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2. Polymers of intrinsic microporosity for aqueous organic redox flow batteries

Author

Ye, Chunchun, Mckeown, Neil, and Ferrari, Maria-Chiara

Subjects
Polymers of Intrinsic Microporosity, Ion Conductive Membranes, Aqueous Organic Redox Flow Batteries
Abstract

Redox flow batteries (RFBs) based on aqueous organic electrolytes are promising technologies for large-scale, safe and cost-effective electrical energy storage. The membrane separator is the key component in a RFB system to keep redox-active species separate in two half cells while allow free transport of charge-balancing ions. Delivering fast and selective ion transport is critical for battery performance yet remains a challenge for current RFB separators, owing to the difficulty in generating membranes with well-defined sub-nanometre channels to serve as efficient molecular sieves. In this thesis, a new family of ion-sieving membranes, based on Polymers of Intrinsic Microporosity (PIMs) with different backbones and integrating varied ion-conductive groups, are developed and function as efficient and stable separators in aqueous organic RFBs. PIMs are platform materials with distinct combination of properties including high microporosity, exceptional chain rigidity and good solution processibility. A range of dibenzodioxin-based PIMs with varied spirocyclic and bridged bicyclic structural units are synthesised and provide a versatile post-functionalisation to introduce ionisable amidoxime groups. These membranes demonstrate the feasibility of PIM-based membranes serving as ion-conductive and low-resistant separators in alkaline aqueous RFB systems. Further, negative-charged sulfonate groups are introduced into spirobifluorene-based PIMs which exhibit exceptional efficiency and stability for battery operation at near neutral aqueous electrolytes, outperforming identical RFB cells that use commercial benchmark Nafion® membranes. PIMs containing Tröger's base building blocks enable the introduction of quaternary ammonium groups together with simultaneous crosslinking network, or zwitterionic groups on amine sites. The combination of polymer rigidity, high microporosity and ion-conductive functionalities of PIMs facilitates the formation of well-confined and sub-nanometre pathway, allowing fast transport of charge-balancing ions whilst unprecedented blocking redox-active species through membranes, fulfilling the function as efficient RFB separators hence achieving impressive performance in RFBs. These proof-of-concept demos using functionalised PIM membranes as efficient molecular sieves can guide the development of new generation membrane separators for a range of clean energy technology applications.

Published
2021
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5. Rapid and Precise Molecular Nanofiltration Using Ultra‐Thin‐Film Membranes Derived from 6,6′‐Dihydroxy‐2,2′‐biphenyldiamine.

Author

Chen, Youcai, Shi, Wenxiong, Li, Shao‐Lu, Wang, Mengfan, Wang, Jian, Hao, Shuang, Gong, Genghao, Ye, Chunchun, McKeown, Neil B., and Hu, Yunxia

Subjects
POSITRON annihilation, POLYMERIC membranes, SEPARATION (Technology), MOLECULAR weights, INDUSTRIAL capacity
Abstract

A key challenge in efficient molecular separation is fabricating large‐scale, highly selective polymeric membranes with precise pore control at the molecular scale. Herein, a new contorted monomer 6,6′‐dihydroxy‐2,2′‐biphenyldiamine (DHBIPDA) is introduced as a building block to generate cross‐linked, ultra‐thin microporous nanofilms (sub‐10 nm) via interfacial polymerization, enabling rapid, and precise molecular nanofiltration. Using diacyl chloride (TPC) as the cross‐linker instead of trimesoyl chloride (TMC) significantly reduces the pore sizes within the membranes and achieves a narrower pore distribution due to a semi‐crystalline structure. The film structures are confirmed using comprehensive characterization techniques including wide‐angle X‐ray scattering (WAXS), X‐ray diffraction (XRD), positron annihilation lifetime spectroscopy (PALS), CO2 adsorption analysis, and molecular‐scale simulation. The DHBIPDA/TPC and DHBIPDA/TMC membranes achieve methanol permeance values of up to 16.4 and 15.1 LMH bar−1 coupled with molecular weight cutoffs (MWCOs) as low as 283 and 306 Da, respectively. The DHBIPDA/TPC membrane demonstrates both higher permeance and higher selectivity compared to its relatively disordered counterpart DHBIPDA/TMC, consistent with characterization data. The DHBIPDA‐derived membrane efficiently separates dye mixtures with similar molecular weights and enables effective recycling of organometallic homogeneous catalysts, suggesting its potential for industrial applications. [ABSTRACT FROM AUTHOR]

Published
2024
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10. Thin Film Composite Membranes with Regulated Crossover and Water Migration for Long‐Life Aqueous Redox Flow Batteries

Author

Tan, Rui, primary, Wang, Anqi, additional, Ye, Chunchun, additional, Li, Jiaxi, additional, Liu, Dezhi, additional, Darwich, Barbara Primera, additional, Petit, Luke, additional, Fan, Zhiyu, additional, Wong, Toby, additional, Alvarez‐Fernandez, Alberto, additional, Furedi, Mate, additional, Guldin, Stefan, additional, Breakwell, Charlotte E., additional, Klusener, Peter A. A., additional, Kucernak, Anthony R., additional, Jelfs, Kim E., additional, McKeown, Neil B., additional, and Song, Qilei, additional

Published
2023
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11. Ion‐Selective Microporous Polymer Membranes with Hydrogen‐Bond and Salt‐Bridge Networks for Aqueous Organic Redox Flow Batteries

