Phenothiazine-based copolymer with redox functional backbones for organic battery cathode materials

Liu, Y.; Niu, Zhihui; Dai, Gaole; Chen, Y.; Li, H.; Huang, Lv; Zhang, X.; Xu, Yang

doi:10.1016/j.mtener.2021.100812

“…The frontier molecular orbital populations of the neutral PVBPX and its oxidation Angewandte Chemie state reveal that only π-electrons participate in the redox reaction process and no bond rearrangement is observed, confirming the structural stability of PVBPX during redox reaction, which is consistent with the analysis of the aromaticity. [27] In addition, the energy gaps of oxidized PVBPX + and PVBPX 2 + are significantly lower compared to that of neutral PVBPX, which facilitates the interaction of PVBPX with anions during charging, promotes electron transfer, and reduces polarization during cycling. [28] Furthermore, the frontier molecular orbital energy levels of the coordinated PVBPX complexes (PVBPX-AlCl 4 À and PVBPX-2AlCl 4 À ) were also calculated (Figure S16 and S17).…”

Section: Methodsmentioning

confidence: 99%

Phenoxazine Polymer‐based p‐type Positive Electrode for Aluminum‐ion Batteries with Ultra‐long Cycle Life

Yang

¹

,

Huang

²

,

Meng

³

et al. 2023

View full text Add to dashboard Cite

Aluminum-ion batteries (AIBs) are a promising candidate for large-scale energy storage due to the abundant reserves, low cost, good safety, and high theoretical capacity of Al. However, AIBs with inorganic positive electrodes still suffer from sluggish kinetics and structural collapse upon cycling. Herein, we propose a novel p-type poly(vinylbenzyl-N-phenoxazine) (PVBPX) positive electrode for AIBs. The dual active sites enable PVBPX to deliver a high capacity of 133 mAh g À 1 at 0.2 A g À 1 . More impressively, the expanded π-conjugated construction, insolubility, and anionic redox chemistry without bond rearrangement of PVBPX for AIBs contribute to an amazing ultra-long lifetime of 50000 cycles. The charge storage mechanism is that the AlCl 4 À ions can reversibly coordinate/ dissociate with the N and O sites in PVBPX sequentially, which is evidenced by both experimental and theoretical results. These findings establish a foundation to advance organic AIBs for large-scale energy storage.

show abstract

“…The frontier molecular orbital populations of the neutral PVBPX and its oxidation Angewandte Chemie Forschungsartikel state reveal that only π-electrons participate in the redox reaction process and no bond rearrangement is observed, confirming the structural stability of PVBPX during redox reaction, which is consistent with the analysis of the aromaticity. [27] In addition, the energy gaps of oxidized PVBPX + and PVBPX 2 + are significantly lower compared to that of neutral PVBPX, which facilitates the interaction of PVBPX with anions during charging, promotes electron transfer, and reduces polarization during cycling. [28] Furthermore, the frontier molecular orbital energy levels of the coordinated PVBPX complexes (PVBPX-AlCl 4 À and PVBPX-2AlCl 4 À ) were also calculated (Figure S16 and S17).…”

Section: Forschungsartikelmentioning

confidence: 99%

Phenoxazine Polymer‐based p‐type Positive Electrode for Aluminum‐ion Batteries with Ultra‐long Cycle Life

Yang

¹

,

Huang

²

,

Meng

³

et al. 2023

Angewandte Chemie

0

View full text Add to dashboard Cite

Aluminum-ion batteries (AIBs) are a promising candidate for large-scale energy storage due to the abundant reserves, low cost, good safety, and high theoretical capacity of Al. However, AIBs with inorganic positive electrodes still suffer from sluggish kinetics and structural collapse upon cycling. Herein, we propose a novel p-type poly(vinylbenzyl-N-phenoxazine) (PVBPX) positive electrode for AIBs. The dual active sites enable PVBPX to deliver a high capacity of 133 mAh g À 1 at 0.2 A g À 1 . More impressively, the expanded π-conjugated construction, insolubility, and anionic redox chemistry without bond rearrangement of PVBPX for AIBs contribute to an amazing ultra-long lifetime of 50000 cycles. The charge storage mechanism is that the AlCl 4 À ions can reversibly coordinate/ dissociate with the N and O sites in PVBPX sequentially, which is evidenced by both experimental and theoretical results. These findings establish a foundation to advance organic AIBs for large-scale energy storage.

show abstract

“…[46] The recently reported phenothiazine-based cathode material displays an average redox voltage of 3.7 V (vs. Li + /Li), which is comparable to the conventional inorganic cathode materials. [47] In contrast to the n-type OEMs, the redox reactions of p-type OEMs involve the compensation process of counter anions, potentially showing faster kinetics of redox reactions. [48] However, most p-type electrodes with limited anionic doping degree show low discharge capacity and complex redox mechanism, which hinders the further research of p-type OEMs in portable metal-ion batteries.…”

Section:  Redox Reaction Types Of Oemsmentioning

confidence: 99%

Challenges and advances of organic electrode materials for sustainable secondary batteries

Shi

¹

,

Jiao

²

,

Yue

³

et al. 2022

View full text Add to dashboard Cite

Organic electrode materials (OEMs) emerge as one of the most promising candidates for the next-generation rechargeable batteries, mainly owing to their advantages of bountiful resources, high theoretical capacity, structural designability, and sustainability. However, OEMs usually suffer from poor electronic conductivity and unsatisfied stability in common organic electrolytes, ultimately leading to their deteriorating output capacity and inferior rate capability. Making clear of the issues from microscale to macroscale level is of great importance for the exploration of novel OEMs. Herein, the challenges and advanced strategies to boost the electrochemical performance of redox-active OEMs for sustainable secondary batteries are systematically summarized. Particularly, the characterization technologies and computational methods to elucidate the complex redox reaction mechanisms and confirm the organic radical intermediates of OEMs have been introduced. Moreover, the structural design of OEMs-based full cells and the outlook for OEMs are further presented. This review will shed light on the in-depth understanding and development of OEMs for sustainable secondary batteries. K E Y WO R D Sadvanced strategies, challenges, characterization techniques, organic electrode materials, redox reaction mechanism  INTRODUCTIONThe rising development of new energy electric vehicles, large-scale fixed energy storage, and the national smart grid has put forward high requirements on the mass energy Ruijuan Shi and Shilong Jiao contributed equally to this work.

show abstract

Phenothiazine-based copolymer with redox functional backbones for organic battery cathode materials

Cited by 15 publications

References 70 publications

Phenoxazine Polymer‐based p‐type Positive Electrode for Aluminum‐ion Batteries with Ultra‐long Cycle Life

Phenoxazine Polymer‐based p‐type Positive Electrode for Aluminum‐ion Batteries with Ultra‐long Cycle Life

Phenoxazine Polymer‐based p‐type Positive Electrode for Aluminum‐ion Batteries with Ultra‐long Cycle Life

Challenges and advances of organic electrode materials for sustainable secondary batteries

Contact Info

Product

Resources

About