Srinivasan Madhavi, White Tim
School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798.
Environ Sci Technol. 2007 Jun 15;41(12):4405-9. doi: 10.1021/es070160b.
Accelerated photodegradation of methylene blue (MB) over three-dimensionally ordered macroporous (3DOM) titania (pore sizes: 0.5 and 1 microm) is demonstrated. The catalysts were synthesized by colloidal crystal templating against polystyrene spheres using a metal alkoxide precursor. The 3DOM titania walls which are predominantly anatase (> 98%) were decorated homogeneously with gold nanoparticles (5-7 nm) by pH-controlled precipitation of Au from HAuCl4 using sodium hydroxide. A combination of powder X-ray diffraction (XRD), analytical transmission electron microscopy (ATEM) and X-ray photoelectron spectroscopy (XPS) confirmed the deposition of Au(0) on the 3DOM titania macroporous walls. Photocatalytic activity was monitored by following the degradation of MB with activity benchmarked against commercial P25 (Degussa) and powdertitania prepared by hydrolysis of titanium ethoxide. Macroporous 3DOM titania with pore diameter 0.5 microm had the highest first-order rate constant of 0.042 min(-1) for decomposition of MB, compared to 0.025 min(-1) for P25 titania. Deposition of gold on the 3DOM titania surfaces decreased the reaction rate by covering the surface active sites.
本文展示了亚甲基蓝(MB)在三维有序大孔(3DOM)二氧化钛(孔径:0.5和1微米)上的加速光降解。催化剂通过使用金属醇盐前驱体,以聚苯乙烯球为模板通过胶体晶体模板法合成。通过用氢氧化钠从HAuCl4中进行pH控制的Au沉淀,在主要为锐钛矿(>98%)的3DOM二氧化钛壁上均匀地装饰了金纳米颗粒(5-7纳米)。粉末X射线衍射(XRD)、分析透射电子显微镜(ATEM)和X射线光电子能谱(XPS)的组合证实了Au(0)沉积在3DOM二氧化钛大孔壁上。通过跟踪MB的降解来监测光催化活性,并以商业P25(德固赛)和通过乙醇钛水解制备的粉末二氧化钛为活性基准。孔径为0.5微米的大孔3DOM二氧化钛对MB分解的一级速率常数最高,为0.042 min(-1),而P25二氧化钛为0.025 min(-1)。在3DOM二氧化钛表面沉积金会覆盖表面活性位点,从而降低反应速率。