{"title":"Ultrafast cathode assembled using small reduced graphene oxide sheets enables a 2,000 C rate supercapacitor with high energy density","authors":"Mengzhao Yang, Huayan Liu, Chenxin Zhou, Haoyang Chen, Xin Chen, Qinglei Liu, Jiajun Gu","doi":"10.1016/j.ensm.2024.103951","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103951","url":null,"abstract":"To realize ultrafast supercapacitors, a series of ultrahigh-rate (≥1,000 mV s<sup>−1</sup>) anodes that break a well-known “energy vs. power dilemma” in aqueous electrolytes have been successfully developed over the past five years. However, their matching cathodes are still limited by slow ion transport dynamics and oxidation. Here, we report a series of hydrated films that comprise small sheets of reduced graphene oxide (SSs−rGO, <100 nm in average lateral size) and feature short interlayered pathways (∼100 nm) for rapid ion transport and high oxidation resistance. As the first ultrahigh-rate cathode with areal capacitance (<em>C</em><sub>a</sub>) satisfying an industrial requirement (>0.6 F cm<sup>−2</sup>), the SSs−rGO electrode (5.0 mg cm<sup>−2</sup>) delivers a <em>C</em><sub>a</sub> of 0.61 F cm<sup>−2</sup> and a gravimetric capacitance of 123 F g<sup>−1</sup> at an ultrahigh-rate of 3,000 mV s<sup>−1</sup>. Combining with a Ti<sub>3</sub>C<sub>2</sub>T<sub>x</sub> anode, the cathode enables a 1.8 V ultrafast aqueous supercapacitor that delivers energy densities of 0.14 and 0.09 mWh cm<sup>−2</sup> for discharges in 1.79 and 0.97 s (∼2,000 and 3,700 C rate), respectively. These values double (at 2,000 C) and almost ten-fold (at 3,700 C) those of the ever-reported supercapacitors operating at the corresponding rates. The present strategy paves a road to ultrafast (>1,000 C) and high-energy-density supercapacitors, by which energy charge/discharge can finish within 3.6 s.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"200 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142804723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Tailoring Electrolyte Solvation of Dimethyl Sulfite with Fluoride Dominant via Electrolyte Engineering for Enabling Low-Temperature Batteries","authors":"Heng Zhang, Xiaolong Wu, Weilong Kong, Minghao Huang, Yejuan Xue, Hongfa Xiang, Zhimei Huang","doi":"10.1016/j.ensm.2024.103955","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103955","url":null,"abstract":"Carbonate electrolytes are the primary determinant for the development of low-temperate lithium metal batteries (LT-LMBs). However, conventional ethyl carbonate (EC)-based electrolytes with solvent-dominated solvation configuration suffer from sluggish reaction kinetics, severe interfacial side reactions and high Li<sup>+</sup> desolvation energy under low temperature. Herein, an EC-free and weakly solvated electrolyte consisting of LiDFOB and mixed solvents including dimethyl sulfite (DMS), ethyl trifluoroacetate (ETFA) and fluoroethylene carbonate (FEC) was designed to facilitate the reaction kinetics and stabilize the interfaces of LT-LMBs, where a fluoride-rich solvation structure including FEC, ETFA and DFOB<sup>-</sup> is formed in the designed electrolyte. Such solvation configuration could significantly facilitate the desolvation process and induce the homogeneous Li deposition by forming high ionic conductive and inorganics-rich protective film on the electrode surfaces. With such electrolyte, the Li||NCM811 cell retains a high capacity retention of 81.7% after 1000 cycles, which is far superior to the 31.3% for EC-based electrolyte. Even at -40°C, the cell exhibits a capacity of 125.7 mAh g<sup>-1</sup> with almost no capacity attenuation after 200 cycles. This work confirms the necessity of fluoride-dominated solvation structure in decreasing the desolvation energy and accelerating the ionic transfer, contributing a promising solution to the development of low-temperature LMBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"20 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797678","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Tingting Xu, Kun Qin, Chunxi Tian, Liangdong Lin, Weiping Li, Liumin Suo
