Long‐lifespan Polyanionic Organic Cathodes for Highly Efficient Organic Sodium‐ion Batteries

Li, Di; Tang, Wu; Yong, Chen Yue; Tan, Zheng Hui; Wang, Chuan; Fan, Cong

doi:10.1002/cssc.202000131

Cited by 33 publications

(13 citation statements)

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“…Major issues that have hindered the utilization of organic molecules such as AQ in battery applications so far are the high solubility in polar organic battery electrolytes (i.e., ethylene carbonate (EC) and dimethyl carbonate (DMC)) and chemical degradation, resulting in poor cycle-life performance. ,,, On the other hand, departing from the concept of small molecules, the polyanionic AQ cathodes recently proposed are more stable but allow only for much smaller theoretical capacities. , Prior research showed that AQ pigment molecules are found to associate to form dimers, trimers, and other polyaggregates . Intermolecular dimerization decreases the available Na ion storage sites, resulting in a deviation from the ideal storage capacity of two electrons per molecule and hence adding to the chemical degradation issue.…”

Section: Introductionmentioning

confidence: 99%

“…11,12,32,33 On the other hand, departing from the concept of small molecules, the polyanionic AQ cathodes recently proposed are more stable but allow only for much smaller theoretical capacities. 34,35 Prior research showed that AQ pigment molecules are found to associate to form dimers, trimers, and other polyaggregates. 36 Intermolecular dimerization decreases the available Na ion storage sites, resulting in a deviation from the ideal storage capacity of two electrons per molecule and hence adding to the chemical degradation issue.…”

Section: Introductionmentioning

confidence: 99%

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Analysis of the Ordering Effects in Anthraquinone Thin Films and Its Potential Application for Sodium Ion Batteries

et al. 2021

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The ordering effects in anthraquinone (AQ) stacking forced by thin-film application and its influence on dimer solubility and current collector adhesion are investigated. The structural characteristics of AQ and its chemical environment are found to have a substantial influence on its electrochemical performance. Computational investigation for different charged states of AQ on a carbon substrate obtained via basin hopping global minimization provides important insights into the physicochemical thin-film properties. The results reveal the ideal stacking configurations of the individual AQ-carrier systems and show ordering effects in a periodic supercell environment. The latter reveals the transition from intermolecular hydrogen bonding toward the formation of salt bridges between the reduced AQ units and a stabilizing effect upon the dimerlike rearrangement, while the strong surface−molecular interactions in the thin-film geometries are found to be crucial for the formed dimers to remain electronically active. Both characteristics, the improved current collector adhesion and the stabilization due to dimerization, are mutual benefits of thin-film electrodes over powder-based systems. This hypothesis has been further investigated for its potential application in sodium ion batteries. Our results show that AQ thin-film electrodes exhibit significantly better specific capacities (233 vs 87 mAh g −1 in the first cycle), Coulombic efficiencies, and long-term cycling performance (80 vs 4 mAh g −1 after 100 cycles) over the AQ powder electrodes. By augmenting the experimental findings via computational investigations, we are able to suggest design strategies that may foster the performance of industrially desirable powder-based electrode materials.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Analysis of the Ordering Effects in Anthraquinone Thin Films and Its Potential Application for Sodium Ion Batteries

et al. 2021

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“…On the other hand, in our previous study, we found organic small-molecule cathodes with multiple strong ionic O–metal bonds (metal = Na/K) could show satisfactory insolubility in ether-based electrolytes. − And these organic metal salts can be regarded as polyanionic organic cathodes, because their organic anion bears a polyvalent negative state. However, it is remarkable that polyanionic organic anodes are seldom reported for KIBs .…”

Section: Introductionmentioning

confidence: 95%

Electrolyte Effect on a Polyanionic Organic Anode for Pure Organic K-Ion Batteries

