Hamas Tahir, Carsten Flores-Hansen, Sheng-Ning Hsu, Zihao Liang, Jayant Naga, Neil R Dilley, Brett M Savoie, Bryan W Boudouris
{"title":"Spintronic Pathways in a Nonconjugated Radical Polymer Glass.","authors":"Hamas Tahir, Carsten Flores-Hansen, Sheng-Ning Hsu, Zihao Liang, Jayant Naga, Neil R Dilley, Brett M Savoie, Bryan W Boudouris","doi":"10.1002/adma.202406727","DOIUrl":"https://doi.org/10.1002/adma.202406727","url":null,"abstract":"<p><p>Radical chemistries have attracted burgeoning attention due to their intriguing technological applications in organic electronics, optoelectronics, and magneto-responsive systems. However, the potential of these magnetically active glassy polymers to transport spin-selective currents has not been demonstrated. Here, the spin-transport characteristics of the radical polymer poly(4-glycidyloxy-2,2,6,6-tetramethylpiperidine-1-oxyl) (PTEO) allow for sustained spin-selective currents when incorporated into typical device geometries with magnetically polarized electrodes. Annealing thin films of PTEO above its glass transition temperature results in a giant magnetoresistance effect (i.e., an MR of ≈80%) at 4 K. Additionally, ferromagnetic resonance spin-pumping results in a relatively large effective spin-mixing conductance of 1.18 × 10<sup>19</sup> m<sup>-2</sup> at the NiFe/PTEO interface. Due to the large spin-density and radical-radical exchange interactions, there is effective propagation of pure spin currents through PTEO in the NiFe/PTEO/Pd multilayer devices. This results in the transport of spin current over long distances with a spin diffusion length of 90.4 nm. The spin diffusion length and spin mixing conductance values surpass those reported in inorganic and metallic systems and are comparable to conventional doped conjugated polymers. This is the first example of spin transport in a nonconjugated radical polymer, and these findings underscore the promising spin-transporting potential of radical polymers.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2406727"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646181","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}
Tan Hu, Jin Pyo Lee, Peiwen Huang, Amanda Jiamin Ong, Jian Yu, Shuihong Zhu, Yixuan Jiang, Zhuo Zhang, Meital Reches, Pooi See Lee
{"title":"Promoting Piezoelectricity in Amino Acids by Fluorination.","authors":"Tan Hu, Jin Pyo Lee, Peiwen Huang, Amanda Jiamin Ong, Jian Yu, Shuihong Zhu, Yixuan Jiang, Zhuo Zhang, Meital Reches, Pooi See Lee","doi":"10.1002/adma.202413049","DOIUrl":"https://doi.org/10.1002/adma.202413049","url":null,"abstract":"<p><p>Bioinspired piezoelectric amino acids and peptides are attracting attention due to their designable sequences, versatile structures, low cost, and biodegradability. However, it remains a challenge to design amino acids and peptides with high piezoelectricity. Herein, a high piezoelectric amino acid by simple fluorination in its side chain is presented. The three phenylalanine derivatives are designed: Cbz-Phe, Cbz-Phe(4F), and Cbz-pentafluoro-Phe. The effect of fluorination on self-assembly and piezoelectricity is investigated. Cbz-Phe(4F) can self-assemble into crystals with a C2 space group, while Cbz-Phe and Cbz-pentafluoro-Phe form aggregated self-assemblies. Moreover, Cbz-Phe(4F) crystals exhibit a remarkably higher piezoelectric coefficient ( <math> <semantics><msubsup><mi>d</mi> <mrow><mspace></mspace> <mn>33</mn></mrow> <mrow><mspace></mspace> <mi>e</mi> <mi>f</mi> <mi>f</mi></mrow> </msubsup> <annotation>$d_{ 33}^{ eff}$</annotation></semantics> </math> ) of ≈17.9 pm V<sup>-1</sup> than Cbz-Phe and Cbz-pentafluoro-Phe. When fabricated as a piezoelectric nanogenerator, it generates an open-circuit voltage of ≈2.4 V. Importantly, Cbz-Phe(4F) crystals as a flexible piezoelectric sensor for the classification of various nuts and their quality sorting, which includes those as small as individual pumpkin seeds with high sensitivity and accuracy of sorting and quality checks. When mounted onto soft grippers, the sensor performs the tactile self-sensing functions. This work provides a promising approach to designing high piezoelectric amino acids by simple fluorination, offering exciting prospects for advancements in bioinspired piezoelectric materials in the application of smart agriculture and soft robotics.