Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery
Prussian blue analogs (PBAs) are potential contestants for aqueous Mg-ion batteries (AMIBs) on account of their high discharge voltage and three-dimensional open frameworks. However, the low capacity arising from single reaction site severely restricts PBAs' practical applications in high-energ...
| Main Authors: | , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/179657 |
| _version_ | 1826121667648159744 |
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| author | Ling, Ying He, Bing Han, Lijie Gong, Wenbin Chang, Chaofeng Zhang, Qichong |
| author2 | School of Electrical and Electronic Engineering |
| author_facet | School of Electrical and Electronic Engineering Ling, Ying He, Bing Han, Lijie Gong, Wenbin Chang, Chaofeng Zhang, Qichong |
| author_sort | Ling, Ying |
| collection | NTU |
| description | Prussian blue analogs (PBAs) are potential contestants for aqueous Mg-ion batteries (AMIBs) on account of their high discharge voltage and three-dimensional open frameworks. However, the low capacity arising from single reaction site severely restricts PBAs' practical applications in high-energy-density AMIBs. Here, an organic acid co-coordination combined with etching method is reported to fabricate defect-rich potassium-free copper hexacyanoferrate with structural water on carbon nanotube fiber (D-CuHCF@CNTF). Benefiting from the high-valence-state reactive sites, arrayed structure and defect effect, the well-designed D-CuHCF@CNTF exhibits an extraordinary reversible capacity of 146.6 mAh g−1 with two-electron reaction, nearly close to its theoretical capacity. It is interesting to unlock the reaction mechanism of the Fe2+/Fe3+ and Cu+/Cu2+ redox couples via x-ray photoelectron spectroscopy. Furthermore, density functional theory calculations reveal that Fe and Cu in potassium-free D-CuHCF participate in charge transfer during the Mg2+ insertion/extraction process. As a proof-of-concept demonstration, a rocking-chair fiber-shaped AMIBs was constructed via coupling with the NaTi2(PO4)3/CNTF anode, achieving high energy density and impressive mechanical flexibility. This work provides new possibilities to develop potassium-free PBAs with dual-active sites as high-capacity cathodes for wearable AMIBs. |
| first_indexed | 2024-10-01T05:35:56Z |
| format | Journal Article |
| id | ntu-10356/179657 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:35:56Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1796572024-08-16T15:45:25Z Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery Ling, Ying He, Bing Han, Lijie Gong, Wenbin Chang, Chaofeng Zhang, Qichong School of Electrical and Electronic Engineering Engineering Prussian blue analogs Two-electron reaction Prussian blue analogs (PBAs) are potential contestants for aqueous Mg-ion batteries (AMIBs) on account of their high discharge voltage and three-dimensional open frameworks. However, the low capacity arising from single reaction site severely restricts PBAs' practical applications in high-energy-density AMIBs. Here, an organic acid co-coordination combined with etching method is reported to fabricate defect-rich potassium-free copper hexacyanoferrate with structural water on carbon nanotube fiber (D-CuHCF@CNTF). Benefiting from the high-valence-state reactive sites, arrayed structure and defect effect, the well-designed D-CuHCF@CNTF exhibits an extraordinary reversible capacity of 146.6 mAh g−1 with two-electron reaction, nearly close to its theoretical capacity. It is interesting to unlock the reaction mechanism of the Fe2+/Fe3+ and Cu+/Cu2+ redox couples via x-ray photoelectron spectroscopy. Furthermore, density functional theory calculations reveal that Fe and Cu in potassium-free D-CuHCF participate in charge transfer during the Mg2+ insertion/extraction process. As a proof-of-concept demonstration, a rocking-chair fiber-shaped AMIBs was constructed via coupling with the NaTi2(PO4)3/CNTF anode, achieving high energy density and impressive mechanical flexibility. This work provides new possibilities to develop potassium-free PBAs with dual-active sites as high-capacity cathodes for wearable AMIBs. Published version This work was supported by the National Key R&D Program of China (2022YFA1203304), the Natural Science Foundation of Jiangsu Province (BK20220288), Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences (Start-up grant E1552102). 2024-08-14T06:31:48Z 2024-08-14T06:31:48Z 2024 Journal Article Ling, Y., He, B., Han, L., Gong, W., Chang, C. & Zhang, Q. (2024). Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery. InfoMat, 6(6). https://dx.doi.org/10.1002/inf2.12549 2567-3165 https://hdl.handle.net/10356/179657 10.1002/inf2.12549 2-s2.0-85191183421 6 6 en InfoMat © 2024 The Authors. InfoMat published by UESTC and John Wiley & Sons Australia, Ltd. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited. application/pdf |
| spellingShingle | Engineering Prussian blue analogs Two-electron reaction Ling, Ying He, Bing Han, Lijie Gong, Wenbin Chang, Chaofeng Zhang, Qichong Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery |
| title | Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery |
| title_full | Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery |
| title_fullStr | Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery |
| title_full_unstemmed | Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery |
| title_short | Two-electron redox chemistry enables potassium-free copper hexacyanoferrate as high-capacity cathode for aqueous Mg-ion battery |
| title_sort | two electron redox chemistry enables potassium free copper hexacyanoferrate as high capacity cathode for aqueous mg ion battery |
| topic | Engineering Prussian blue analogs Two-electron reaction |
| url | https://hdl.handle.net/10356/179657 |
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