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Coupling of Adhesion and Anti‑Freezing Properties in Hydrogel electrolytes for Low‑Temperature Aqueous‑Based Hybrid Capacitors

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Nano-Micro Letters 2024年第2期16卷 15-31页

作者： Jingya Nan Yue Sun Fusheng Yang Yijing Zhang Yuxi Li Zihao Wang Chuchu Wang Dingkun Wang Fuxiang Chu Chunpeng Wang Tianyu Zhu Jianchun Jiang Institute of Chemical Industry of Forest Products Chinese Academy of ForestryKey Laboratory of Biomass Energy and MaterialJiangsu ProvinceNanjing 210042JiangsuPeople’s Republic of China Co‑Innovation Center of Efficient Processing and Utilization of Forest Resources Nanjing Forestry UniversityNanjing 210037JiangsuPeople’s Republic of China Energy Technologies Area Lawrence Berkeley National LaboratoryBerkeleyCA 94720USA Department of Materials Science and Engineering Clemson UniversityClemsonSC 29634USA

Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appealing solid-state electrolytes because of eco-friendliness,high conductivity and intrinsic flexibility.However,the electrolyte/electrode interfacial contact and anti-freezing properties of current Hydrogel electrolytes are still challenging for practical applications of zinc-ion capacitors.Here,we report a class of Hydrogel electrolytes that couple high interfacial adhesion and anti-freezing performance.The synergy of tough hydrogel matrix and chemical anchorage enables a well-adhered interface between hydrogel electrolyte and electrode.Meanwhile,the cooperative solvation of ZnCl2 and LiCl hybrid salts renders the hydrogel electrolyte high ionic conductivity and mechanical elasticity simultaneously at low temperatures.More significantly,the Zn||carbon nanotubes hybrid capacitor based on this hydrogel electrolyte exhibits low-temperature capacitive performance,delivering high-energy density of 39 Wh kg^(-1)at-60°C with capacity retention of 98.7%over 10,000 cycles.With the benefits of the well-adhered electrolyte/electrode interface and the anti-freezing hydrogel electrolyte,the Zn/Li hybrid capacitor is able to accommodate dynamic deformations and function well under 1000 tension cycles even at-60°C.This work provides a powerful strategy for enabling stable operation of low-temperature zinc-ion capacitors.

关键词： Interfacial adhesion Anti-freezing Hydrogel electrolytes Low-temperature hybrid capacitors Dynamic deformati

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High Na-ion conductivity andmechanical integrity of anion-exchanged polymeric Hydrogel electrolytes for flexible sodium ion hybrid energy storage

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SusMat 2024年第1期4卷 140-153页

作者： JungWoo Hong Harpalsinh H.Rana Jeong Hee Park Jun Su Kim Sang Joon Lee Gun Jang Tae Hoon Kang Kang Ho Shin Sang Ha Baek Wooseok Yang Kwang Ho Kim Ju-Hyuk Lee Ho Seok Park School of Chemical Engineering Sungkyunkwan UniversitySuwonRepublic of Korea Clean Energy Research Center Korea Institute of Science and Technology(KIST)SeoulRepublic of Korea KIST-SKKU Carbon-Neutral Research Center Sungkyunkwan University(SKKU)SuwonRepublic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwonRepublic of Korea COSMOS LAB/92 Jomaru-ro 385beon-gilBucheon-siRepublic of Korea SKKU Advanced Institute of Nano Technology(SAINT) Sungkyunkwan UniversitySuwonRepublic of Korea Department of Health Sciences and Technology Samsung Advanced Institute for Health Sciences and Technology(SAIHST)Sungkyunkwan UniversitySuwonRepublic of Korea

The polymeric gel electrolytes are attractive owing to their higher ionic conductivities than those of dry polymer electrolytes and lowered water activity for enlarged potential window.However,the ionic conductivity and mechanical strength of the Na-ion conducting polymeric gel electrolytes are limited by below 20 mS cm−1 and 2.2 MPa.Herein,we demonstrate Na-ion conducting and flexible polymeric Hydrogel electrolytes of the chemically coupled poly(diallyldimethylammonium chloride)-dextrin-N,N′-methylene-bisacrylamide film immersed in NaClO_(4) solution(ex-DDA-Dex+NaClO_(4))for flexible sodium-ion hybrid capacitors(f-NIHC).In particular,the anion exchange reaction and synergistic interaction of ex-DDA-Dex with the optimum ClO_(4)−enable to greatly improve the ionic conductivity up to 27.63 mS cm−1 at 25◦C and electrochemical stability window up to 2.6 V,whereas the double networking structure leads to achieve both the mechanical strength(7.48 MPa)and softness of Hydrogel electrolytes.Therefore,the f-NIHCs with the ex-DDA-Dex+NaClO_(4) achieved high specific and high-rate capacities of 192.04 F g^(−1)at 500 mA g^(−1)and 116.06 F g^(−1)at 10000 mA g^(−1),respectively,delivering a large energy density of 120.03Wh kg^(−1)at 906Wkg^(−1)and long cyclability of 70%over 500 cycles as well as demonstrating functional operation under mechanical stresses.

关键词： anion exchange chemistry flexible energy storage hybrid energy storage Hydrogel electrolytes renewable electrolytes sodium storage

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Regulating Thermogalvanic Effect and Mechanical Robustness via Redox Ions for Flexible Quasi‑Solid‑State Thermocells

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Nano-Micro Letters 2022年第5期14卷 153-167页

作者： Peng Peng Jiaqian Zhou Lirong Liang Xuan Huang Haicai Lv Zhuoxin Liu Guangming Chen College of Materials Science and Engineering Shenzhen UniversityShenzhen 518055People’s Republic of China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060People’s Republic of China

The design of power supply systems for wearable applications requires both flexibility and durability.Thermoelectrochemical cells(TECs)with large Seebeck coefficient can efficiently convert lowgrade heat into electricity,thus having attracted considerable attention in recent years.Utilizing hydrogel electrolyte essentially addresses the electrolyte leakage and complicated packaging issues existing in conventional liquid-based TECs,which well satisfies the need for flexibility.Whereas,the concern of mechanical robustness to ensure stable energy output remains yet to be addressed.Herein,a flexible quasisolid-state TEC is proposed based on the rational design of a hydrogel electrolyte,of which the thermogalvanic effect and mechanical robustness are simultaneously regulated via the multivalent ions of a redox couple.The introduced redox ions not only endow the hydrogel with excellent heat-to-electricity conversion capability,but also act as ionic crosslinks to afford a dual-crosslinked structure,resulting in reversible bonds for effective energy dissipation.The optimized TEC exhibits a high Seebeck coefficient of 1.43 mV K−1 and a significantly improved fracture toughness of 3555 J m^(−2),thereby can maintain a stable thermoelectrochemical performance against various harsh mechanical stimuli.This study reveals the high potential of the quasi-solid-state TEC as a flexible and durable energy supply system for wearable applications.

关键词： Thermocells Thermoelectric Flexible energy devices Wearable applications Hydrogel electrolytes

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