Construction of High-Density Fe Clusters Embedded in a Porous Carbon Nitride Catalyst with Effectively Selective Transformation of Benzene

被引:17
作者
Chen, Xiao [1 ]
Cheng, Lanlan [1 ]
Yang, Yiguo [1 ]
Chen, Xiufang [1 ]
Chen, Fengtao [1 ]
Lu, Wangyang [1 ]
机构
[1] Zhejiang Sci Tech Univ, Natl Engn Lab Text Fiber Mat & Proc Technol Zhejia, Hangzhou 310018, Peoples R China
关键词
porous carbon nitride; Fe clusters; photocatalysis; phenol; H2O2; activation; FACILE SYNTHESIS; PHENOL; HYDROXYLATION; OXIDATION; G-C3N4; PHOSPHORUS; REDUCTION; COMPLEXES;
D O I
10.1021/acssuschemeng.2c06224
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:1518 / 1526
页数:9
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