<p>The liquid-phase selective oxidation of benzyl alcohol (BZA) by atmospheric oxygen is a more sustainable and cleaner strategy for the synthesis of benzaldehyde (BZL) compared with the traditional hydrolysis of chlorobenzene. Herein, a series of C<sub>3</sub>N<sub>4</sub>–CeO<sub>2</sub> composites were prepared and then utilized as catalyst supports to load Pd nanoparticles. The effects of the amount of carbon nitride (C<sub>3</sub>N<sub>4</sub>) and the calcination conditions on the physicochemical properties of C<sub>3</sub>N<sub>4</sub>–CeO<sub>2</sub> materials were investigated. In the solvent-free selective oxidation of BZA, the Pd/C<sub>3</sub>N<sub>4</sub>–CeO<sub>2</sub> materials demonstrated higher catalytic activity than Pd/C<sub>3</sub>N<sub>4</sub> and Pd/CeO<sub>2</sub>. Under the reaction temperature of 90&#xa0;°C and 4 mL of BZA, the BZA conversion could reach 84.6%, whereas the selectivity of benzaldehyde was 98.7%. In addition, the solid catalyst could be reused six times while the conversion did not significantly decrease. Based on the characterization results, the possible catalytically active sites of 2Pd/C<sub>3</sub>N<sub>4</sub>–CeO<sub>2</sub>-1 for the selective oxidation of BZA were Ce<sup>3+</sup> and oxygen vacancies, and the introduction of C<sub>3</sub>N<sub>4</sub> effectively increased the content of these two species.</p> Graphical Abstract <p></p>

错误:搜索内容不能为空,请输入英文关键词
错误:关键词超出字数限制,请精简
高级检索

Preparation of Pd Nanocatalysts Supported on C3N4–CeO2 Composites for Solvent-Free and Atmospheric Selective Oxidation of Benzyl Alcohol

  • Xiao-Yan Wang,
  • Ya-Jing Wang,
  • Fei Wang,
  • Jie Xu,
  • Bing Xue

摘要

The liquid-phase selective oxidation of benzyl alcohol (BZA) by atmospheric oxygen is a more sustainable and cleaner strategy for the synthesis of benzaldehyde (BZL) compared with the traditional hydrolysis of chlorobenzene. Herein, a series of C3N4–CeO2 composites were prepared and then utilized as catalyst supports to load Pd nanoparticles. The effects of the amount of carbon nitride (C3N4) and the calcination conditions on the physicochemical properties of C3N4–CeO2 materials were investigated. In the solvent-free selective oxidation of BZA, the Pd/C3N4–CeO2 materials demonstrated higher catalytic activity than Pd/C3N4 and Pd/CeO2. Under the reaction temperature of 90 °C and 4 mL of BZA, the BZA conversion could reach 84.6%, whereas the selectivity of benzaldehyde was 98.7%. In addition, the solid catalyst could be reused six times while the conversion did not significantly decrease. Based on the characterization results, the possible catalytically active sites of 2Pd/C3N4–CeO2-1 for the selective oxidation of BZA were Ce3+ and oxygen vacancies, and the introduction of C3N4 effectively increased the content of these two species.

Graphical Abstract