatalytic activity among all the catalysts. Our study provides a facile way to prepare inorganic-organic composites for the synchronous photocatalytic removal of heavy metal ions and organic pollutants.

Key words: Photocatalysis, Heavy metal ion, Organic pollutant, Polymer poly(diphenylbutadiyne), Synchronous removal