{"title":"Searching for the Ideal Li1+xTMO2 Cathode for Anode-free Li Metal Batteries","authors":"Tingting Xu, Kun Qin, Chunxi Tian, Liangdong Lin, Weiping Li, Liumin Suo","doi":"10.1016/j.ensm.2024.103956","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103956","url":null,"abstract":"Anode-free lithium metal batteries push the energy density higher and minimize battery production costs as low as possible. However, the fast capacity decay impedes their commercial viability, primarily due to the lack of excessive Li from the anode to compensate for the irreversible lithium loss. Thus, the Li-rich NCM cathode is a feasible way to solve the issue. In this work, to search for the ideal Li<sub>1+x</sub>TMO<sub>2</sub> cathode for anode-free Li metal batteries, we selected the two types of commonly used layered cathode materials (LiTMO<sub>2</sub>: NCM622 and NCM811) to enrich Li converting into Li<sub>2</sub>TMO<sub>2</sub> by both chemical lithiation (C-Li) and electrochemical lithiation (E-Li) methods. Our findings show that the Li-rich NCM622 lithiated by the E-Li method is an ideal choice among our candidates, which has a high lithiation degree that almost covers the entire reversible transition range from Li<sub>1</sub> to Li<sub>2</sub> without additional by-products and a negative impact on kinetic performance. Based on the above results, we further demonstrated that the Li<sub>1.33</sub>NCM622|Cu pouch cell presents a longer cycle life of more than 200 times with a high capacity retention of 74%.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"37 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797679","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wei Zhao, Fengmei Wang, Zerui Chen, Yue Yang, Yaqiong Su, Leyi Ye, Jianyuan Hu, Fei Wang, Hao Bin Wu
{"title":"Metal-Organic Polyhedrons Modulated Eccentric Solvation Sheath Enables Fast Charge Transfer Kinetics in Nonaqueous Zn Electrolytes","authors":"Wei Zhao, Fengmei Wang, Zerui Chen, Yue Yang, Yaqiong Su, Leyi Ye, Jianyuan Hu, Fei Wang, Hao Bin Wu","doi":"10.1016/j.ensm.2024.103957","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103957","url":null,"abstract":"Zn batteries emerge as a promising class of energy storage devices with high energy density, low cost and high safety. Nonaqueous Zn electrolytes offer high interfacial stability yet suffer from sluggish interfacial charge transfer kinetics. Here, we report an eccentric Zn<sup>2+</sup> solvation structure enabled by metal-organic polyhedrons (MOPs) in nonaqueous colloidal electrolytes, which facilitates charge transfer at electrode-electrolyte interface. The resultant Zn<sup>2+</sup>(ZrT)(DMF)<sub>1</sub> solvation structure features a large solvation sheath and a small ion-to-electrode distance, thus reducing the energy required for reorganizing the solvation sheath to accept electron. As a result, the MOPs-modulated colloidal electrolyte enables Zn anode with supreme stability for over 1200 h at 8 mA cm<sup>−2</sup> and 270 h at 12 mA cm<sup>−2</sup>, along with high coulombic efficiency (∼99.8% over 1000 cycles), notably exceeding the performance of conventional aqueous and nonaqueous electrolytes. The design principle of solvation sheath might be broadly applicable to other high-valence metal cation batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"41 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiaming Li, Mengli Li, Chi Guo, Xianglin Zhou, Jiawen Zhang, John Wang, Yunfei Chen, Zhiyang Lyu
{"title":"3D printing of multiscale biomimetic structural electrodes: achieving ultrahigh deformability and areal capacity for Li-ion batteries","authors":"Jiaming Li, Mengli Li, Chi Guo, Xianglin Zhou, Jiawen Zhang, John Wang, Yunfei Chen, Zhiyang Lyu","doi":"10.1016/j.ensm.2024.103958","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103958","url":null,"abstract":"Deformable batteries that are flexible and adaptable to various shapes are crucial power sources for flexible and wearable electronics. Designing of structural electrodes has proven effective in enhancing battery deformability. However, this often compromises electrode areal loading, resulting in lower areal capacities. Herein, we design multiscale biomimetic structural electrodes fabricated via an <em>in-situ</em> directional freezing-assisted 3D printing approach. This new approach effectively incorporates microscopic directionally porous structures and macroscopic serpentine structures, achieving the designed compatibility with ultrahigh deformation and ultrahigh areal capacities simultaneously. The thus-made electrodes allow for exceptional deformability, including 300% stretching, 180° twisting, and 360° bending, while maintaining a high areal loading of up to ∼65%. The half-cells with directional micro-channel electrodes demonstrate superior specific capacities, cycling stability, and rate capability, when compared to the cells with nondirectional electrodes. The assembled Li-ion full-cell can readily power LEDs in various deformable states, and a structure-integrated wearable watch device is designed in a bent watchband configuration. Our new strategy offers a rational design approach for highly deformable and customized electrodes, advancing the development of deformable batteries for wearable devices.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"9 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797732","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhaoyu Ran, Mingcong Yang, Rui Wang, Junluo Li, Manxi Li, Li Meng, Yuhang Liu, Jun Hu, Jinliang He, Qi Li
