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A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions

The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is important. However, such practices remain challenging to develop. Here, we report a self-polymerization confinement strategy to fabricate a series of...

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Detalles Bibliográficos
Autores principales: Wang, Lixin, Rao, Longjun, Ran, Maoxi, Shentu, Qikai, Wu, Zenglong, Song, Wenkai, Zhang, Ziwei, Li, Hao, Yao, Yuyuan, Lv, Weiyang, Xing, Mingyang
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10687042/
https://www.ncbi.nlm.nih.gov/pubmed/38030639
http://dx.doi.org/10.1038/s41467-023-43678-1
Descripción
Sumario:The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is important. However, such practices remain challenging to develop. Here, we report a self-polymerization confinement strategy to fabricate a series of ultrafine metal embedded N-doped carbon nanosheets (M@N-C) with loadings of up to 30 wt%. Systematic investigation confirms that abundant catechol groups for anchoring metal ions and entangled polymer networks with the stable coordinate environment are essential for realizing high-loading M@N-C catalysts. As a demonstration, Fe@N-C exhibits the dual high-efficiency performance in Fenton reaction with both impressive catalytic activity (0.818 min(−1)) and H(2)O(2) utilization efficiency (84.1%) using sulfamethoxazole as the probe, which has not yet been achieved simultaneously. Theoretical calculations reveal that the abundant Fe nanocrystals increase the electron density of the N-doped carbon frameworks, thereby facilitating the continuous generation of long-lasting surface-bound (•)OH through lowering the energy barrier for H(2)O(2) activation. This facile and universal strategy paves the way for the fabrication of diverse high-loading heterogeneous catalysts for broad applications.