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

• Published in: Nature communications Vol. 14; no. 1; pp. 7841 - 11
• Main Authors: Wang, Lixin, Rao, Longjun, Ran, Maoxi, Shentu, Qikai, Wu, Zenglong, Song, Wenkai, Zhang, Ziwei, Li, Hao, Yao, Yuyuan, Lv, Weiyang, Xing, Mingyang
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 29.11.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 140/146; 147/135; 147/143; 639/301/299; 639/638/298; 704/172/169/896; Carbon; Catalysts; Catalytic activity; Catechol; Chemical synthesis; Confinement; Dispersion; Electron density; Fabrication; Humanities and Social Sciences; Hydrogen peroxide; Iron; Metal ions; Metals; multidisciplinary; Nanocrystals; Polymerization; Polymers; Science; Science (multidisciplinary); Sulfamethoxazole; Tethering; Ultrafines
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-43678-1

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. This work reports a self-polymerization confinement strategy to develop and synthesize carbon-supported metal catalysts with high metal loading. Efficient Fenton reactivity is observed for samples containing well dispersed iron sites.