期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.2c06224
关键词
porous carbon nitride; Fe clusters; photocatalysis; phenol; H2O2 activation
In this work, ultra-small Fe clusters embedded in a 3D porous interconnected open-framework g-C3N4 were successfully fabricated by the combination of a mechanochemical reaction with one-step pyrolysis. The novel Fe cluster catalyst exhibited high activity and stability in phenol synthesis, with a maximum phenol yield of 28.1% in visible light. Our work provides valuable information on the development of active metal cluster nanocatalysts for organic synthesis.
An Fe-based heterogeneous catalyst is an attractive Fenton-like catalyst for phenol synthesis due to many advantages. Nevertheless, it is challenging to control the particle size in various high-loading Fe-based materials, which limits its activity and selectivity. In this work, ultra-small Fe clusters embedded in a 3D porous interconnected open-framework g-C3N4 (denoted FeNx/CCN) were successfully fabricated by the combination of a mechanochemical reaction with one-step pyrolysis. Various characterization results showed that ultra-small Fe clusters with a high loading of 32% were uniformly distributed in the hierarchical porous carbon nitride, which offered an access for faster transportation of charge carriers. Fe sites were probably coordinated with carbon nitride by Fe2+-C N-Fe3+ and Fe-N-x bonding. High-density Fe clusters could provide abundant active sites and improve the light absorption and the activating ability of H2O2. By taking advantage of semiconductor functions in combination with a rich porous structure and high-density active sites, the novel Fe cluster catalyst exhibited high activity and stability in phenol synthesis, with a maximum phenol yield of 28.1% in visible light. Combining the experimental results with Fenton chemistry, we proposed a possible photocatalytic reaction mechanism. Our work will give valuable information on the development of active metal cluster nanocatalysts for organic synthesis.
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