{"title":"Surface-gradient-structured polymer films with restricted thermal expansion for high-temperature capacitive energy storage","authors":"Zhaoyu Ran, Mingcong Yang, Rui Wang, Junluo Li, Manxi Li, Li Meng, Yuhang Liu, Jun Hu, Jinliang He, Qi Li","doi":"10.1016/j.ensm.2024.103952","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103952","url":null,"abstract":"The capacitive performance of existing dielectric polymers deteriorates significantly at elevated temperatures, although their thermal stability far exceeds, which remains a major challenge for efficient dielectric energy storage under extreme conditions. Here, a material design inspired by the cross-property connection phenomena, which bridges the seemingly unrelated material properties through similar or relevant determining microscopic factors, is reported to achieve substantially improved high-temperature capacitive performance in dielectric polymers. A high consistency is unveiled between the high-temperature electrical properties and thermal expansion of dielectric polymers, based on which a surface-gradient crosslinking structure is designed to inhibit the thermal distortion. It is confirmed by both experimental results and computational simulations that the restricted thermal expansion gives rise to reduced free volume as well as suppressed β-relaxation, which account for the marked improvements in high-temperature capacitive performances. At the optimal composition, the resultant polymer exhibits an ultrahigh discharged energy density up to 4.9 J/cm<sup>3</sup> at 200 °C with a charge-discharge efficiency of 90%, which is superior to all the existing polymer films based on the surface modification. This work highlights the significance of correlating variations in different physical properties for the design of high-energy-density polymer dielectrics capable of operating under harsh environments.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"7 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793194","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Advanced High‒Entropy Materials for High‒Quality Energy Storage and Conversion","authors":"Zengyuan Fan, Jiawei Wang, Yunpeng Wu, Peng Zhang","doi":"10.1016/j.ensm.2024.103954","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103954","url":null,"abstract":"Due to global shifts in energy consumption and increasing demand for efficient, safe, and cost‒effective energy storage solutions, high‒entropy materials (HEMs) have garnered great attention. The HEMs, composed of five or more elements in near‒equimolar ratios, exhibit unique properties such as high entropy effects, lattice distortion, sluggish diffusion kinetics, and the \"cocktail\" effect. These characteristics of HEMs significantly enhance the performance of rechargeable batteries and supercapacitors by improving electronic conductivity and ionic transport of the relevant battery composition as well as expanding the operational battery temperature. This paper timely summarizes the function principles of the four primary enhancement mechanisms of HEMs and resultant recent applications in energy storage and conversion technologies, including cathodes, anodes, and electrolytes. Considerable emphasis is focused on the functional orientation screen and the synthesis of HEM elements/structures towards stability and power capability of the electrode reactions. Finally, the current challenge, the possible solving strategies and the future research trend for HEMs are outlined. It is believed that this review will offer timely and comprehensive information on the future research directions of HEMs to boost high‒performance energy storage communities.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"27 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793193","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hao Huang, Jingang Zheng, Hongyang Li, Siqi Guan, Hongwei Zhao, Weichen Han, Han Zhang, Guangshen Jiang, Lixiang Li, Baigang An, Chengguo Sun
