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

Lixin Wang, Longjun Rao, Maoxi Ran, Qikai Shentu, Zenglong Wu, Wenkai Song, Ziwei Zhang, Hao Li, Yuyuan Yao, Weiyang Lv () and Mingyang Xing ()
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Lixin Wang: Zhejiang Sci-Tech University
Longjun Rao: Zhejiang Sci-Tech University
Maoxi Ran: East China University of Science and Technology
Qikai Shentu: Zhejiang Sci-Tech University
Zenglong Wu: Zhejiang Sci-Tech University
Wenkai Song: Zhejiang Sci-Tech University
Ziwei Zhang: Zhejiang Sci-Tech University
Hao Li: Zhejiang Sci-Tech University
Yuyuan Yao: Zhejiang Sci-Tech University
Weiyang Lv: Zhejiang Sci-Tech University
Mingyang Xing: Zhejiang Sci-Tech University

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract 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 H2O2 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 H2O2 activation. This facile and universal strategy paves the way for the fabrication of diverse high-loading heterogeneous catalysts for broad applications.

Date: 2023
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DOI: 10.1038/s41467-023-43678-1

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