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首页> 外文期刊>RSC Advances >Aqueous solution photocatalytic synthesis of p-anisaldehyde by using graphite-like carbon nitride photocatalysts obtained via the hard-templating route
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Aqueous solution photocatalytic synthesis of p-anisaldehyde by using graphite-like carbon nitride photocatalysts obtained via the hard-templating route

机译：通过使用硬模板途径获得的石墨氮化物光催化剂，使用石墨氮化物光催化剂来光催化合成p-苯甲酰盐

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Graphite-like carbon nitride (GCN)-based materials were developed via the hard-templating route, using dicyandiamide as the GCN precursor and silica templates. That resulted in urchin-like GCN (GCN-UL), 3D ordered macroporous GCN (GCN-OM) and mesoporous GCN (GCN-MP). The introduction of silica templates during GCN synthesis produced physical defects on its surface, as confirmed by SEM analysis, increasing their specific surface area. A high amount of nitrogen vacancies is present in modified catalysts (revealed by XPS measurements), which can be related to an increase in the reactive sites available to catalyse redox reactions. The textural and morphological modifications induced in GCN an enhanced light absorption capacity and reduced electron/hole recombination rate, contributing to its improved photocatalytic performance. In the photocatalytic conversion of p-anisyl alcohol to p-anisaldehyde in deoxygenated aqueous solutions under UV-LED irradiation, the GCN-UL was the best photocatalyst reaching 60% yield at 64% conversion for p-anisaldehyde production after 240 min of reaction. Under oxygenated conditions (air), the process efficiency was increased to 79% yield at 92% conversion only after 90 min reaction. The GCN-based photocatalyst kept its performance when using visible-LED radiation under air atmosphere. Trapping of photogenerated holes and radicals by selective scavengers showed that under deoxygenated conditions, holes played the primary role in the p-anisaldehyde synthesis. Under oxygenated conditions, the process is governed by the effect of reactive oxygen species, namely superoxide radicals, with a significant contribution from holes.
机译：通过硬质模板途径，使用双氰胺作为GCN前体和二氧化硅模板，通过硬模板途径显影石墨氮化物（GCN）的材料。它导致核苷类GCN（GCN-UL），3D有序的大孔GCN（GCN-OM）和中孔GCN（GCN-MP）。在GCN合成期间引入二氧化硅模板在其表面产生物理缺陷，如SEM分析所确认，增加其特定表面积。在改性催化剂（通过XPS测量显示）中存在高量的氮空位，其可以与可用于催化氧化还原反应的反应性位点的增加有关。 GCN诱导的纹理和形态学改性增强了光吸收能力和降低的电子/空穴复合速率，有助于其改善的光催化性能。在UV-LED照射下的脱氧水溶液中对亚吲哚醇的光催化转化为脱氧水溶液，GCN-UL是最佳的光催化剂，在240分钟反应后对P-苯甲酰醛产生的64％转化率达到60％产率。在氧化条件下（空气），在90分钟后，该过程效率仅在92％转化率下升高至79％。基于GCN的光催化剂在空气气氛下使用可见光辐射时保持其性能。通过选择性清除剂捕获光静脉孔和自由基表明，在脱氧条件下，孔在对丙醛合成中发挥着主要作用。在含氧条件下，该方法受反应性氧物种，即超氧基自由基的影响，具有孔的显着贡献。

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  • 来源
    《RSC Advances》 |2020年第33期|共12页
  • 作者

    Fernandes Raquel; Sampaio Maria J.; Faria Joaquim L.; Silva Claudia G.;

  • 作者单位

    Univ Porto Lab Separat &

    React Engn Lab Catalysis &

    Mat LSRE LCM Fac Engn Rua Dr Roberto Frias S-N P-4200465 Porto Portugal;

    Univ Porto Lab Separat &

    React Engn Lab Catalysis &

    Mat LSRE LCM Fac Engn Rua Dr Roberto Frias S-N P-4200465 Porto Portugal;

    Univ Porto Lab Separat &

    React Engn Lab Catalysis &

    Mat LSRE LCM Fac Engn Rua Dr Roberto Frias S-N P-4200465 Porto Portugal;

    Univ Porto Lab Separat &

    React Engn Lab Catalysis &

    Mat LSRE LCM Fac Engn Rua Dr Roberto Frias S-N P-4200465 Porto Portugal;

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