4.8 Article

Modulation of hydrogel electrolyte enabling stable zinc metal anode

Journal

ENERGY STORAGE MATERIALS
Volume 51, Issue -, Pages 588-598

Publisher

ELSEVIER
DOI: 10.1016/j.ensm.2022.06.034

Keywords

Zn metal anode; Hydrogel electrolyte; Polymetric anion; Uniform zinc deposition; Anti-corrosion

Funding

  1. National Natural Science Foundation of China [51874362, 52002270]
  2. China Postdoctoral Science Foundation [2020M670661]

Ask authors/readers for more resources

This study systematically investigates hydrogel electrolytes for zinc metal anodes (ZMAs) by regulating their crosslinking and grafting structures. The results highlight the importance of network structure and polymeric anions in the hydrogel. The PSX gel, crosslinked by carboxyl-grafted polyvinyl alcohol and xanthan gum, demonstrates superior performance with high ionic conductivity and a considerable Zn2+ transference number. Zn//Zn cells with PSX electrolytes show uniform zinc deposition, minimal by-products, and suppressed hydrogen evolution. The PSX electrolyte also exhibits good compatibility and excellent performance when paired with V2O5 or active carbon cathodes. Flexible pouch cells withstand different deformation and stress conditions.
The uneven flux and strong solvation of Zn2+ ions in aqueous electrolytes bring undesirable dendritic deposition and side reactions to zinc metal anodes (ZMAs). Hydrogel electrolytes have considerable mechanical strength and limited water content, which can suppress dendrite growth and alleviate side reactions. Nevertheless, the design of hydrogel electrolytes with desired electrochemical and mechanical properties is still challenged due to the lack of understanding of how structural features affect performances. Herein, we systematically investigate the hydrogel electrolytes for ZMAs by regulating their crosslinking and grafting structures. Experiments and theoretical simulations emphasize the importance of the network structure and the polymetric anions bonded on the hydrogel. The PSX gel crosslinked by carboxyl-grafted polyvinyl alcohol and xanthan gum shows superior performance, contributed by its abundant -COO- groups and stable three-dimensional structure. The PSX electrolyte shows high ionic conductivity (18.86 mS cm-1) and a considerable Zn2+ transference number (0.8). Zn// Zn cells with PSX electrolytes deliver long cycle lives accompanied by uniform zinc deposition, few by-products, and suppressed hydrogen evolution. When paired with V2O5 or active carbon cathodes, the PSX electrolyte also shows good compatibility and excellent performance. Flexible pouch cells are further demonstrated to work normally under different deformation and stress conditions.

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.8
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Chemistry, Physical

Highly stable operation of LiCoO2 at cut-off ≥ 4.6 V enabled by synergistic structural and interfacial manipulation

Ang Fu, Zhengfeng Zhang, Jiande Lin, Yue Zou, Changdong Qin, Chuanjing Xu, Pengfei Yan, Ke Zhou, Jialiang Hao, Xuerui Yang, Yong Cheng, De-Yin Wu, Yong Yang, Ming-Sheng Wang, Jianming Zheng

Summary: In this work, a synergistic strategy of Mg doping and Se coating is proposed to enhance the high-voltage electrochemical performance and cycling life of LiCoO2 as a cathode material for high energy density batteries.

ENERGY STORAGE MATERIALS (2022)

Article Chemistry, Physical

Eight-Electron Redox Cyclohexanehexone Anode for High-Rate High-Capacity Lithium Storage

Sha Li, Jiande Lin, Yimiao Zhang, Shilin Zhang, Tao Jiang, Zhongli Hu, Junjie Liu, De-Yin Wu, Li Zhang, Zhongqun Tian

Summary: Replacing inorganic anodes with organic electrode materials is a promising direction for future green Li-ion batteries. By constructing an insoluble and highly conductive C6O6-polymeric binder-carbon network architecture, this study reveals the potential of C6O6 as an ultra-high capacity and high-rate anode material.

