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Abstract Developing low‐voltage carboxylate anode materials is critical for achieving low‐cost, high‐performance, and sustainable Na‐ion batteries (NIBs). However, the structure design rationale and structure‐performance correlation for organic carboxylates in NIBs remains elusive. Herein, the spatial effect on the performance of carboxylate anode materials is studied by introducing heteroatoms in the conjugation structure and manipulating the positions of carboxylate groups in the aromatic rings. Planar and twisted organic carboxylates are designed and synthesized to gain insight into the impact of geometric structures to the electrochemical performance of carboxylate anodes in NIBs. Among the carboxylates, disodium 2,2’‐bipyridine‐5,5’‐dicarboxylate (2255‐Na) with a planar structure outperforms the others in terms of highest specific capacity (210 mAh g−1), longest cycle life (2000 cycles), and best rate capability (up to 5 A g−1). The cyclic stability and redox mechanism of 2255‐Na in NIBs are exploited by various characterization techniques. Moreover, high‐temperature (up to 100 °C) and all‐organic batteries based on a 2255‐Na anode, a polyaniline (PANI) cathode, and an ether‐based electrolyte are achieved and exhibited exceptional electrochemical performance. Therefore, this work demonstrates that designing organic carboxylates with extended planar conjugation structures is an effective strategy to achieve high‐performance and sustainable NIBs.
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Stable Cycling of Sodium All‐Solid‐State Batteries with High‐Capacity Cathode Presodiation
Abstract Sodium all‐solid‐state batteries (NaSSBs) with an alloy‐type anode (e.g., Sn and Sb) offer superior capacity and energy density compared to hard carbon anode. However, the irreversible loss of Na+at the alloy anode during the initial cycle results in diminished capacity and stability, impairing full‐cell performance. This study presents an easy‐to‐implement cathode presodiation strategy by employing a Na‐rich material to address these challenges. Leveraging the high theoretical capacity and suitable voltage window, Na2S is chosen as the Na donor, which is activated by creating a mixed electron‐ion conducting network, delivering a high capacity of 511.7 mAh g−1. By adding a small amount (i.e., 3 wt.%) of Na2S to the cathode composite, a NaCrO2|| Sn full cell demonstrated capacity improvement from 90.8 to 118.2 mAh g−1(based on cathode mass). The capacity‐balanced full cell can thus cycle to more than 300 times with >90% capacity retention. This work provides a practical solution to enhance the full‐cell performance and advance the transformation from half‐cell to full‐cell applications of NaSSBs.
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- Award ID(s):
- 2134764
- PAR ID:
- 10633265
- Publisher / Repository:
- Wiley
- Date Published:
- Journal Name:
- Advanced Energy Materials
- Volume:
- 15
- Issue:
- 23
- ISSN:
- 1614-6832
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
-
Accepted Manuscript
- Journal Article:
- https://doi.org/10.1002/aenm.202405678
