Long‐Life Aqueous Organic Redox Flow Batteries Enabled by Amidoxime‐Functionalized Ion‐Selective Polymer Membranes

Ye, Chunchun; Tan, Rui; Wang, Anqi; Chen, Jie; Comesaña-Gándara, Bibiana; Breakwell, Charlotte; Álvarez-Fernández, Alberto; Fan, Zhiyu; Weng, Jiaqi; Bezzu, Grazia; Guldin, Stefan; Brandon, Nigel P.; Kucernak, Anthony; Jelfs, Kim E.; McKeown, Neil B.; Song, Qilei

doi:10.1002/anie.202207580

Cited by 38 publications

(39 citation statements)

References 41 publications

(1 reference statement)

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“… [5] In addition, modification of the nitrile groups of PIM‐DBMP to amidoxime (AO) substituents, [20] to give PIM‐DBMP‐AO, via reaction with hydroxylamine (Scheme 2), provided solubility in the polar aprotic solvent N ‐methyl‐2‐pyrrolidone (NMP). It was recently reported that PIM‐DBMP‐AO shows promise as an ionic transport membrane for redox flow batteries [21] …”

Section: Resultsmentioning

confidence: 99%

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Dibenzomethanopentacene‐Based Polymers of Intrinsic Microporosity for Use in Gas‐Separation Membranes

et al. 2023

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Dibenzomethanopentacene (DBMP) is shown to be a useful structural component for making Polymers of Intrinsic Microporosity (PIMs) with promise for making efficient membranes for gas separations. DBMP-based monomers for PIMs are readily prepared using a Diels-Alder reaction between 2,3-dimethoxyanthracene and norbornadiene as the key synthetic step. Compared to date for the archetypal PIM-1, the incorporation of DBMP simultaneously enhances both gas permeability and the ideal selectivity for one gas over another. Hence, both ideal and mixed gas permeability data for DBMP-rich co-polymers and an amidoxime modified PIM are close to the current Robeson upper bounds, which define the state-of-the-art for the trade-off between permeability and selectivity, for several important gas pairs. Furthermore, long-term studies (over � 3 years) reveal that the reduction in gas permeabilities on ageing is less for DBMP-containing PIMs relative to that for other high performing PIMs, which is an attractive property for the fabrication of membranes for efficient gas separations.

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Section: Resultsmentioning

confidence: 99%

“…It was recently reported that PIM-DBMP-AO shows promise as an ionic transport membrane for redox flow batteries. [21] Details of the physical properties of each polymer are provided in Table 1. The copolymer PIM-DBMP 0.75 was only soluble in quinoline.…”

Section: Resultsmentioning

confidence: 99%

Dibenzomethanopentacene‐Based Polymers of Intrinsic Microporosity for Use in Gas‐Separation Membranes

et al. 2023

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“…Designing ion-selective membranes with ordered ion transport channels has attracted significant interests in recent years 9 . Typical strategies include synthetic polymers with precise chain lengths and chain microstructures 10 , metal-organic framework 11 and covalent-organic frameworks with ordered ion channels 12 , or high-free-volume polymers with intrinsic micropores 13 – 16 . These synthetic membranes with subnanometer-sized channels facilitate vehicular transport and enhance ionic conductivity, however, the membrane selectivity can be compromised in concentrated electrolyte solutions due to weakened Donnan exclusion 17 .…”

Section: Introductionmentioning

confidence: 99%

Metal-coordinated polybenzimidazole membranes with preferential K+ transport

Liao

et al. 2023

Nat Commun

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Membranes with fast and selective ion transport are essential for separations and electrochemical energy conversion and storage devices. Metal-coordinated polymers are promising for fabricating ion-conducting membranes with molecular channels, however, the structures and ion transport channels remain poorly understood. Here, we reported mechanistic insights into the structures of metal-ion coordinated polybenzimidazole membranes and the preferential K+ transport. Molecular dynamics simulations suggested that coordination between metal ions and polybenzimidazole expanded the free volume, forming subnanometre molecular channels. The combined physical confinement in nanosized channels and electrostatic interactions of membranes resulted in a high K+ transference number up to 0.9 even in concentrated salt and alkaline solutions. The zinc-coordinated polybenzimidazole membrane enabled fast transport of charge carriers as well as suppressed water migration in an alkaline zinc-iron flow battery, enabling the battery to operate stably for over 340 hours. This study provided an alternative strategy to regulate the ion transport properties of polymer membranes by tuning polymer chain architectures via metal ion coordination.

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“…Polymers of intrinsic microporosity (PIMs) are solution-processable microporous materials with subnanometer channels generated from the inefficient packing of the rigid, contorted polymer chains. , PIMs have shown great promise as next-generation membrane materials for molecular separations, − batteries, − and fuel cells . We anticipate that if incorporated with redox-active structural units, PIMs with fast ion-transport channels could be used as high-performance electrode materials in electrochemical devices.…”

Section: Introductionmentioning

confidence: 99%

Solution-Processable Redox-Active Polymers of Intrinsic Microporosity for Electrochemical Energy Storage

et al. 2022

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Redox-active organic materials have emerged as promising alternatives to conventional inorganic electrode materials in electrochemical devices for energy storage. However, the deployment of redox-active organic materials in practical lithium-ion battery devices is hindered by their undesired solubility in electrolyte solvents, sluggish charge transfer and mass transport, as well as processing complexity. Here, we report a new molecular engineering approach to prepare redox-active polymers of intrinsic microporosity (PIMs) that possess an open network of subnanometer pores and abundant accessible carbonyl-based redox sites for fast lithium-ion transport and storage. Redox-active PIMs can be solution-processed into thin films and polymer− carbon composites with a homogeneously dispersed microstructure while remaining insoluble in electrolyte solvents. Solutionprocessed redox-active PIM electrodes demonstrate improved cycling performance in lithium-ion batteries with no apparent capacity decay. Redox-active PIMs with combined properties of intrinsic microporosity, reversible redox activity, and solution processability may have broad utility in a variety of electrochemical devices for energy storage, sensors, and electronic applications.

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Long‐Life Aqueous Organic Redox Flow Batteries Enabled by Amidoxime‐Functionalized Ion‐Selective Polymer Membranes

Cited by 38 publications

References 41 publications

Dibenzomethanopentacene‐Based Polymers of Intrinsic Microporosity for Use in Gas‐Separation Membranes

Dibenzomethanopentacene‐Based Polymers of Intrinsic Microporosity for Use in Gas‐Separation Membranes

Metal-coordinated polybenzimidazole membranes with preferential K+ transport

Solution-Processable Redox-Active Polymers of Intrinsic Microporosity for Electrochemical Energy Storage

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