ADVANCED ENERGY MATERIALS (2022)

Review Chemistry, Physical

Plasmonic photoelectrochemical reactions on noble metal electrodes of nanostructures

Karuppasamy Kohila Rani, Rajkumar Devasenathipathy, Jia-Zheng Wang, Xiao-Yuan Hui, Jian-De Lin, Yi-Miao Zhang, Liu-Bin Zhao, Jian-Zhang Zhou, De-Yin Wu, Zhong-Qun Tian

Summary: In this review, we discuss the latest progress on plasmon-mediated chemical reactions of organic molecules such as para-aminothiophenol, substituted para-aminothiophenol and para-nitrothiophenol at nanostructures modified noble metal electrodes using surface enhanced Raman spectroscopy, electrochemical methods, and theoretical calculations.

CURRENT OPINION IN ELECTROCHEMISTRY (2022)

Article Chemistry, Physical

Enabling interfacial stability of LiCoO2 batteries at an ultrahigh cutoff voltage ≥ 4.65 V via a synergetic electrolyte strategy

Ang Fu, Chuanjing Xu, Jiande Lin, Yu Su, Haitang Zhang, De-Yin Wu, Xiaozheng Zhang, Meng Xia, Zhongru Zhang, Jianming Zheng, Yong Yang

Summary: Increasing the cutoff charge voltage of LiCoO2 (LCO) poses a challenge in balancing high energy density and long cycling life. By adding 2,3-dimethylmaleic anhydride (DMMA) as an electrolyte additive, a stable and robust CEI film enriched with inorganic species is formed, preventing decomposition of electrolytes and erosion of LCO. Experimental techniques combined with theoretical calculations reveal the functioning mechanism. The addition of DMMA improves LCO's capacity retention after cycles, and the presence of other additives further enhances LCO's high-voltage stability.

JOURNAL OF MATERIALS CHEMISTRY A (2023)

Article Chemistry, Physical

Implanting single-atom N2-Fe-B2 catalytic sites in carbon hosts to stabilize high-loading and lean-electrolyte lithium-sulfur batteries

Sha Li, Jiande Lin, Bin Chang, Daiwen Yang, De-Yin Wu, Junhao Wang, Weijia Zhou, Hong Liu, Shuhui Sun, Li Zhang

Summary: Researchers have developed a carbon-supported single-atom catalyst (SAC) for lithium-sulfur batteries. The catalyst not only immobilizes lithium polysulfide (LiPS) but also promotes sulfur redox reactions, leading to improved battery performance. The SACs showed high durability and areal capacities, even under harsh conditions.

ENERGY STORAGE MATERIALS (2023)

Article Chemistry, Physical

Interface Engineering Enhances Pseudocapacitive Contribution to Alkali Metal Ion Batteries

Xuefang Xie, Shuang Zhou, Guozhao Fang, Jiande Lin, Yuanlang Wan, Guozhong Cao, Anqiang Pan

Summary: Enhancing pseudocapacitive contribution through interface engineering is an effective method to improve the diffusion-limited redox mechanism in electrode materials. In this study, a nitrogen-doped three-dimensional carbon skeleton with Sb2S3@TiO2 composite was designed as an anode for lithium (sodium)-ion batteries, which showed significantly enhanced pseudocapacitive contribution. Sb2S3 contributed to high capacity, while the addition of amorphous TiO2 improved stability by suppressing excessive growth of Sb2S3 on the carbon framework.

ACS APPLIED ENERGY MATERIALS (2023)

Article Chemistry, Physical

Constructing a Stabilized Cathode Electrolyte Interphase for High- Voltage LiCoO2 Batteries via the Phenylmaleic Anhydride Additive

Xi Liu, Ang Fu, Jiande Lin, Yue Zou, Gaopan Liu, Weitong Wang, De-Yin Wu, Yong Yang, Jianming Zheng, Liyi Ye

Summary: By adding the electrolyte additive phenylmaleic anhydride (PMA), a stable cathode electrolyte interphase (CEI) film can be formed, which improves the cycle life and capacity retention of LCO batteries.

ACS APPLIED ENERGY MATERIALS (2023)

Article Chemistry, Multidisciplinary

Building Fast Ion-Conducting Pathways on 3D Metallic Scaffolds for High-Performance Sodium Metal Anodes

Xuan Lu, Hongyang Zhao, Yanyang Qin, Edward Matios, Jianmin Luo, Ruochen Chen, Hu Nan, Bo Wen, Yanan Zhang, Yuyang Li, Qiangrui He, Xuetian Deng, Jiande Lin, Kai Zhang, Hongkang Wang, Kai Xi, Yaqiong Su, Xiaofei Hu, Shujiang Ding, Weiyang Li

Summary: Building 3D electron-conducting scaffolds is an effective way to alleviate dendritic growth and volume change of sodium (Na) metal anodes. A uniform Na plating on the 3D scaffold is achieved by synthesizing NiF2 hollow nanobowls grown on nickel foam (NiF2@NF), which can be electrochemically converted to a NaF-enriched SEI layer. The NaF-enriched SEI layer enables rapid Na(+) transfer throughout the entire 3D scaffold, resulting in densely filled and dendrite-free Na metal anodes.

