Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells
Developing low-cost and highly efficient oxygen reduction reaction (ORR) catalysts with excellent methanol tolerance is crucial for the commercialization of direct methanol fuel cells (DMFCs). In this work, we construct single Fe atoms anchored on N,S-codoped graphene (Fe1/NSG), where the S atom in...
| Main Authors: | , , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/168720 |
| _version_ | 1811694813329752064 |
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| author | Zhang, Jincheng Wang, Qilun Qiu, Chunyu Gan, Liyong Ding, Jie Li, Fuhua Wang, Tian Liu, Yuhang Wang, Yucheng Tao, Huabing Hung, Sung-Fu Yang, Hongbin Liu, Bin |
| author2 | School of Chemical and Biomedical Engineering |
| author_facet | School of Chemical and Biomedical Engineering Zhang, Jincheng Wang, Qilun Qiu, Chunyu Gan, Liyong Ding, Jie Li, Fuhua Wang, Tian Liu, Yuhang Wang, Yucheng Tao, Huabing Hung, Sung-Fu Yang, Hongbin Liu, Bin |
| author_sort | Zhang, Jincheng |
| collection | NTU |
| description | Developing low-cost and highly efficient oxygen reduction reaction (ORR) catalysts with excellent methanol tolerance is crucial for the commercialization of direct methanol fuel cells (DMFCs). In this work, we construct single Fe atoms anchored on N,S-codoped graphene (Fe1/NSG), where the S atom in the second coordination sphere of the Fe catalytic center regulates the electronic structure of the Fe center and stabilizes the ∗OOH intermediate in the ORR. Thanks to the optimal adsorption of O2 intermediates and the isolated Fe active sites, as probed by in situ infrared spectroscopy and density functional theory, Fe1/NSG exhibits high ORR activity with a half-wave potential of 0.90 V vs. reversible hydrogen electrode (RHE) and a super anti-methanol capability. The DMFC with the Fe1/NSG cathode is able to deliver a peak power density as high as 198 mW cm−2, outperforming the reported DMFCs assembled using non-precious-metal-based cathode catalysts. |
| first_indexed | 2024-10-01T07:13:32Z |
| format | Journal Article |
| id | ntu-10356/168720 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T07:13:32Z |
| publishDate | 2023 |
| record_format | dspace |
| spelling | ntu-10356/1687202023-12-29T06:51:52Z Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells Zhang, Jincheng Wang, Qilun Qiu, Chunyu Gan, Liyong Ding, Jie Li, Fuhua Wang, Tian Liu, Yuhang Wang, Yucheng Tao, Huabing Hung, Sung-Fu Yang, Hongbin Liu, Bin School of Chemical and Biomedical Engineering Engineering::Chemical engineering Zinc Air Batteries Electrocatalysts Developing low-cost and highly efficient oxygen reduction reaction (ORR) catalysts with excellent methanol tolerance is crucial for the commercialization of direct methanol fuel cells (DMFCs). In this work, we construct single Fe atoms anchored on N,S-codoped graphene (Fe1/NSG), where the S atom in the second coordination sphere of the Fe catalytic center regulates the electronic structure of the Fe center and stabilizes the ∗OOH intermediate in the ORR. Thanks to the optimal adsorption of O2 intermediates and the isolated Fe active sites, as probed by in situ infrared spectroscopy and density functional theory, Fe1/NSG exhibits high ORR activity with a half-wave potential of 0.90 V vs. reversible hydrogen electrode (RHE) and a super anti-methanol capability. The DMFC with the Fe1/NSG cathode is able to deliver a peak power density as high as 198 mW cm−2, outperforming the reported DMFCs assembled using non-precious-metal-based cathode catalysts. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) Published version This work was supported by funds from the National Natural Science Foundation of China (no. 22075195), the Singapore Ministry of Education Academic Research Fund (AcRF) Tier 1: RG4/20 and RG2/21 and Tier 2: MOET2EP10120- 0002, and the Agency for Science, Technology and Research: AME IRG A20E5c0080. 2023-06-16T05:18:14Z 2023-06-16T05:18:14Z 2023 Journal Article Zhang, J., Wang, Q., Qiu, C., Gan, L., Ding, J., Li, F., Wang, T., Liu, Y., Wang, Y., Tao, H., Hung, S., Yang, H. & Liu, B. (2023). Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells. Cell Reports Physical Science, 4(3), 101330-. https://dx.doi.org/10.1016/j.xcrp.2023.101330 2666-3864 https://hdl.handle.net/10356/168720 10.1016/j.xcrp.2023.101330 2-s2.0-85150063444 3 4 101330 en RG4/20 RG2/21 MOET2EP10120- 0002 AME IRG A20E5c0080 Cell Reports Physical Science © 2023 The Author(s). This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/). application/pdf |
| spellingShingle | Engineering::Chemical engineering Zinc Air Batteries Electrocatalysts Zhang, Jincheng Wang, Qilun Qiu, Chunyu Gan, Liyong Ding, Jie Li, Fuhua Wang, Tian Liu, Yuhang Wang, Yucheng Tao, Huabing Hung, Sung-Fu Yang, Hongbin Liu, Bin Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells |
| title | Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells |
| title_full | Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells |
| title_fullStr | Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells |
| title_full_unstemmed | Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells |
| title_short | Boosting activity of Fe-N4 sites in single-Fe-atom catalysts via S in the second coordination sphere for direct methanol fuel cells |
| title_sort | boosting activity of fe n4 sites in single fe atom catalysts via s in the second coordination sphere for direct methanol fuel cells |
| topic | Engineering::Chemical engineering Zinc Air Batteries Electrocatalysts |
| url | https://hdl.handle.net/10356/168720 |
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