Breaking the Scaling Relationship in Water Oxidation Enabled by the Electron Buffering Effect of the Fullerene Network
The scaling relationship among reaction intermediates with strongly correlated adsorption energy in the oxygen evolution reaction (OER) severely restricts the energy-conversion efficiency of water electrolysis. For the conventional adsorbate evolution mechanism, breaking the scaling relationship rem...
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| Published in | Journal of the American Chemical Society Vol. 147; no. 24; pp. 20600 - 20611 |
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| Main Authors | , , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
18.06.2025
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| Abstract | The scaling relationship among reaction intermediates with strongly correlated adsorption energy in the oxygen evolution reaction (OER) severely restricts the energy-conversion efficiency of water electrolysis. For the conventional adsorbate evolution mechanism, breaking the scaling relationship remains challenging, as it is difficult to modulate the adsorption of multiple intermediates on a specific active site simultaneously. Herein, we utilize the electron buffering effect of a two-dimensional fullerene network (C60NET) to dynamically tune the electronic structure of the iridium (Ir) active site with the change of adsorbed intermediates, which can tailor the adsorption strength of intermediates from multistep reactions and break the adsorption-energy scaling relationships among *OOH, *O, and *OH. The C60NET-buffered Ir nanocluster catalyst exhibits excellent OER activity with a low overpotential of 237 mV and stability over 600 h at 10 mA cm–2, outperforming graphene-supported Ir nanoclusters and commercial IrO x , attributed to the breaking of the linear scaling relationship enabled by the unique ability to reversibly accept and donate electrons of C60NET. |
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| AbstractList | The scaling relationship among reaction intermediates with strongly correlated adsorption energy in the oxygen evolution reaction (OER) severely restricts the energy-conversion efficiency of water electrolysis. For the conventional adsorbate evolution mechanism, breaking the scaling relationship remains challenging, as it is difficult to modulate the adsorption of multiple intermediates on a specific active site simultaneously. Herein, we utilize the electron buffering effect of a two-dimensional fullerene network (C
NET) to dynamically tune the electronic structure of the iridium (Ir) active site with the change of adsorbed intermediates, which can tailor the adsorption strength of intermediates from multistep reactions and break the adsorption-energy scaling relationships among *OOH, *O, and *OH. The C
NET-buffered Ir nanocluster catalyst exhibits excellent OER activity with a low overpotential of 237 mV and stability over 600 h at 10 mA cm
, outperforming graphene-supported Ir nanoclusters and commercial IrO
, attributed to the breaking of the linear scaling relationship enabled by the unique ability to reversibly accept and donate electrons of C
NET. The scaling relationship among reaction intermediates with strongly correlated adsorption energy in the oxygen evolution reaction (OER) severely restricts the energy-conversion efficiency of water electrolysis. For the conventional adsorbate evolution mechanism, breaking the scaling relationship remains challenging, as it is difficult to modulate the adsorption of multiple intermediates on a specific active site simultaneously. Herein, we utilize the electron buffering effect of a two-dimensional fullerene network (C60NET) to dynamically tune the electronic structure of the iridium (Ir) active site with the change of adsorbed intermediates, which can tailor the adsorption strength of intermediates from multistep reactions and break the adsorption-energy scaling relationships among *OOH, *O, and *OH. The C60NET-buffered Ir nanocluster catalyst exhibits excellent OER activity with a low overpotential of 237 mV and stability over 600 h at 10 mA cm-2, outperforming graphene-supported Ir nanoclusters and commercial IrOx, attributed to the breaking of the linear scaling relationship enabled by the unique ability to reversibly accept and donate electrons of C60NET.The scaling relationship among reaction intermediates with strongly correlated adsorption energy in the oxygen evolution reaction (OER) severely restricts the energy-conversion efficiency of water electrolysis. For the conventional adsorbate evolution mechanism, breaking the scaling relationship remains challenging, as it is difficult to modulate the adsorption of multiple intermediates on a specific active site simultaneously. Herein, we utilize the electron buffering effect of a two-dimensional fullerene network (C60NET) to dynamically tune the electronic structure of the iridium (Ir) active site with the change of adsorbed intermediates, which can tailor the adsorption strength of intermediates from multistep reactions and break the adsorption-energy scaling relationships among *OOH, *O, and *OH. The C60NET-buffered Ir nanocluster catalyst exhibits excellent OER activity with a low overpotential of 237 mV and stability over 600 h at 10 mA cm-2, outperforming graphene-supported Ir nanoclusters and commercial IrOx, attributed to the breaking of the linear scaling relationship enabled by the unique ability to reversibly accept and donate electrons of C60NET. The scaling relationship among reaction intermediates with strongly correlated adsorption energy in the oxygen evolution reaction (OER) severely restricts the energy-conversion efficiency of water electrolysis. For the conventional adsorbate evolution mechanism, breaking the scaling relationship remains challenging, as it is difficult to modulate the adsorption of multiple intermediates on a specific active site simultaneously. Herein, we utilize the electron buffering effect of a two-dimensional fullerene network (C60NET) to dynamically tune the electronic structure of the iridium (Ir) active site with the change of adsorbed intermediates, which can tailor the adsorption strength of intermediates from multistep reactions and break the adsorption-energy scaling relationships among *OOH, *O, and *OH. The C60NET-buffered Ir nanocluster catalyst exhibits excellent OER activity with a low overpotential of 237 mV and stability over 600 h at 10 mA cm–2, outperforming graphene-supported Ir nanoclusters and commercial IrO x , attributed to the breaking of the linear scaling relationship enabled by the unique ability to reversibly accept and donate electrons of C60NET. |