ACS NANO (2023)

Article Chemistry, Physical

Switchable Organic Low-Loss Spin Filters Based on Gold-Viologen- Gold Molecular Junctions

Zhuan-Yun Cai, Si-Yuan Guan, Zi-Wei Ma, Jian-De Lin, Rajkumar Devasenathipathy, De-Yin Wu, Bing-Wei Mao, Zhong-Qun Tian

Summary: Modulating functional groups on molecules can achieve novel electron transport properties in single-molecule electronics. In this work, viologen derivatives with three attached organic radicals including sp2 hybridized O•, NH•, and CH2• are studied for their spin transport properties. The results show excellent spin filtering efficiency (SFE) with α spin conductance being about 100 times larger than β spin conductance within a low-bias window. The findings also demonstrate the tunability of SFE by altering alkyl chain length and applied bias, providing a new strategy for developing viologen-based radical systems as single-molecule spin switches.

JOURNAL OF PHYSICAL CHEMISTRY C (2023)

Article Multidisciplinary Sciences

Resolving nanostructure and chemistry of solid-electrolyte interphase on lithium anodes by depth-sensitive plasmon-enhanced Raman spectroscopy

Yu Gu, En-Ming You, Jian-De Lin, Jun-Hao Wang, Si-Heng Luo, Ru-Yu Zhou, Chen-Jie Zhang, Jian-Lin Yao, Hui-Yang Li, Gen Li, Wei-Wei Wang, Yu Qiao, Jia-Wei Yan, De-Yin Wu, Guo-Kun Liu, Li Zhang, Jian-Feng Li, Rong Xu, Zhong-Qun Tian, Yi Cui, Bing-Wei Mao

Summary: In this study, a depth-sensitive plasmon-enhanced Raman spectroscopy (DS-PERS) method is developed for in situ and nondestructive characterization of the nanostructure and chemistry of the solid-electrolyte interphase (SEI) in lithium metal batteries. Insights from the DS-PERS study reveal the profound influences of lithium in modifying SEI formation and regulating Li-ion desolvation and subsequent Li deposition. Furthermore, a cycling protocol that promotes direct SEI formation is developed, significantly enhancing the performance of anode-free Li metal batteries.

NATURE COMMUNICATIONS (2023)

Article Chemistry, Applied

Construction of strong built-in electric field in binary metal sulfide heterojunction to propel high-loading lithium-sulfur batteries

Weiming Xiong, Jiande Lin, Huiqun Wang, Sha Li, Junhao Wang, Yuxiang Mao, Xiao Zhan, De-Yin Wu, Li Zhang

Summary: This study presents the design and construction of high-sulfur-loaded and durable Li-S batteries using a binary metal sulfide MnS-MoS2 heterojunction electrocatalyst. The MnS-MoS2 hybrid host exhibits strong soluble polysulfide affinity, enhanced electronic conductivity, and exceptional catalytic effect on sulfur reduction. The S/ MnS-MoS2 cathode derived from this hybrid host shows superb rate capability and durable cyclability.

JOURNAL OF ENERGY CHEMISTRY (2023)

Article Chemistry, Multidisciplinary

Doping Engineering of M-N-C Electrocatalyst Based Membrane-Electrode Assembly for High-Performance Aqueous Polysulfides Redox Flow Batteries

Bixian Chen, Huan Huang, Jiande Lin, Kailing Zhu, Le Yang, Xiang Wang, Jiajia Chen

Summary: Co, Zn dual-doped N-C complex enhances the electrochemical adsorption behaviors for Na2S2 and improves the redox activity compared to the bare glassy carbon electrode. The membrane-electrode assembly (MEA) based on Co, Zn-doped N-C complex enhances the redox performances and relieves the crossover in PS-ARFBs, achieving an impressively high and reversible capacity of 157.5 Ah L-1 for Na2S2. Moreover, a full cell PS-ARFB exhibits high energy efficiency of approximately 88.4% at 10 mA cm(-2) and a very low capacity decay rate of 0.0025% per cycle at 60 mA cm(-2) over 200 cycles.

