Steinebrunner David, Schnurpfeil Günter, Wöhrle Dieter, Wittstock Arne
Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology, University Bremen Leobener Str. UFT 28359 Bremen Germany
MAPEX Center for Materials and Processes, University Bremen Bibliothekstr. 1 28359 Bremen Germany.
RSC Adv. 2019 Dec 23;10(1):53-59. doi: 10.1039/c9ra08841e. eCollection 2019 Dec 20.
A series of singlet oxygen sensitizing hybrid materials is reported consisting of a zinc(ii) phthalocyanine (ZnPc) derivative immobilized on nanoporous gold leafs (npAu) with various pore sizes. The resulting photocatalytic coatings exhibit a thickness of around 100 nm and pore sizes between 9-50 nm. Herein, we report the synthesis and characterization of those hybrid materials which were synthesized by functionalization of npAu leafs by an azide terminated alkanethiol self-assembled monolayer (SAM) and subsequent copper catalyzed azide-alkyne cycloaddition (CuAAC). The characterization of the samples morphology included scanning electron microscopy (SEM), UV-Vis spectroscopy as well as energy dispersive X-ray spectroscopy (EDX). The morphology-reactivity relationship was investigated employing the hybrid photocatalysts in the photooxidation of diphenylisobenzofuran (DPBF) as selective singlet oxygen quencher. An increasing photocatalytic activity was found for smaller pore sizes up to 15 nm, due to the gain in specific surface area concomitant with an increasing amount of immobilized photosensitizer, completely dominating the effect of the higher spectral overlap caused by the shift of the plasmon resonance of npAu, until mass transport and diffusion limitation gets predominant for pore sizes below 15 nm.
报道了一系列单线态氧敏化杂化材料,其由固定在具有不同孔径的纳米多孔金箔(npAu)上的锌(II)酞菁(ZnPc)衍生物组成。所得的光催化涂层厚度约为100nm,孔径在9 - 50nm之间。在此,我们报道了这些杂化材料的合成与表征,它们是通过叠氮基封端的烷硫醇自组装单分子层(SAM)对npAu箔进行功能化,随后进行铜催化的叠氮 - 炔环加成反应(CuAAC)合成的。样品形态的表征包括扫描电子显微镜(SEM)、紫外 - 可见光谱以及能量色散X射线光谱(EDX)。利用杂化光催化剂在作为选择性单线态氧猝灭剂的二苯基异苯并呋喃(DPBF)的光氧化反应中研究了形态 - 反应性关系。发现对于孔径小至15nm的情况,光催化活性增加,这是由于比表面积的增加以及固定化光敏剂数量的增加,完全主导了由npAu的等离子体共振位移引起的更高光谱重叠的影响,直到对于孔径低于15nm时质量传输和扩散限制占主导地位。