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2413049"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646160","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":"Poly(Lactic Acid): Recent Stereochemical Advances and New Materials Engineering.","authors":"Chenyang Hu, Yu Zhang, Xuan Pang, Xuesi Chen","doi":"10.1002/adma.202412185","DOIUrl":"https://doi.org/10.1002/adma.202412185","url":null,"abstract":"<p><p>Poly(lactic acid) (PLA) is a representative biobased and biodegradable aliphatic polyester and a front-runner among sustainable materials. As a semicrystalline thermoplastic, PLA exhibits excellent mechanical and physical properties, attracting considerable attention in commodity and medical fields. Stereochemistry is a key factor affecting PLA's properties, and to this end, the engineering of PLA's microstructure for tailored material properties has been an active area of research over the decade. This Review first covers the basic structural variety of PLA. A perspective on the current states of stereocontrolled synthesis as well as the relationships between the structures and properties of PLA stereosequences are included, with an emphasis on record regularity and properties. At last, state-of-the-art examples of high-performance PLA-based materials within an array of applications are given, including packaging, fibers, and textiles, healthcare and electronic devices. Among various stereo-regular sequences of PLA, poly(L-lactic acid) (PLLA) is the most prominent category and has myriad unique properties and applications. In this regard, cutting-edge applications of PLLA are mainly overviewed in this review. At the same time, new materials developed based on other PLA stereosequences are highlighted, which holds the potential to a wide variety of PLA-based sustainable materials.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2412185"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646156","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":"Design Principles for Enhancing Both Carrier Mobility and Stretchability in Polymer Semiconductors via Lewis Acid Doping.","authors":"Yu-Ching Weng, Chung-Chieh Kang, Ting-Wei Chang, Yi-Ting Tsai, Shahid Khan, Tzu-Ming Hung, Chien-Chung Shih","doi":"10.1002/adma.202411572","DOIUrl":"https://doi.org/10.1002/adma.202411572","url":null,"abstract":"<p><p>With the rise of skin-like electronics, devices are increasingly coming into close contact with the human body, creating a demand for polymer semiconductors (PSCs) that combine stretchability with reliable electrical performance. However, balancing mechanical robustness with high carrier mobility remains a challenge. To address this, tris(pentafluorophenyl)borane (BCF) for Lewis acid doping is proposed to improve charge mobility while enhancing stretchability by increasing structural disorder. Through systematic investigation, several key structural principles have been identified to maximize the effectiveness of BCF doping in stretchable PSCs. Notably, increasing the lamellar stacking distance and reducing crystallinity facilitate the incorporation of BCF into the alkyl side-chain regions, thereby enhancing both mobility and stretchability. Conversely, stronger Lewis base groups in the main chain negatively impact these improvements. These results demonstrate that with a small addition of BCF, a two-fold increase in carrier mobility is achieved while simultaneously enhancing the crack onset strain to 100%. Furthermore, doped PSCs exhibit stable mobility retention under repeated 30% strains over 1000 cycles. This method of decoupling carrier mobility from mechanical properties opens up new avenues in the search for high-mobility stretchable PSCs.