ADVANCED SCIENCE (2023)

Article Chemistry, Physical

Influence of Adsorption of para-Aminothiophenol on Trap States and Recombination Kinetics at Plasmonic Ag-TiO2 Heterostructure Interfaces

Dan Wang, Zhi-Hao Liang, Yuan-Hui Xiao, Jian-De Lin, Jian-Zhang Zhou, De-Yin Wu

Summary: Through the combination of spectroscopic, electrochemical, and photoelectrochemical methods, the variation of trap states and kinetics on the Ag-TiO2 interfaces after the adsorption of reactant molecules was investigated using para-aminothiophenol (PATP) as a probe molecule. Results from photoluminescence spectroscopy and chronoamperometry revealed the distribution of trap states and the influence of PATP's adsorption on Ag-TiO2 heterostructures. Kinetic measurements of open-circuit photovoltage showed that PATP adsorption affects the electron lifetime and recombination mechanism of charge carriers on Ag-TiO2 heterostructures.

CHEMPHOTOCHEM (2023)

Article Chemistry, Multidisciplinary

Reversible Multielectron Redox Chemistry in a NASICON-Type Cathode toward High-Energy-Density and Long-Life Sodium-Ion Full Batteries

Yifan Zhou, Guofu Xu, Jiande Lin, Yangpu Zhang, Guozhao Fang, Jiang Zhou, Xinxin Cao, Shuquan Liang

Summary: In this study, a novel Fe-substituted Na3.5V1.5Fe0.5(PO4)3 (NVFP) cathode with Na-superionic-conductor (NASICON) structure is proposed, which realizes reversible structural evolution and multi-electron redox reactions (Fe2+/Fe3+, V3+/V4+, and V4+/V5+) by incorporating iron. The NVFP cathode delivers excellent capacity and cycling stability, and the low ionic migration energy barrier and ideal Na+ diffusion kinetics are elucidated. Coupling with a hard carbon anode, HC//NVFP full cells demonstrate high-rate capability and long cycling lifespan, with material-level energy density up to 304 Wh kg-1.

ADVANCED MATERIALS (2023)

Article Chemistry, Physical

Stereoelectronic Switches of Single-Molecule Junctions through Conformation-Modulated Intramolecular Coupling Approaches

Zhuan-Yun Cai, Zi-Wei Ma, Wen-Kai Wu, Jian-De Lin, Lin-Qi Pei, Jia-Zheng Wang, Tai-Rui Wu, Shan Jin, De-Yin Wu, Zhong-Qun Tian

Summary: This study demonstrates the existence of three stable intramolecular conformations in single-molecule junctions, with different electronic coupling approaches and significant differences in molecular conductance. The populations of these conformations are highly dependent on solvent effects and external electric fields. Modulating intramolecular electronic coupling approaches offers a useful manner to achieve molecular switches with high switching ratios.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2023)

Article Chemistry, Physical

Quantifying the impact of operating temperature on cracking in battery electrodes, using super-resolution of microscopy images and stereology

Orkun Furat, Donal P. Finegan, Zhenzhen Yang, Matthias Neumann, Sangwook Kim, Tanvir R. Tanim, Peter Weddle, Kandler Smith, Volker Schmidt

Summary: The operating temperature has a significant impact on the degradation behavior of batteries. This study investigates the structural degradation of lithium-ion positive electrodes under different operating temperatures, and finds that particle porosity increases with higher cycling temperature, while particle surface area remains similar across different cycling-temperature aging conditions.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Ion-intercalation architecture for robust functionalization of two-dimensional MXenes

Junyan Li, Ming Lu, Weijia Zheng, Wei Zhang

Summary: MXenes are two-dimensional materials with unique structures and properties, which have attracted significant scientific interest. Ion intercalation, as an important mechanism, plays a crucial role in regulating the electronic and chemical properties of MXene materials. This review provides an overview of the interaction events between ions and MXenes, including advanced characterization techniques, influencing factors, mechanisms, and functionalization roles of ion intercalation.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Zwitterion as electrical double layer regulator to in-situ formation of fluorinated interphase towards stable zinc anode

