A nitroaromatic cathode with an ultrahigh energy density based on six-electron reaction per nitro group for lithium batteries

Chen, Zifeng; Su, Hai; Sun, Pengfei; Bai, Panxing; Yang, Jixing; Li, Mengjie; Deng, Yunfeng; Liu, Yang; Geng, Yanhou; Xu, Yunhua

doi:10.1073/pnas.2116775119

Cited by 25 publications

(37 citation statements)

References 60 publications

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“…Profiting from strong electronegativity, nitro groups deliver powerful coupling capability and susceptibility to form metal–ligand complexes with electrolyte ions, affording robust redox nature [12] . Meanwhile, with the ability to accept two electrons per nitro group, it can trigger multielectron redox for efficient charge storage [13] .…”

Section: Introductionmentioning

confidence: 99%

Anionic Co‐insertion Charge Storage in Dinitrobenzene Cathodes for High‐Performance Aqueous Zinc–Organic Batteries

et al. 2022

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Highly active and stable cathodes are critical for aqueous Zn–organic batteries with high capacity, fast redox kinetics, and long life. We herein report para‐, meta‐, and ortho‐dinitrobenzene (p‐, m‐, and o‐DB) containing two successive two‐electron processes, as cathode materials to boost the battery performance. Theoretical and experimental studies reveal that nitro constitutional isomerism is key to zincophilic activity and redox kinetics. p‐DB hosted in carbon nanoflower harvests a high capacity of 402 mAh g−1 and a superior stability up to 25 000 cycles at 5 A g−1, giving a Zn–organic battery with a high energy density of 230 Wh kg−1. An anionic co‐insertion charge storage mechanism is proposed, entailing a two‐step (de)coordination of Zn(CF3SO3)+ with nitro oxygen. Besides, dinitrobenzene can be electrochemically optimized by side group regulation via implanting electron‐withdrawing motifs. This work opens a new window to design multielectron nitroaromatics for Zn–organic batteries.

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Section: Introductionmentioning

confidence: 99%

Anionic Co‐insertion Charge Storage in Dinitrobenzene Cathodes for High‐Performance Aqueous Zinc–Organic Batteries

et al. 2022

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“…It is well-known that the chemical structures of cathode materials as well as electrolytes have a great influence on the performance of a battery. Thus, in this research, besides new cathode materials, we also used a more complicated electrolyte for this new nitro compound compared to the reported electrolytes for other nitro compounds. , Additionally, different values of CVs and different scanning rates were also optimized in order to obtain the voltage platform. Furthermore, at 1 A g –1 , the capacity could be maintained at 180 mAh g –1 after 1100 cycles (Figure d).…”

Section: Resultsmentioning

confidence: 99%

“…Even so, this result clearly suggests that attaching nitro groups onto aromatic rings is an efficient method to improve the capacity of LIBs. More recently, Xu et al 43 reported that a nitroaromatic small molecule (1,5-dinitronaphthalene, 1,5-DNN) as a cathode compound in lithium primary batteries could give an ultrahigh specific capacity of 1338 mAh g −1 and an energy density of 3273 Wh kg −1 , which surpass those of all existing organic cathodes. They also found that a nitro group could perform a six-electron reaction, significantly increasing the specific capacity and energy density compared with other organic cathodes.…”

Section: Introductionmentioning

confidence: 99%

A Nitro-Rich Small-Molecule-Based Organic Cathode Material for Effective Rechargeable Lithium Batteries

Shi

Lin

Kang

et al. 2022

ACS Appl. Mater. Interfaces

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Organic cathode materials have attracted extensive research interest for rechargeable lithium-ion batteries (LIBs) because of their diverse structures and tunable properties. However, the preparation of organic cathode materials with high capacities, long cycling life, and high energy densities still remains a big challenge. To address these issues, we designed and synthesized a novel multinitro-decorated organic small molecule, N 4,N 4′′-bis(2,4-dinitrophenyl)-5′-(4-((2,4-dinitrophenyl)amino)phenyl)-[1,1′:3′,1′′-terphenyl]-4,4′′-diamine (TAPB-6NO2), where the unique electronic character of nitro group should enable TAPB-6NO2 to be a promising cathode candidate for LIBs. We found that the introduction of multiple nitro groups could efficiently reduce the solubility of TAPB-6NO2 in organic electrolytes, resulting in a high specific capacity of around 180 mAh g–1 and stable cycling with a capacity retention of 91% after 1100 cycles at 1000 mA g–1. This work suggests that attaching multiple nitro groups on a small molecule is an effective approach to construct high-performance organic cathode materials for stable and sustainable rechargeable LIBs.

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“…in organic electrode materials can only experience singleelectron reaction per active group while the Zn 2+ ions carry two positive charges. 88 Thus, the coordination reaction between Zn 2+ and the organic electrode materials take place in adjacent electrochemical active groups within one molecule 58,[69][70][71]75 or from adjacent molecules. 67,68,78 In either case, the utilization rate of active groups is limited due to the restrictions on their spatial location.…”

Section: The Impact Of Proton Storage On Capacitymentioning

confidence: 99%

Proton storage chemistry in aqueous zinc‐organic batteries: A review

Deng

Sarpong

Zhang

et al. 2022

InfoMat

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Benefiting from the advantageous features of structural diversity and resource renewability, organic electroactive compounds are considered as attractive cathode materials for aqueous Zn-ion batteries (ZIBs). In this review, we discuss the recent developments of organic electrode materials for aqueous ZIBs. Although the proton (H + ) storage chemistry in aqueous Zn-organic batteries has triggered an overwhelming literature surge in recent years, this topic remains controversial. Therefore, our review focuses on this significant issue and summarizes the reported electrochemical mechanisms, including pure Zn 2+ intercalation, pure H + storage, and H + /Zn 2+ co-storage. Moreover, the impact of H + storage on the electrochemical performance of aqueous ZIBs is discussed systematically. Given the significance of H + storage, we also highlight the relevant characterization methods employed. Finally, perspectives and directions on further understanding the charge storage mechanisms of organic materials are outlined. We hope that this review will stimulate more attention on the H + storage chemistry of organic electrode materials to advance our understanding and further its application.

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A nitroaromatic cathode with an ultrahigh energy density based on six-electron reaction per nitro group for lithium batteries

Cited by 25 publications

References 60 publications

Anionic Co‐insertion Charge Storage in Dinitrobenzene Cathodes for High‐Performance Aqueous Zinc–Organic Batteries

Anionic Co‐insertion Charge Storage in Dinitrobenzene Cathodes for High‐Performance Aqueous Zinc–Organic Batteries

A Nitro-Rich Small-Molecule-Based Organic Cathode Material for Effective Rechargeable Lithium Batteries

Proton storage chemistry in aqueous zinc‐organic batteries: A review

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