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2411572"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646220","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":"Polarization: A Universal Driving Force for Energy, Environment, and Electronics.","authors":"Xinwei Guan, Zhihao Lei, Ruichang Xue, Zhixuan Li, Peng Li, Matthew David, Jiabao Yi, Baohua Jia, Hongwei Huang, Xiaoning Li, Tianyi Ma","doi":"10.1002/adma.202413525","DOIUrl":"https://doi.org/10.1002/adma.202413525","url":null,"abstract":"<p><p>The sustainable future relies on the synergistic development of energy, environmental, and electronic systems, founded on the development of functional materials by exploring their quantum mechanisms. Effective control over the distribution and behavior of charges within these materials, a basic quantum attribute, is crucial in dictating their physical, chemical, and electronic properties. At the core of charge manipulation lies \"polarization\"-a ubiquitous phenomenon marked by separating positive and negative charges. This review thoroughly examines polarization techniques, spotlighting their transformative role in catalysis, energy storage, solar cells, and electronics. Starting with the foundational mechanisms underlying various forms of polarization, including piezoelectric, ferroelectric, and pyroelectric effects, the perspective is expanded to cover any asymmetric phenomena that generate internal fields, such as heterostructures and doping. Afterward, the critical role of polarization across various applications, including charge separation, surface chemistry modification, and energy band alignment, is highlighted. Special emphasis is placed on the synergy between polarization and material properties, demonstrating how this interplay is pivotal in overcoming existing technological limitations and unlocking new functionalities. Through a comprehensive analysis, a holistic roadmap is offered for harnessing polarization across the broad spectrum of applications, thus finding sustainable solutions for future energy, environment, and electronics.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2413525"},"PeriodicalIF":27.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646250","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}
Huimin Yu, Huanyu Jin, Meijia Qiu, Yunzheng Liang, Peng Sun, Chuanqi Cheng, Pan Wu, Yida Wang, Xuan Wu, Dewei Chu, Min Zheng, Tong Qiu, Yi Lu, Bin Zhang, Wenjie Mai, Xiaofei Yang, Gary Owens, Haolan Xu
{"title":"Making Interfacial Solar Evaporation of Seawater Faster than Fresh Water","authors":"Huimin Yu, Huanyu Jin, Meijia Qiu, Yunzheng Liang, Peng Sun, Chuanqi Cheng, Pan Wu, Yida Wang, Xuan Wu, Dewei Chu, Min Zheng, Tong Qiu, Yi Lu, Bin Zhang, Wenjie Mai, Xiaofei Yang, Gary Owens, Haolan Xu","doi":"10.1002/adma.202414045","DOIUrl":"https://doi.org/10.1002/adma.202414045","url":null,"abstract":"Interfacial solar evaporation‐based seawater desalination is regarded as one of the most promising strategies to alleviate freshwater scarcity. However, the solar evaporation rate of real seawater is significantly constricted by the ubiquitous salts present in seawater. In addition to the common issue of salt accumulation on the evaporation surface during solar evaporation, strong hydration between salt ions and water molecules leads to a lower evaporation rate for real seawater compared to pure water. Here a facile and general strategy is developed to reverse this occurrence, that is, making real seawater evaporation faster than pure water. By simply introducing specific mineral materials into the floating photothermal evaporator, ion exchange at air–water interfaces directly results in a decrease in seawater evaporation enthalpy, and consequently achieves much higher seawater evaporation rates compared to pure water. This process is spontaneously realized during seawater solar evaporation. Considering the current enormous clean water production from evaporation‐based desalination plants, such an evaporation performance improvement can remarkably increase annual clean water production, benefiting millions of people worldwide.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"9 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642950","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}
