Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis
Abstract Dual-atom catalysts featuring synergetic dinuclear active sites, have the potential of breaking the linear scaling relationship of the well-established single-atom catalysts for oxygen reduction reaction; however, the design of dual-atom catalysts with rationalized local microenvironment fo...
Saved in:
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2025-01-01
|
| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-56066-8 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1832585605083561984 |
|---|---|
| author | Zhen Zhang Zhenyu Xing Xianglin Luo Chong Cheng Xikui Liu |
| author_facet | Zhen Zhang Zhenyu Xing Xianglin Luo Chong Cheng Xikui Liu |
| author_sort | Zhen Zhang |
| collection | DOAJ |
| description | Abstract Dual-atom catalysts featuring synergetic dinuclear active sites, have the potential of breaking the linear scaling relationship of the well-established single-atom catalysts for oxygen reduction reaction; however, the design of dual-atom catalysts with rationalized local microenvironment for high activity and selectivity remains a great challenge. Here we design a bisalphen ladder polymer with well-defined densely populated binuclear cobalt sites on Ketjenblack substrates. The strong electron coupling effect between the fully-conjugated ladder structure and carbon substrates enhances the electron transfer between the cobalt center and oxygen intermediates, inducing the low-to-high spin transition for the 3d electron of Co(II). In situ techniques and theoretical calculations reveal the dynamic evolution of Co2N4O2 active sites and reaction intermediates. In alkaline conditions, the catalyst exhibits impressive oxygen reduction reaction activity featuring an onset potential of 1.10 V and a half-wave potential of 1.00 V, insignificant decay after 30,000 cycles, pushing the overpotential boundaries of ORR electrocatalysis to a low level. This work provides a platform for designing efficient dual-atom catalysts with well-defined coordination and electronic structures in energy conversion technologies. |
| format | Article |
| id | doaj-art-ef908eee4afb4b0b9e1ff9e9392e3a65 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-ef908eee4afb4b0b9e1ff9e9392e3a652025-01-26T12:40:28ZengNature PortfolioNature Communications2041-17232025-01-0116111210.1038/s41467-025-56066-8Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysisZhen Zhang0Zhenyu Xing1Xianglin Luo2Chong Cheng3Xikui Liu4College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan UniversityCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan UniversityCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan UniversityCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan UniversityCollege of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan UniversityAbstract Dual-atom catalysts featuring synergetic dinuclear active sites, have the potential of breaking the linear scaling relationship of the well-established single-atom catalysts for oxygen reduction reaction; however, the design of dual-atom catalysts with rationalized local microenvironment for high activity and selectivity remains a great challenge. Here we design a bisalphen ladder polymer with well-defined densely populated binuclear cobalt sites on Ketjenblack substrates. The strong electron coupling effect between the fully-conjugated ladder structure and carbon substrates enhances the electron transfer between the cobalt center and oxygen intermediates, inducing the low-to-high spin transition for the 3d electron of Co(II). In situ techniques and theoretical calculations reveal the dynamic evolution of Co2N4O2 active sites and reaction intermediates. In alkaline conditions, the catalyst exhibits impressive oxygen reduction reaction activity featuring an onset potential of 1.10 V and a half-wave potential of 1.00 V, insignificant decay after 30,000 cycles, pushing the overpotential boundaries of ORR electrocatalysis to a low level. This work provides a platform for designing efficient dual-atom catalysts with well-defined coordination and electronic structures in energy conversion technologies.https://doi.org/10.1038/s41467-025-56066-8 |
| spellingShingle | Zhen Zhang Zhenyu Xing Xianglin Luo Chong Cheng Xikui Liu Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis Nature Communications |
| title | Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis |
| title_full | Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis |
| title_fullStr | Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis |
| title_full_unstemmed | Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis |
| title_short | Densely populated macrocyclic dicobalt sites in ladder polymers for low-overpotential oxygen reduction catalysis |
| title_sort | densely populated macrocyclic dicobalt sites in ladder polymers for low overpotential oxygen reduction catalysis |
| url | https://doi.org/10.1038/s41467-025-56066-8 |
| work_keys_str_mv | AT zhenzhang denselypopulatedmacrocyclicdicobaltsitesinladderpolymersforlowoverpotentialoxygenreductioncatalysis AT zhenyuxing denselypopulatedmacrocyclicdicobaltsitesinladderpolymersforlowoverpotentialoxygenreductioncatalysis AT xianglinluo denselypopulatedmacrocyclicdicobaltsitesinladderpolymersforlowoverpotentialoxygenreductioncatalysis AT chongcheng denselypopulatedmacrocyclicdicobaltsitesinladderpolymersforlowoverpotentialoxygenreductioncatalysis AT xikuiliu denselypopulatedmacrocyclicdicobaltsitesinladderpolymersforlowoverpotentialoxygenreductioncatalysis |