Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities
It is important to tune the coordination configuration of dual-atom catalyst (DAC), especially in the first coordination sphere, to render high intrinsic catalytic activities for oxygen reduction/evolution reactions (ORR/OER). Herein, a type of atomically dispersed and boron-coordinated DAC structur...
| Main Authors: | , , , , , , , , , , , |
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| Format: | Journal Article |
| Language: | English |
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2024
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| Online Access: | https://hdl.handle.net/10356/174713 |
| _version_ | 1826128628199456768 |
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| author | Wang, Zhe Xu, Ruojie Ye, Qitong Jin, Xiaoyan Lu, Zhe Yang, Zhenbei Wang, Yong Yan, Tao Liu, Yipu Pan, Zhijuan Hwang, Seong-Ju Fan, Hong Jin |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Wang, Zhe Xu, Ruojie Ye, Qitong Jin, Xiaoyan Lu, Zhe Yang, Zhenbei Wang, Yong Yan, Tao Liu, Yipu Pan, Zhijuan Hwang, Seong-Ju Fan, Hong Jin |
| author_sort | Wang, Zhe |
| collection | NTU |
| description | It is important to tune the coordination configuration of dual-atom catalyst (DAC), especially in the first coordination sphere, to render high intrinsic catalytic activities for oxygen reduction/evolution reactions (ORR/OER). Herein, a type of atomically dispersed and boron-coordinated DAC structure, namely, FeN4B-NiN4B dual sites, is reported. In this structure, the incorporation of boron into the first coordination sphere of FeN4/NiN4 atomic sites regulates its geometry and electronic structure by forming “Fe-B-N” and “Ni-B-N” bridges. The FeN4B-NiN4B DAC exhibits much enhanced ORR and OER property compared to the FeN4-NiN4 counterparts. Density functional theory calculations reveal that the boron-induced charge transfer and asymmetric charge distributions of the central Fe/Ni atoms optimize the adsorption and desorption behavior of the ORR/OER intermediates and reduce the activation energy for the potential-determining step. Zinc-air batteries employing the FeN4B-NiN4B cathode exhibit a high maximum power density (236.9 mW cm−2) and stable cyclability up to 1100 h. The result illustrates the pivotal role of the first-coordination sphere of DACs in tuning the electrochemical energy conversion and storage activities. |
| first_indexed | 2024-10-01T07:28:03Z |
| format | Journal Article |
| id | ntu-10356/174713 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T07:28:03Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1747132024-04-08T15:35:18Z Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities Wang, Zhe Xu, Ruojie Ye, Qitong Jin, Xiaoyan Lu, Zhe Yang, Zhenbei Wang, Yong Yan, Tao Liu, Yipu Pan, Zhijuan Hwang, Seong-Ju Fan, Hong Jin School of Physical and Mathematical Sciences School of Materials Science and Engineering Physics Boron introduction Dual-atom catalysts It is important to tune the coordination configuration of dual-atom catalyst (DAC), especially in the first coordination sphere, to render high intrinsic catalytic activities for oxygen reduction/evolution reactions (ORR/OER). Herein, a type of atomically dispersed and boron-coordinated DAC structure, namely, FeN4B-NiN4B dual sites, is reported. In this structure, the incorporation of boron into the first coordination sphere of FeN4/NiN4 atomic sites regulates its geometry and electronic structure by forming “Fe-B-N” and “Ni-B-N” bridges. The FeN4B-NiN4B DAC exhibits much enhanced ORR and OER property compared to the FeN4-NiN4 counterparts. Density functional theory calculations reveal that the boron-induced charge transfer and asymmetric charge distributions of the central Fe/Ni atoms optimize the adsorption and desorption behavior of the ORR/OER intermediates and reduce the activation energy for the potential-determining step. Zinc-air batteries employing the FeN4B-NiN4B cathode exhibit a high maximum power density (236.9 mW cm−2) and stable cyclability up to 1100 h. The result illustrates the pivotal role of the first-coordination sphere of DACs in tuning the electrochemical energy conversion and storage activities. National Research Foundation (NRF) Submitted/Accepted version The authors thank Soochow University, China, for providing financial support (2111500622). This work was also supported by National Natural Science Foundation of China (No. 22005116, 22369003). The authors also acknowledge National Research Foundation-Competitive Research Programs (NRF-CRP22-2019-0007), and the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (RS-2023–00208355, NRF-2022M3H4A4086103). 2024-04-08T05:08:28Z 2024-04-08T05:08:28Z 2024 Journal Article Wang, Z., Xu, R., Ye, Q., Jin, X., Lu, Z., Yang, Z., Wang, Y., Yan, T., Liu, Y., Pan, Z., Hwang, S. & Fan, H. J. (2024). Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities. Advanced Functional Materials. https://dx.doi.org/10.1002/adfm.202315376 1616-301X https://hdl.handle.net/10356/174713 10.1002/adfm.202315376 2-s2.0-85187312143 en NRF-CRP22-2019-0007 Advanced Functional Materials © 2024 Wiley-VCH GmbH. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1002/adfm.202315376. application/pdf |
| spellingShingle | Physics Boron introduction Dual-atom catalysts Wang, Zhe Xu, Ruojie Ye, Qitong Jin, Xiaoyan Lu, Zhe Yang, Zhenbei Wang, Yong Yan, Tao Liu, Yipu Pan, Zhijuan Hwang, Seong-Ju Fan, Hong Jin Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities |
| title | Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities |
| title_full | Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities |
| title_fullStr | Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities |
| title_full_unstemmed | Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities |
| title_short | Tailoring first coordination sphere of dual-metal atom sites boosts oxygen reduction and evolution activities |
| title_sort | tailoring first coordination sphere of dual metal atom sites boosts oxygen reduction and evolution activities |
| topic | Physics Boron introduction Dual-atom catalysts |
| url | https://hdl.handle.net/10356/174713 |
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