| Author | Xiao, Yukun Yang, Shangfeng Li, Hexing Liu, Dongming Wang, Xing Da, Yumin Xi, Shibo Chen, Xiang Ma, Hao Chen, Wei Lum, Yanwei Wu, Yao Sun, Yuanmiao Fan, Lei Jin, Hongqiang Wang, Sibo Jiang, Rui He, Qian |
| AuthorAffiliation | Department of Chemistry Agency for Science, Technology and Research (ASTAR) Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology National University of Singapore School of Materials Science and Engineering, Key Lab of Efficient Conversion and Solid-State Storage of Hydrogen & Electricity Institute of Sustainability for Chemicals, Energy and Environment (ISCE2) Department of Chemical and Biomolecular Engineering Hefei National Laboratory for Physical Sciences at Microscale, State Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Anhui Laboratory of Advanced Photon Science and Technology, Department of Materials Science and Engineering Department of Material Science and Engineering, College of Design and Engineering The Education Ministry Key Lab of Resource Chemistry, Joint International Research Laboratory of Resource Chemistry of Ministry of Education, Shanghai Key Laboratory of |
| AuthorAffiliation_xml | – name: Hefei National Laboratory for Physical Sciences at Microscale, State Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Anhui Laboratory of Advanced Photon Science and Technology, Department of Materials Science and Engineering – name: Department of Material Science and Engineering, College of Design and Engineering – name: The Education Ministry Key Lab of Resource Chemistry, Joint International Research Laboratory of Resource Chemistry of Ministry of Education, Shanghai Key Laboratory of Rare Earth Functional Materials, and Shanghai Frontiers Science Center of Biomimetic Catalysis – name: Department of Chemistry – name: Institute of Sustainability for Chemicals, Energy and Environment (ISCE2) – name: Department of Chemical and Biomolecular Engineering – name: Agency for Science, Technology and Research (ASTAR) – name: School of Materials Science and Engineering, Key Lab of Efficient Conversion and Solid-State Storage of Hydrogen & Electricity – name: Department of Physics – name: Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology – name: National University of Singapore |
| Author_xml | – sequence: 1 givenname: Xiang orcidid: 0000-0002-8480-4203 surname: Chen fullname: Chen, Xiang organization: Department of Chemistry – sequence: 2 givenname: Hao surname: Ma fullname: Ma, Hao organization: Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology – sequence: 3 givenname: Xing surname: Wang fullname: Wang, Xing organization: Hefei National Laboratory for Physical Sciences at Microscale, State Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Anhui Laboratory of Advanced Photon Science and Technology, Department of Materials Science and Engineering – sequence: 4 givenname: Hongqiang orcidid: 0009-0001-6171-5718 surname: Jin fullname: Jin, Hongqiang email: hqjin@nus.edu.sg organization: Department of Chemistry – sequence: 5 givenname: Yao surname: Wu fullname: Wu, Yao organization: Department of Material Science and Engineering, College of Design and Engineering – sequence: 6 givenname: Sibo surname: Wang fullname: Wang, Sibo organization: Department of Chemical and Biomolecular Engineering – sequence: 7 givenname: Yukun surname: Xiao fullname: Xiao, Yukun organization: Department of Chemistry – sequence: 8 givenname: Rui surname: Jiang fullname: Jiang, Rui organization: Department of Chemistry – sequence: 9 givenname: Yumin surname: Da fullname: Da, Yumin organization: Department of Chemistry – sequence: 10 givenname: Lei surname: Fan fullname: Fan, Lei organization: Department of Chemistry – sequence: 11 givenname: Yuanmiao orcidid: 0000-0003-4650-5226 surname: Sun fullname: Sun, Yuanmiao email: sunym@siat.ac.cn organization: Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology – sequence: 12 givenname: Shibo orcidid: 0000-0002-8521-3237 surname: Xi fullname: Xi, Shibo organization: Agency for Science, Technology and Research (ASTAR) – sequence: 13 givenname: Yanwei orcidid: 0000-0001-7261-2098 surname: Lum fullname: Lum, Yanwei organization: Department of Chemical and Biomolecular Engineering – sequence: 14 givenname: Qian surname: He fullname: He, Qian organization: Department of Material Science and Engineering, College of Design and Engineering – sequence: 15 givenname: Hexing orcidid: 0000-0002-3558-5227 surname: Li fullname: Li, Hexing organization: The Education Ministry Key Lab of Resource Chemistry, Joint International Research Laboratory of Resource Chemistry of Ministry of Education, Shanghai Key Laboratory of Rare Earth Functional Materials, and Shanghai Frontiers Science Center of Biomimetic Catalysis – sequence: 16 givenname: Dongming surname: Liu fullname: Liu, Dongming organization: School of Materials Science and Engineering, Key Lab of Efficient Conversion and Solid-State Storage of Hydrogen & Electricity – sequence: 17 givenname: Shangfeng orcidid: 0000-0002-6931-9613 surname: Yang fullname: Yang, Shangfeng email: sfyang@ustc.edu.cn organization: Hefei National Laboratory for Physical Sciences at Microscale, State Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Anhui Laboratory of Advanced Photon Science and Technology, Department of Materials Science and Engineering – sequence: 18 givenname: Wei orcidid: 0000-0002-1131-3585 surname: Chen fullname: Chen, Wei email: phycw@nus.edu.sg organization: National University of Singapore |
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| Title | Breaking the Scaling Relationship in Water Oxidation Enabled by the Electron Buffering Effect of the Fullerene Network |
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