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基于石墨烯/ZnO 多杂交纳米结构的光化学合成贵金属(Ag、Pd、Au、Pt)作为 H2O2 还原的电催化剂。

Photochemical synthesis of noble metal (Ag, Pd, Au, Pt) on graphene/ZnO multihybrid nanoarchitectures as electrocatalysis for H2O2 reduction.

机构信息

Department of Chemistry, East China Normal University, 500 Dongchuan Road, Shanghai, 200241, P.R. China.

出版信息

ACS Appl Mater Interfaces. 2013 Jul 24;5(14):6762-8. doi: 10.1021/am401738k. Epub 2013 Jul 8.

Abstract

For the first time, a series of noble metal (Ag, Au, Pd, and Pt) nanoparticles (NPs) based on new functional graphene were successfully achieved via UV-assisted photocatalytic reduction by ZnO nanorods. The whole preparation strategy for constructing noble metal deposited graphene sheets/ZnO (GS/ZnO) was elucidated in detail in this work. First, graphene oxide based two-dimensional carbon nanostructures served as a support to disperse ZnO nanorods through a hydrothermal route. The ZnO nanorods were self-assembled onto the surface of graphene sheets, forming GS/ZnO nanocomposite, and the graphene oxide was reduced, yielding reduced graphene sheets in this synthetic procedure. Second, the GS/ZnO films were further employed as supporting materials for the dispersion of metal nanoparticles. Photogenerated electrons from UV-irradiated ZnO were transported across GS to stepwise and respectively reduce v μL metal ions (Ag(+), Pd(2+), AuCl4(-), PtCl6(2-), 20 mg/mL) into metal (Ag, Pd, Au, Pt) NPs at a location distinct from the ZnO anchored site, forming five graphene-based hybrid nanocomposites designated as GS/ZnO, GS/ZnO@Agv, GS/ZnO@Pdv, GS/ZnO@Auv, GS/ZnO@Ptv, respectively. The obtained mutihybrid nanoarchitectured materials were clearly characterized by transmission electron microscopy (TEM) and X-ray diffraction (XRD). According to the diameters and distribution, the four metal NPs on GS/ZnO were divided into two categories: Ag&Au and Pd&Pt. Their difference was rooted in the rival abilities of gathering electron between graphene and different metal islands in the photochemical reduction process. The electrochemical behaviors of the five resultant hybrid nanocomposites were investigated in H2O2 as well as in potassium ferricyanide (Fe(CN)6(3-/4-)) and displayed distinct electrocatalytic activity.

摘要

首次通过 ZnO 纳米棒的 UV 辅助光催化还原,成功地基于新型功能化石墨烯制备了一系列贵金属(Ag、Au、Pd 和 Pt)纳米粒子(NPs)。本工作详细阐述了构建贵金属沉积石墨烯片/ZnO(GS/ZnO)的整个制备策略。首先,基于氧化石墨烯的二维碳纳米结构通过水热途径作为支撑来分散 ZnO 纳米棒。通过该合成过程,ZnO 纳米棒自组装到石墨烯片的表面上,形成 GS/ZnO 纳米复合材料,并且氧化石墨烯被还原,生成还原氧化石墨烯。其次,GS/ZnO 薄膜进一步用作分散金属纳米粒子的支撑材料。UV 照射的 ZnO 产生的光生电子通过 GS 传输,分别将 v μL 金属离子(Ag(+)、Pd(2+)、AuCl4(-)、PtCl6(2-),20 mg/mL)逐步还原成金属(Ag、Pd、Au、Pt)纳米粒子,位置与 ZnO 锚定位置不同,形成五种基于石墨烯的杂化纳米复合材料,分别命名为 GS/ZnO、GS/ZnO@Agv、GS/ZnO@Pdv、GS/ZnO@Auv、GS/ZnO@Ptv。通过透射电子显微镜(TEM)和 X 射线衍射(XRD)清楚地对所得多杂化纳米结构材料进行了表征。根据直径和分布,GS/ZnO 上的四种金属 NPs 分为两类:Ag&Au 和 Pd&Pt。它们的区别源于在光化学还原过程中石墨烯和不同金属岛聚集电子的能力差异。还研究了五种所得杂化纳米复合材料在 H2O2 以及铁氰化钾(Fe(CN)6(3-/4-))中的电化学行为,显示出明显的电催化活性。

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