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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| Published in | Nature communications Vol. 14; no. 1; pp. 7841 - 11 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
29.11.2023
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
| ISSN | 2041-1723 2041-1723 |
| DOI | 10.1038/s41467-023-43678-1 |
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| 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 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. |
|---|---|
| AbstractList | 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.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. 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. 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.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. 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. 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. |
| ArticleNumber | 7841 |
| Author | Song, Wenkai Lv, Weiyang Wang, Lixin Rao, Longjun Ran, Maoxi Wu, Zenglong Yao, Yuyuan Shentu, Qikai Li, Hao Xing, Mingyang Zhang, Ziwei |
| Author_xml | – sequence: 1 givenname: Lixin surname: Wang fullname: Wang, Lixin organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 2 givenname: Longjun surname: Rao fullname: Rao, Longjun organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 3 givenname: Maoxi surname: Ran fullname: Ran, Maoxi organization: National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, School of Resources and Environmental Engineering, East China University of Science and Technology – sequence: 4 givenname: Qikai surname: Shentu fullname: Shentu, Qikai organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 5 givenname: Zenglong surname: Wu fullname: Wu, Zenglong organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 6 givenname: Wenkai surname: Song fullname: Song, Wenkai organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 7 givenname: Ziwei surname: Zhang fullname: Zhang, Ziwei organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 8 givenname: Hao surname: Li fullname: Li, Hao organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University – sequence: 9 givenname: Yuyuan surname: Yao fullname: Yao, Yuyuan organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Zhejiang Provincial Innovation Center of Advanced Textile Technology – sequence: 10 givenname: Weiyang orcidid: 0000-0002-7541-4844 surname: Lv fullname: Lv, Weiyang email: wylv@zstu.edu.cn organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, Zhejiang Provincial Innovation Center of Advanced Textile Technology – sequence: 11 givenname: Mingyang orcidid: 0000-0002-0518-2849 surname: Xing fullname: Xing, Mingyang email: mingyangxing@ecust.edu.cn organization: National Engineering Lab of Textile Fiber Materials & Processing Technology (Zhejiang), Zhejiang Sci-Tech University, National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery, School of Resources and Environmental Engineering, East China University of Science and Technology |
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| Snippet | The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is... Abstract The development of heterogenous catalysts based on the synthesis of 2D carbon-supported metal nanocatalysts with high metal loading and dispersion is... |
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| SubjectTerms | 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 |
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| Title | A polymer tethering strategy to achieve high metal loading on catalysts for Fenton reactions |
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