Synergistic Effect in Zinc Phthalocyanine—Nanoporous Gold Hybrid Materials for Enhanced Photocatalytic Oxidations

Synergistic Effect in Zinc Phthalocyanine—Nanoporous Gold Hybrid Materials for Enhanced Photocatalytic Oxidations
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DOI:
10.3390/catal9060555
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发表时间:
2019-06
期刊:
影响因子:
3.9
通讯作者:
David Steinebrunner;G. Schnurpfeil;A. Wichmann;D. Wöhrle;Arne Wittstock
David Steinebrunner;G. Schnurpfeil;A. Wichmann;D. Wöhrle;Arne Wittstock
中科院分区:
化学3区
文献类型:
--
作者:
David Steinebrunner;G. Schnurpfeil;A. Wichmann;D. Wöhrle;Arne Wittstock

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通过腐蚀Au-Ag合金制备了纳米多孔金(npAu)载体。npAu材料具有如通过扫描电子显微镜(SEM)所示的在40 nm范围内的孔径。表面改性的自组装单分子层(SAM)与叠氮己基硫代酸盐,然后官能化的锌(II)酞菁(ZnPc)衍生物使用“点击化学”。用原子吸收光谱法(AAS)和电感耦合等离子体质谱法(ICP-MS)测定了锌的含量,并计算了锌酞菁在npAu上的固定量。能量色散X射线(EDX)光谱给出了整个多孔结构的ZnPc的空间分布的信息。NpAu和ZnPc在可见光区都有很强的光吸收,因此,本文研究了它们作为光催化剂对分子氧的光氧化反应。通过照射的混合系统,单线态氧的形成,这是量化使用的光氧化的1,3-二苯基异苯并呋喃(DPBF)作为选择性单线态氧猝灭剂。优化了npAu-ZnPc混合体系的受照表面积和ZnPc的覆盖范围。npAu和光敏剂ZnPc的等离子体共振之间的协同效应,显示通过选择性照射和激发的酞菁,npAu的支持和两个吸收带的等离子体共振同时,导致在增强的光氧化活性的近一个数量级。
Nanoporous gold (npAu) supports were prepared as disks and powders by corrosion of Au-Ag alloys. The npAu materials have pore sizes in the range of 40 nm as shown by scanning electron microscopy (SEM). The surface was modified by a self-assembled monolayer (SAM) with an azidohexylthioate and then functionalized by a zinc (II) phthalocyanine (ZnPc) derivative using “click chemistry”. By atomic absorption spectroscopy (AAS) and inductively coupled plasma mass spectrometry (ICP-MS) the content of zinc was determined and the amount of immobilized ZnPc on npAu was calculated. Energy-dispersive X-ray (EDX) spectroscopy gave information about the spatial distribution of the ZnPc throughout the whole porous structure. NpAu and ZnPc are both absorbing light in the visible region, therefore, the heterogeneous hybrid systems were studied as photocatalysts for photooxidations using molecular oxygen. By irradiation of the hybrid system, singlet oxygen is formed, which was quantified using the photooxidation of 1,3-diphenylisobenzofuran (DPBF) as a selective singlet oxygen quencher. The illuminated surface area of the npAu-ZnPc hybrid system and the coverage of the ZnPc were optimized. The synergistic effect between the plasmon resonance of npAu and the photosensitizer ZnPc was shown by selective irradiation and excitation of only the phthalocyanine, the plasmon resonance of the npAu support and both absorption bands simultaneously, resulting in an enhanced photooxidation activity by nearly an order of magnitude.