He Liu, Xuemei Wei, Huagang Peng, Yi Yang, Zhen Hu, Yifan Rao, Zhefen Wang, Jianxiong Dou, Xiaonan Huang, Qiwen Hu, Li Tan, Yuting Wang, Juan Chen, Lu Liu, Yuhua Yang, Jianghong Wu, Xiaomei Hu, Shuguang Lu, Weilong Shang, Xiancai Rao
{"title":"LysSYL‐Loaded pH‐Switchable Self‐Assembling Peptide Hydrogels Promote Methicillin‐Resistant Staphylococcus Aureus Elimination and Wound Healing","authors":"He Liu, Xuemei Wei, Huagang Peng, Yi Yang, Zhen Hu, Yifan Rao, Zhefen Wang, Jianxiong Dou, Xiaonan Huang, Qiwen Hu, Li Tan, Yuting Wang, Juan Chen, Lu Liu, Yuhua Yang, Jianghong Wu, Xiaomei Hu, Shuguang Lu, Weilong Shang, Xiancai Rao","doi":"10.1002/adma.202412154","DOIUrl":"https://doi.org/10.1002/adma.202412154","url":null,"abstract":"<jats:italic>Staphylococcus aureus</jats:italic> (<jats:italic>S. aureus</jats:italic>), especially methicillin‐resistant <jats:italic>S. aureus</jats:italic> (MRSA), causes wound infections, whose treatment remains a clinical challenge. Bacterium‐infected wounds often create acidic niches with a pH 4.5–6.5. Endolysin LysSYL, which is derived from phage SYL, shows promise as an antistaphylococcal agent. However, endolysins generally exhibit instability and possess low bioavailability in acidic microenvironments. Here, an array of self‐assembling peptides is designed, and peptide L5 is screened out based on its gel formation property and bioavailability. L5 exerted a pH‐switchable antimicrobial effect (pH 5.5) and formed biocompatible hydrogels at neutral pH (pH 7.4). The LysSYL‐loaded L5 can assemble L5@LysSYL hydrogels, increase thermal stability, and exhibit the slow‐release effect of LysSYL. Effective elimination of <jats:italic>S. aureus</jats:italic> is achieved by L5@LysSYL through bacterial membrane disruption and cell separation inhibition. Moreover, L5@LysSYL hydrogels exhibit great potential in promoting wound healing in a mouse wound model infected by MRSA. Furthermore, L5@LysSYL hydrogels are safe and can decrease the cytokine levels and increase the number of key factors for vessel formation, which contribute to wound healing. Overall, the self‐assembling L5@LysSYL can effectively clean MRSA and promote wound healing, which suggests its potential as a pH‐sensitive wound dressing for the management of wound infections.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"23 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642949","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":"Fabrication of Ultrahigh‐Loading Dual Copper Sites in Nitrogen‐Doped Porous Carbons Boosting Electroreduction of CO2 to C2H4 Under Neutral Conditions","authors":"Jin‐Meng Heng, Hao‐Lin Zhu, Zhen‐Hua Zhao, Pei‐Qin Liao, Xiao‐Ming Chen","doi":"10.1002/adma.202415101","DOIUrl":"https://doi.org/10.1002/adma.202415101","url":null,"abstract":"Synthesis of high‐loading atomic‐level dispersed catalysts for highly efficient electrochemical CO<jats:sub>2</jats:sub> reduction reaction (eCO<jats:sub>2</jats:sub>RR) to ethylene (C<jats:sub>2</jats:sub>H<jats:sub>4</jats:sub>) in neutral electrolyte remain challenging tasks. To address common aggregation issues, a host‐guest strategy is employed, by using a metal‐azolate framework (MAF‐4) with nanocages as the host and a dinuclear Cu(I) complex as the guest, to form precursors for pyrolysis into a series of nitrogen‐doped porous carbons (NPCs) with varying loadings of dual copper sites, namely NPC<jats:sub>MAF‐4</jats:sub>‐Cu<jats:sub>2</jats:sub>‐21 (21.2 wt%), NPC<jats:sub>MAF‐4</jats:sub>‐Cu<jats:sub>2</jats:sub>‐11 (10.6 wt%), and NPC<jats:sub>MAF‐4</jats:sub>‐Cu<jats:sub>2</jats:sub>‐7 (6.9 wt%). Interestingly, as the loading of dual copper sites increased from 6.9 to 21.2 wt%, the partial current density for eCO<jats:sub>2</jats:sub>RR to yield C<jats:sub>2</jats:sub>H<jats:sub>4</jats:sub> also gradually increased from 38.7 to 93.6 mA cm<jats:sup>−2</jats:sup>. In a 0.1 <jats:sc>m</jats:sc> KHCO<jats:sub>3</jats:sub> electrolyte, at −1.4 V versus reversible hydrogen electrode (<jats:italic>vs</jats:italic>. RHE), NPC<jats:sub>MAF‐4</jats:sub>‐Cu<jats:sub>2</jats:sub>‐21 exhibits the excellent performance with a Faradaic efficiency of 52% and a current density of 180 mA cm<jats:sup>−2</jats:sup>. Such performance can be attributed to the presence of ultrahigh‐loading dual copper sites, which promotes C─C coupling and the formation of C<jats:sub>2</jats:sub> products. The findings demonstrate the confinement effect of MAF‐4 with nanocages is conducive to the preparation of high‐loading atomic‐level catalysts.