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250807s2025 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202509022
|2 doi
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|a pubmed25n1602.xml
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|a (DE-627)NLM390778508
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|a (NLM)40772390
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|a DE-627
|b ger
|c DE-627
|e rakwb
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| 041 |
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|a eng
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| 100 |
1 |
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|a Han, Kang
|e verfasserin
|4 aut
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| 245 |
1 |
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|a Unlocking the Ligand-Dominated Redox Activity in π-d Conjugated Coordination Polymers for High-Capacity and Stable Potassium Storage
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|c 2025
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
|b c
|2 rdamedia
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| 338 |
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|a ƒa Online-Ressource
|b cr
|2 rdacarrier
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|a Date Revised 17.10.2025
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2025 Wiley‐VCH GmbH.
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|a Potassium-ion batteries (KIBs) offer a cost-effective, resource-abundant alternative to lithium-ion systems, yet the development of high-performance anodes with adequate capacity, stability, and rate capability remains a major challenge. Here, an electronic structure engineering strategy is introduced via d-orbital configuration optimization in a novel class of π-d conjugated coordination polymers (TM-BTA, TM = Ni, Co, Mn). Orbital-level and charge density analyses reveal that the metal center's electronic configuration governs metal-ligand interaction strength, thereby modulating charge delocalization and ligand redox behavior. Among the series, Ni2⁺ exhibits the strongest π-d conjugation with nitrogen donor atoms, stabilizing C═N bonds and enabling highly reversible C═N/C─N transformations as the dominant redox process. This optimized coordination lowers the K⁺ adsorption energy barrier by 44% compared to Co2⁺ and Mn2⁺, markedly improving kinetics. As a result, Ni-BTA delivers a high reversible capacity of 452 mAh g-1 with 99.2% retention over 500 cycles at 100 mA g-1, and maintains 292 mAh g-1 after 4,000 cycles at 1,000 mA g-1. In situ spectroscopy and DFT calculations reveal a ligand-centered three-electron redox mechanism, where nitrogen heterocycles dominate K⁺ storage and electrochemically inert Ni centers maintain structural integrity. This work establishes a general design principle for KIB anodes via d-orbital engineering in coordination polymers
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4 |
|a Journal Article
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|a conductive coordination polymers
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| 650 |
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4 |
|a ligand‐dominated storage
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| 650 |
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|a potassium‐ion batteries
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| 650 |
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4 |
|a π–d conjugation
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| 700 |
1 |
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|a Zhong, Zhenhang
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Zhang, Hao
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Zhang, Guangwan
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Wang, Xuanpeng
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Liu, Fang
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Niu, Chaojiang
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Mai, Liqiang
|e verfasserin
|4 aut
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| 773 |
0 |
8 |
|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 37(2025), 41 vom: 06. Okt., Seite e09022
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnas
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| 773 |
1 |
8 |
|g volume:37
|g year:2025
|g number:41
|g day:06
|g month:10
|g pages:e09022
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| 856 |
4 |
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|u http://dx.doi.org/10.1002/adma.202509022
|3 Volltext
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|a AR
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|d 37
|j 2025
|e 41
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|c 10
|h e09022
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