{"title":"Self-induced corrosion of Ni-rich cathode materials by fluor-lithium salts","authors":"Hao Huang, Jingang Zheng, Hongyang Li, Siqi Guan, Hongwei Zhao, Weichen Han, Han Zhang, Guangshen Jiang, Lixiang Li, Baigang An, Chengguo Sun","doi":"10.1016/j.ensm.2024.103953","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103953","url":null,"abstract":"Fluor-lithium salts have been found for the serious aluminum collector corrosion in lithium-ion batteries. Herein, we unexpectedly observe that adding 10 wt% fluor-lithium salts into Ni-rich cathode can lead to irreversible decay of the initial discharge capacity. The capacity loss is related to the surface phase corrosion of Ni-rich cathode materials, where the local nickel ions work as catalytic sites to induce the breakage of the C-F bond in fluor-lithium salts, promoting the decomposition of fluor-lithium salts under the driving force of external voltage exceeding 1.93 V. The formation of F<sup>−</sup> anion will attack Ni-rich cathode surface to produce nickel fluoride, resulting in the layered to rock-salt phase transformation. No corrosion behavior was found for iron, cobalt, and manganese of cathode materials. The synergistic activation by both nickel ions and voltage causes fluor-lithium salts to corrode the Ni-rich cathode materials.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"1 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mengke Peng, Chun Xue, Mengyao Yang, Fei Wang, Juan Du, Kai Yuan, Aibing Chen
{"title":"Advanced carbon materials for efficient zinc ion storage: Structures, mechanisms and prospects","authors":"Mengke Peng, Chun Xue, Mengyao Yang, Fei Wang, Juan Du, Kai Yuan, Aibing Chen","doi":"10.1016/j.ensm.2024.103945","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103945","url":null,"abstract":"Zinc ion hybrid capacitors (ZIHCs), combining the high energy density of zinc ion batteries with the high-power output of supercapacitors, are poised to become significant players in the field of electrochemical energy storage. Carbon-based materials have emerged as competitive candidates for ZIHC cathodes owing to their cost-efficiency, exceptional electronic conductivity, chemical stability, modifiable surface states, and adjustable pore structures. Recent research has been intensely focused on enhancing the energy density and cycling stability of ZIHCs through rational modification and structural optimization of carbon-based materials. This review delves into the structural design, electrochemical performance and charge storage mechanism of carbon-based cathode materials for ZIHCs via spanning a diverse range of dimensions, and the internal relations among them are explained. The challenges and opportunities facing ZIHCs are highlighted, aiming to steer the innovative development of carbon-based cathode materials and the creation of novel ZIHC technologies.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"9 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142789950","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Electrochemical-mechanical coupling failure of Ni-rich cathodes: failure mechanisms and remedying strategies","authors":"Zhouliang Tan, Feng Xu, Tianlong Wu, Xueyan Ma, Qingcui Liu, Huan Zhou, Han Zhang, Wenyi Li, Zhenjie Liu, Yingde Huang, Long Kong, Yudai Huang","doi":"10.1016/j.ensm.2024.103949","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103949","url":null,"abstract":"Ni-rich layered oxide cathodes are considered paramount cathode materials for high-energy density lithium-ion batteries because of their outstanding capacity, enhanced working potentials, and economic advantages. Nonetheless, the inherent structural and interfacial instabilities significantly degrade electrochemical performance and poses serious safety risks during repetitive delithiation/lithiation processes, particularly when the nickel content exceeds 80%. Herein, the electrochemical features and distinctive structural of advanced Ni-rich layered cathodes, as well as an exhaustive analysis of their bulk and surface failure mechanisms are summarized. Subsequently, remedying strategies to stabilize the structure/interface of Ni-rich cathode, including heteroatom doping, surface modification, concentration-gradient structure and microstructural engineering (single-crystal particle) are reviewed. Finally, outlook and perspectives aimed at encouraging the practical implementation of Ni-rich cathode materials in automotive applications are presented.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"49 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-12-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142782891","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}