Author

Wang, Anqi, primary, Tan, Rui, additional, Liu, Dezhi, additional, Lu, Jiaxin, additional, Wei, Xiaochu, additional, Alvarez‐Fernandez, Alberto, additional, Ye, Chunchun, additional, Breakwell, Charlotte, additional, Guldin, Stefan, additional, Kucernak, Anthony R., additional, Jelfs, Kim E., additional, Brandon, Nigel P., additional, McKeown, Neil B., additional, and Song, Qilei, additional

Published
2023
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12. Author Correction: Hydrophilic microporous membranes for selective ion separation and flow-battery energy storage

Author

Tan, Rui, Wang, Anqi, Malpass-Evans, Richard, Williams, Rhodri, Zhao, Evan Wenbo, Liu, Tao, Ye, Chunchun, Zhou, Xiaoqun, Darwich, Barbara Primera, Fan, Zhiyu, Turcani, Lukas, Jackson, Edward, Chen, Linjiang, Chong, Samantha Y., Li, Tao, Jelfs, Kim E., Cooper, Andrew I., Brandon, Nigel P., Grey, Clare P., McKeown, Neil B., and Song, Qilei

Published
2020
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14. Solution-Processable Redox-Active Polymers of Intrinsic Microporosity for Electrochemical Energy Storage

Author

Wang, Anqi, primary, Tan, Rui, additional, Breakwell, Charlotte, additional, Wei, Xiaochu, additional, Fan, Zhiyu, additional, Ye, Chunchun, additional, Malpass-Evans, Richard, additional, Liu, Tao, additional, Zwijnenburg, Martijn A., additional, Jelfs, Kim E., additional, McKeown, Neil B., additional, Chen, Jun, additional, and Song, Qilei, additional

Published
2022
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17. Long‐Life Aqueous Organic Redox Flow Batteries Enabled by Amidoxime‐Functionalized Ion‐Selective Polymer Membranes

Author

Ye, Chunchun, primary, Tan, Rui, additional, Wang, Anqi, additional, Chen, Jie, additional, Comesaña Gándara, Bibiana, additional, Breakwell, Charlotte, additional, Alvarez‐Fernandez, Alberto, additional, Fan, Zhiyu, additional, Weng, Jiaqi, additional, Bezzu, C. Grazia, additional, Guldin, Stefan, additional, Brandon, Nigel P., additional, Kucernak, Anthony R., additional, Jelfs, Kim E., additional, McKeown, Neil B., additional, and Song, Qilei, additional

Published
2022
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19. Author Correction: Hydrophilic microporous membranes for selective ion separation and flow-battery energy storage

Author

Tan, Rui, primary, Wang, Anqi, additional, Malpass-Evans, Richard, additional, Williams, Rhodri, additional, Zhao, Evan Wenbo, additional, Liu, Tao, additional, Ye, Chunchun, additional, Zhou, Xiaoqun, additional, Darwich, Barbara Primera, additional, Fan, Zhiyu, additional, Turcani, Lukas, additional, Jackson, Edward, additional, Chen, Linjiang, additional, Chong, Samantha Y., additional, Li, Tao, additional, Jelfs, Kim E., additional, Cooper, Andrew I., additional, Brandon, Nigel P., additional, Grey, Clare P., additional, McKeown, Neil B., additional, and Song, Qilei, additional

Published
2019
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20. Hydrophilic microporous membranes for selective ion separation and flow-battery energy storage

Author

Tan, Rui, primary, Wang, Anqi, additional, Malpass-Evans, Richard, additional, Williams, Rhodri, additional, Zhao, Evan Wenbo, additional, Liu, Tao, additional, Ye, Chunchun, additional, Zhou, Xiaoqun, additional, Darwich, Barbara Primera, additional, Fan, Zhiyu, additional, Turcani, Lukas, additional, Jackson, Edward, additional, Chen, Linjiang, additional, Chong, Samantha Y., additional, Li, Tao, additional, Jelfs, Kim E., additional, Cooper, Andrew I., additional, Brandon, Nigel P., additional, Grey, Clare P., additional, McKeown, Neil B., additional, and Song, Qilei, additional

Published
2019
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21. Interfacial Engineering of Polymer Membranes with Intrinsic Microporosity for Dendrite‐Free Zinc Metal Batteries.

Author

Tan, Rui, He, Hongzhen, Wang, Anqi, Wong, Toby, Yang, Yilin, Iguodala, Sunshine, Ye, Chunchun, Liu, Dezhi, Fan, Zhiyu, Furedi, Mate, He, Guanjie, Guldin, Stefan, Brett, Dan J. L., McKeown, Neil B., and Song, Qilei

Abstract

Metallic zinc has emerged as a promising anode material for high‐energy battery systems due to its high theoretical capacity (820 mAh g−1), low redox potential for two‐electron reactions, cost‐effectiveness and inherent safety. However, current zinc metal batteries face challenges in low coulombic efficiency and limited longevity due to uncontrollable dendrite growth, the corrosive hydrogen evolution reaction (HER) and decomposition of the aqueous ZnSO4 electrolyte. Here, we report an interfacial‐engineering approach to mitigate dendrite growth and reduce corrosive reactions through the design of ultrathin selective membranes coated on the zinc anodes. The submicron‐thick membranes derived from polymers of intrinsic microporosity (PIMs), featuring pores with tunable interconnectivity, facilitate regulated transport of Zn2+‐ions, thereby promoting a uniform plating/stripping process. Benefiting from the protection by PIM membranes, zinc symmetric cells deliver a stable cycling performance over 1500 h at 1 mA/cm2 with a capacity of 0.5 mAh while full cells with NaMnO2 cathode operate stably at 1 A g−1 over 300 cycles without capacity decay. Our work represents a new strategy of preparing multi‐functional membranes that can advance the development of safe and stable zinc metal batteries. [ABSTRACT FROM AUTHOR]

Published
2024
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