Liu

Xiong

Tang

et al. 2021

ACS Appl. Mater. Interfaces

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Potassium naphthalene-1,4,5,8-tetracarboxylate (K4NTC, 117 mAh g–1) is a new organic anode for K-ion batteries, which possesses four strong K–O ionic bonds within a −4-valent naphthalene-1,4,5,8-tetracarboxylate skeleton (NTC4–). And thus, K4NTC is a polyanionic organic salt. Simultaneously, new insights are provided by comparing two typical electrolyte systems (carbonate and ether electrolytes) with KPF6 as the same solute. Finally, the pure organic K-ion batteries (OKIBs) are fabricated by using perylene-3,4,9,10-tetracarboxydianhydride (PTCDA) as the organic cathode and the reduced state (K6NTC) of K4NTC as the anode. And this OKIB can deliver a peak discharge capacity of 121 mAh g–1 anode and run over 1500 cycles in 0.5–3 V using ether electrolytes.

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“…[ 16 ] For this purpose, a wide catalog of materials are under research, such as conducting polymers, organosulfur compounds, organic radical compounds, carbonyl compounds (PTCDA and disodium rhodizonate). [ 18,80–82 ] These latter, carbonyl compounds, are the most studied family of organic electrodes in the last years, but they are still concerns that must be resolved. The main drawbacks of these systems are the dissolution of the cathode in the electrolyte that leads to rapid capacity fade, their low electronic conductivity that causes poor rate performance, and the increase of working potentials and tap density of the electrodes that would lead to high energy density cathodes.…”

Section: Sodium Ion Batteries: Retrospective and Advancesmentioning

confidence: 99%

Na‐Ion Batteries—Approaching Old and New Challenges

Goikolea

Palomares

Wang

et al. 2020

Advanced Energy Materials

351

190

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are proving to be an emergent technology with potentially very attractive properties. They are potentially low cost and environmentally friendly with reduced supply risk. However, the development of NIBs faces various challenges such as low gravimetric and volumetric energy densities and difficulty in achieving broader voltage windows. Although early studies in NIBs date back to the 1970s, just like Li-ion battery (LIB) research, the commercialization of the former systems in 1991 by the team formed by Sony and Asahi Kasei marked a milestone not only in the field of energy storage technology but also in the evolution of the modern society. This technological breakthrough had been possible thanks to several preceding contributions, particularly the works by M. S Whittingham, [1] J. Goodenough, [2,3] and A. Yoshino [4] on the discovery of Li-ion intercalation materials (Nobel Laureates in Chemistry 2019). This important historical event polarized material science research toward Li-ion technology and slowed down considerably the advances in the field of sodium. However, at the end of the 2000s, mainly driven by the concerns about future lithium supply and the uneven worldwide distribution of its reserves and resources, the research on Na-ion reemerged and so did the number of articles published (Figure 1). The intercalation chemistry of both metal ions is very alike, and thus, the materials tested for NIBs could be similar to those used in Li-ion systems. Both systems share the same working principle, and therefore, in terms of manufacturing, the industry producing LIBs can be easily tuned towards NIB fabrication, which is an important asset to invest in and support this technology. NIBs started to reach the market in the early 2010s, about two decades after their Li counterparts. Nevertheless, the progress has been relatively fast due to the straightforward LIB equipment and facility transfer just mentioned. In the search of high performance, low cost, abundance, low environmental impact, long-term cyclability and safety, layered metal oxides, polyanionic compounds and Prussian blue analogues (PBAs) are among the most studied families of Na-ion cathode materials. On the anode side, metallic sodium exhibits the same operation and safety problems as lithium, and therefore, it cannot be considered an option in conventional NIBs. Thus, in this scenario, most of the research has been dominated by the use of disordered carbons, mainly hard carbons (HCs). Other prospective anodes

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Long‐lifespan Polyanionic Organic Cathodes for Highly Efficient Organic Sodium‐ion Batteries

Cited by 33 publications

References 42 publications

Analysis of the Ordering Effects in Anthraquinone Thin Films and Its Potential Application for Sodium Ion Batteries

Analysis of the Ordering Effects in Anthraquinone Thin Films and Its Potential Application for Sodium Ion Batteries

Electrolyte Effect on a Polyanionic Organic Anode for Pure Organic K-Ion Batteries

Na‐Ion Batteries—Approaching Old and New Challenges

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