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"52 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642840","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":"In‐Plane Chirality Control of a Charge Density Wave by Means of Shear Stress","authors":"Weiyan Qi, Stefano Ponzoni, Guénolé Huitric, Romain Grasset, Yannis Laplace, Laurent Cario, Alberto Zobelli, Marino Marsi, Evangelos Papalazarou, Alexandr Alekhin, Yann Gallais, Azzedine Bendounan, Suk Hyun Sung, Noah Schnitzer, Berit Hansen Goodge, Robert Hovden, Luca Perfetti","doi":"10.1002/adma.202410950","DOIUrl":"https://doi.org/10.1002/adma.202410950","url":null,"abstract":"The transition metal dichalcogenide 1T‐TaS<jats:sub>2</jats:sub> exhibits a Charge Density Wave (CDW) with in‐plane chirality. Due to the rich phase diagram, the Ferro‐Rotational Order (FRO) can be tuned by external stimuli. The FRO is studied by Angle‐Resolved Photoelectron Spectroscopy (ARPES), Raman spectroscopy, and Selected Area Electron Diffraction (SAED). The in‐plane chirality of the CDW is lost at the transition from Nearly‐Commensurate (NC) to In‐Commensurate (IC) phase and can be controlled by applying shear stress to the sample while cooling it through the transition from IC‐CDW to NC‐CDW. Based on these observations, a protocol is proposed to achieve reliable, non‐volatile state switching of the FRO configuration in 1T‐TaS<jats:sub>2</jats:sub> bulk crystals. These results pave the way for new functional devices in which in‐plane chirality can be set on demand.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"83 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642952","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":"Engineering Triple-Phase Interfaces with Hierarchical Carbon Nanocages for High-Areal-Capacity All-Solid-State Li-S Batteries","authors":"Yu Luo, Siyuan Pan, JingYi Tian, Yali Liang, Haoyue Zhong, Ruqin Ma, Jiabao Gu, Yuqi Wu, Huiyan Zhang, Hongxin Lin, Weilin Huang, Yuxi Deng, Yu Su, Zhengliang Gong, Jianyu Huang, Zheng Hu, Yong Yang","doi":"10.1002/adma.202413325","DOIUrl":"https://doi.org/10.1002/adma.202413325","url":null,"abstract":"All-solid-state lithium-sulfur batteries (ASSLSBs) have garnered widespread attention due to their advantages of high energy density and enhanced safety. However, the typical composite structure composed of solid-state electrolyte (SE), discrete conducting carbon black, and microsized sulfur (μ-S) with long-range Li<sup>+</sup>/e<sup>−</sup> conducting path and huge volume changes, suffers from sluggish charge transport and severe electrochemical-mechanical failure. In this work, a unique hierarchical carbon nanocage (hCNC) is applied as a continuous conducting network where nanosized sulfur are confined. Due to the synergistic effects of multi-dimensional (particle, interface, and electrode) structural engineering, this new sulfur-carbon composite cathode (S@hCNC39) can achieve uniform distribution of sulfur and carbon, and efficiently constructs triple-phase interfaces, showing enhanced charge-carrier transport and improved electrochemical-mechanical stability. Remarkable cycling performance of 89% after 300 cycles at 0.2 C at 30 °C is realized in ASSLSBs assembled with S@hCNC39. Notably, ASSLSBs achieve an ultrahigh areal capacity of 9.95 mAh cm<sup>−2</sup> with stable cycling at 60 °C with high sulfur contents of 40% and high sulfur loadings of 6 mg cm<sup>−2</sup>. These results provide critical insights into the design of rational sulfur-carbon composites and offer a viable approach to enhance the overall performance of ASSLSBs.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"128 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642944","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}