Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density
Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great chall...
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| Published in | Proceedings of the National Academy of Sciences - PNAS Vol. 119; no. 8; pp. 1 - 8 |
|---|---|
| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
National Academy of Sciences
22.02.2022
|
| Subjects | |
| Online Access | Get full text |
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| Abstract | Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N₄ sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electrondepleted Cu-N₄/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N₄ single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N₄/C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N₄ sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts. |
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| AbstractList | The Fenton-like process based on peroxymonosulfate (PMS) has been widely investigated and recognized as a promising alternative in recent years for the degradation of persistent organic pollutants. However, the sluggish kinetics of PMS activation results in prohibitive costs and substantial chemical inputs, impeding its practical applications in water purification. This work demonstrates that tuning the electronic structure of single-atom sites at the atomic level is a powerful approach to achieve superior PMS activation kinetics. The Cu-based catalyst with the optimized electronic structure exhibits superior performance over most of the state-of-the-art heterogeneous Fenton-like catalysts, while homogeneous Cu(II) shows very poor activity. This work provides insights into the electronic structure regulation of metal centers and structure–activity relationship at the atomic level.
Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N
4
sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electron-depleted Cu-N
4
/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N
4
single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N
4
/C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N
4
sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts. Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electron-depleted Cu-N /C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N /C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts. Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N4 sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electron-depleted Cu-N4/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N4 single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N4/C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N4 sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts.Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N4 sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electron-depleted Cu-N4/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N4 single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N4/C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N4 sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts. Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N₄ sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electrondepleted Cu-N₄/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N₄ single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N₄/C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N₄ sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts. Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but how to controllably adjust the electronic configuration of metal centers to further improve the activation kinetics still remains a great challenge. Herein, we report a systematic investigation into heteroatom-doped engineering for tuning the electronic structure of Cu-N4 sites by integrating electron-deficient boron (B) or electron-rich phosphorus (P) heteroatoms into carbon substrate for PMS activation. The electron-depleted Cu-N4/C-B is found to exhibit the most active oxidation capacity among the prepared Cu-N4 single-atom catalysts, which is at the top rankings of the Cu-based catalysts and is superior to most of the state-of-the-art heterogeneous Fenton-like catalysts. Conversely, the electron-enriched Cu-N4/C-P induces a decrease in PMS activation. Both experimental results and theoretical simulations unravel that the long-range interaction with B atoms decreases the electronic density of Cu active sites and down-shifts the d-band center, and thereby optimizes the adsorption energy for PMS activation. This study provides an approach to finely control the electronic structure of Cu-N4 sites at the atomic level and is expected to guide the design of smart Fenton-like catalysts. |
| Author | Chen, Cai Li, Fengting Yang, Jia Yu, Han-Qing Huang, Gui-Xiang Wu, Yuen Wang, Ying Zhou, Xiao Liang, Kuang Chen, Wenxing Qu, Yunteng |
| Author_xml | – sequence: 1 givenname: Xiao surname: Zhou fullname: Zhou, Xiao – sequence: 3 givenname: Gui-Xiang surname: Huang fullname: Huang, Gui-Xiang – sequence: 4 givenname: Cai surname: Chen fullname: Chen, Cai – sequence: 5 givenname: Wenxing surname: Chen fullname: Chen, Wenxing – sequence: 6 givenname: Kuang surname: Liang fullname: Liang, Kuang – sequence: 7 givenname: Yunteng surname: Qu fullname: Qu, Yunteng – sequence: 8 givenname: Jia surname: Yang fullname: Yang, Jia – sequence: 9 givenname: Ying surname: Wang fullname: Wang, Ying – sequence: 10 givenname: Fengting surname: Li fullname: Li, Fengting – sequence: 11 givenname: Han-Qing surname: Yu fullname: Yu, Han-Qing – sequence: 12 givenname: Yuen surname: Wu fullname: Wu, Yuen |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/35165185$$D View this record in MEDLINE/PubMed |
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| Keywords | single-atom catalysts Fenton-like process reaction kinetics heteroatom-doped engineering electronic structure |
| Language | English |
| License | Copyright © 2022 the Author(s). Published by PNAS. This article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND). |
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| Notes | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 14 content type line 23 1X.Z. and M-K.K. contributed equally to this work. Edited by Alexis Bell, Department of Chemical and Biomolecular Engineering, University of California, Berkeley, CA; received October 25, 2021; accepted December 15, 2021 Author contributions: Y. Wang, H.-Q.Y., and Y. Wu designed research; X.Z. and M.-K.K. performed research; G.-X.H., C.C., K.L., and J.Y. contributed new reagents/analytic tools; X.Z., M.-K.K., W.C., Y.Q., and F.L. analyzed data; and X.Z., Y. Wang, H.-Q.Y., and Y. Wu wrote the paper. |
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| Snippet | Developing heterogeneous catalysts with atomically dispersed active sites is vital to boost peroxymonosulfate (PMS) activation for Fenton-like activity, but... The Fenton-like process based on peroxymonosulfate (PMS) has been widely investigated and recognized as a promising alternative in recent years for the... |
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| SubjectTerms | Boron Carbon sources Catalysts Copper Density Electronic structure Electrons Oxidation Phosphorus Physical Sciences Single atom catalysts Substrates |
| Title | Identification of Fenton-like active Cu sites by heteroatom modulation of electronic density |
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