Zhengtai Zha, Tianjiang Sun, Diantao Li, Tao Ma, Weijia Zhang, Zhanliang Tao

Summary: A novel zwitterion additive is developed to improve the electrochemical performance and cycling stability of aqueous zinc batteries. The zwitterion forms a stable solid electrolyte interphase on the electrode surface, isolating the zinc anode from the electrolytes and enabling fast zinc ion migration. The proposed electrolyte shows promising results in symmetric cells and full cells, with long cycling stability and high capacity retention.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Promoting homogeneous lithiation of silicon anodes via the application of bifunctional PEDOT:PSS/PEG composite binders

Nyung Joo Kong, Myeong Seon Kim, Jae Hyun Park, Jongbok Kim, Jungho Jin, Hyun-Wook Lee, Seok Ju Kang

Summary: Polymeric conducting binders have significant research value as they can serve as both binders and conducting agents, increasing the proportion of active materials in batteries and the volumetric energy density. This study explores the potential of a composite of PEDOT:PSS and polyethylene glycol (PEG) as a high-performing binder for silicon anodes. The addition of PEG polymer enhances the conductivity of PEDOT:PSS and improves the mechanical properties of the silicon anode, resulting in extended cycle endurance. The use of operando optical microscopy allows for direct observation of the binder's operation. Consequently, the bifunctional PEDOT:PSS/PEG binder shows promise for high-performance lithium-ion battery binders.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Temperature-dependent viscoelastic liquid MOFs based cellulose gel electrolyte for advanced lithium-sulfur batteries over an extensive temperature range

Yangze Huang, Lixuan Zhang, Jiawen Ji, Chenyang Cai, Yu Fu

Summary: This study proposed a novel temperature-dependent viscoelastic liquid electrolyte and a hollow transition bi-metal selenide as the sulfur host material to address the issues in Li-S batteries. The experiments showed promising results in stabilizing the anode and improving cycling performance.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Recent advances in anode design for mild aqueous Zn-ion batteries

Ao Yu, Wei Zhang, Nimanyu Joshi, Yang Yang

Summary: This review provides a comprehensive overview of research progress in ZIB anodes, including protective coating layers on zinc surfaces and intercalated anode materials. By designing protective coating layers and selecting appropriate intercalated anode materials, the inherent limitations of zinc metal anode can be overcome, leading to improved reliability and performance of ZIBs.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Sandwich-structured anode enables high stability and enhanced zinc utilization for aqueous Zn-ion batteries

Xin Wang, Yumiao Tian, Konghua Yang, Chenhui Ma, Wenqiang Lu, Xiaofei Bian, Nan Chen, Heng Jiang, Yan Li, Xing Meng, Pengyue Gao, Dong Zhang, Fei Du

Summary: Researchers developed a new sandwich deposition approach using boron nitride layer as a current collector, which enhances the performance of aqueous zinc-ion batteries.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Stable sodium-metal batteries with a hierarchical structured electrode toward reversible confinement of Na dendrites

Sang Jun Lee, Dongwoo Kang, Dong Yeol Hyeon, Dong Seok Kim, Suyoon Eom, Su Hwan Jeong, Dong Park Lee, Dawon Baek, Jou-Hyeon Ahn, Gyeong Hee Ryu, Kwi-Il Park, San Moon, Joo-Hyung Kim

Summary: This study utilizes the ice-templating method to create a self-supporting three-dimensional hierarchical porous structure, which effectively inhibits sodium dendrite growth and improves the performance and longevity of sodium-metal batteries.

ENERGY STORAGE MATERIALS (2024)

Article Chemistry, Physical

Enable reversible conversion reaction of copper fluoride batteries by hydroxyl solution and anion acceptor

Yifan Yu, Meng Lei, Yangyang Liu, Keyi Chen, Chuanzhong Lai, Jiulin Hu, Chilin Li

Summary: Metal fluorides as conversion-reaction cathodes have advantages such as low cost, environmentally friendly, and high energy density. In this study, a hydroxyl-rich copper fluoride (Cu2(OH)3F) was proposed as a conversion cathode, coupled with an electrolyte additive engineering, to address the poor reversibility issue. The presence of OH in Cu2(OH)3F enables effective suppression of Cu+ dissolution, resulting in better reaction reversibility and kinetics.

ENERGY STORAGE MATERIALS (2024)