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Enhanced Electrical Interfaces in Flexible 2D Material Transistors via Liquid Metal and Ionic Liquid Injection. 通过液态金属和离子液体注入增强柔性二维材料晶体管的电接口。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202501501
Junjie Xiong,Gaotian Lu,Xinfeng Tan,Ruixiao Liu,Kaizhuo Hu,Zimu Ouyang,Yang Wei,Dan Guo
{"title":"Enhanced Electrical Interfaces in Flexible 2D Material Transistors via Liquid Metal and Ionic Liquid Injection.","authors":"Junjie Xiong,Gaotian Lu,Xinfeng Tan,Ruixiao Liu,Kaizhuo Hu,Zimu Ouyang,Yang Wei,Dan Guo","doi":"10.1002/adma.202501501","DOIUrl":"https://doi.org/10.1002/adma.202501501","url":null,"abstract":"Contact engineering at the semiconductor-electrode and semiconductor-dielectric interfaces is critical to the performance of electronic devices, especially for delicate 2D semiconductors. Here, this study proposes a new paradigm of flexible field-effect transistors featuring solid-liquid hybrid interfaces, in which liquid metal and ionic liquid, confined within microchannels, function as the source/drain electrodes and gate dielectric, respectively. These interfaces provide MoS₂ with undisturbed, atomically smooth electrical contacts, and enable efficient gate control via electric double layers. Benefiting from the inherent softness of liquids and their damage-free processing, Fermi level pinning is significantly mitigated by the liquid metal, achieving a pinning factor |s| = 0.7. Meanwhile, the ionic liquid enables a subthreshold swing of 60.7 mV dec-1, approaching the theoretical thermal limit. Furthermore, our flexible transistors demonstrate multifunctionality as enhanced logic gates, low-voltage inverters, and ultra-high-linearity synaptic devices. This work underscores the promise of liquid-enabled contact strategies for advancing low-power, flexible electronics and soft robotic systems.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"63 1","pages":"e2501501"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488203","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}
引用次数: 0
Semiconducting Pt Structures Stabilized on 2D MoS2 Crystals Enable Ultrafast Hydrogen Evolution. 在二维MoS2晶体上稳定的半导体Pt结构实现了超快析氢。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202504113
Tamás Ollár,Péter Vancsó,Péter Kun,Antal A Koós,Gergely Dobrik,Ekaterina V Sukhanova,Zakhar I Popov,Miklós Németh,Krisztina Frey,Béla Pécz,Péter Nemes-Incze,Chanyong Hwang,József Sándor Pap,Levente Tapasztó
{"title":"Semiconducting Pt Structures Stabilized on 2D MoS2 Crystals Enable Ultrafast Hydrogen Evolution.","authors":"Tamás Ollár,Péter Vancsó,Péter Kun,Antal A Koós,Gergely Dobrik,Ekaterina V Sukhanova,Zakhar I Popov,Miklós Németh,Krisztina Frey,Béla Pécz,Péter Nemes-Incze,Chanyong Hwang,József Sándor Pap,Levente Tapasztó","doi":"10.1002/adma.202504113","DOIUrl":"https://doi.org/10.1002/adma.202504113","url":null,"abstract":"Metallic platinum is the best and most widely investigated catalyst for hydrogen evolution, yet little is known about Pt in its semiconducting form. Here, it is shown that semiconducting Pt structures with a thickness of only two atomic layers (0.4 nm) can be stabilized on 2D MoS2 crystals. Reducing the thickness of Pt particles below the Fermi wavelength (0.5 nm) opens a sizeable (0.3-0.4 eV) gap in their electronic structure. The resulting electronic structure is qualitatively different from both the metallic bands of larger Pt nanoparticles and the atomic orbitals of Pt single atom catalysts while displaying the highest intrinsic activity among them. Semiconducting Pt bilayers enable H2 production at ten times higher rates (≈1400 H2 s-1 @ η = 100 mV) than Pt single atom catalysts, and match the activity of commercial Pt nanoparticles (Pt /C catalysts) at three orders of magnitude lower Pt loadings.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"17 1","pages":"e2504113"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488200","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}
引用次数: 0
Reversible Phase Transitions of Anionic and Cationic Surfactant Mixtures Drive Shape Morphing Droplets. 阴离子和阳离子表面活性剂混合物的可逆相变驱动形状变形液滴。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202506100
Bradley D Frank,Pilar Romero,Alberto Concellón,Lukas Zeininger
{"title":"Reversible Phase Transitions of Anionic and Cationic Surfactant Mixtures Drive Shape Morphing Droplets.","authors":"Bradley D Frank,Pilar Romero,Alberto Concellón,Lukas Zeininger","doi":"10.1002/adma.202506100","DOIUrl":"https://doi.org/10.1002/adma.202506100","url":null,"abstract":"Converting chemical signals into mechanical responses is fundamental to biological systems, driving processes such as cellular motility and tissue morphogenesis. Yet, harnessing chemo-mechanical signal conversions in synthetic systems remains a key challenge in energy-dissipative materials design. While droplets can move and interact with their environment reminiscent of active biological matter, chemo-mechanical interactions are limited by the translation of chemical changes into extensive force variations required on small timescales. Droplets naturally adopt spherical shapes to minimize surface-energy and restructuring liquids into non-equilibrium geometries requires mechanisms beyond current stimuli-responsive surfactant systems, which lack the force-amplifying mechanisms needed for transient liquid structuring. Here, a spring-like charging and latch-controlled release mechanism is introduced for actuating droplets. This is based on reversible, light-induced crystal-to-coacervate phase transitions of photo-responsive surfactant assemblies, namely between anionic sodium dodecylsulfate and cationic azobenzene-based surfactants. During phase-transition, reversible partitioning of the surfactants into the oil or aqueous phases of the emulsion transiently induce rapid changes in interfacial tensions, which are up to 900 times greater than those observed for conventional stimuli-responsive surfactant systems. The insights into this novel chemo-mechanical transduction mechanism provide new control over purely liquid systems, paving the way for programmable, hierarchically structured, all-liquid matter acting with physicality.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"54 1","pages":"e2506100"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488202","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}
引用次数: 0
A Non-Concentrated Gradient-Solvation Electrolyte Enables a High-Voltage Lithium Metal Battery with 447.6 Wh Kg-1. 一种非浓缩梯度溶剂化电解液实现了447.6 Wh Kg-1的高压锂金属电池。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202509760
Hao Wang,Dong Yan,Hongyu Liu,Shuai Li,Xiaobin Niu,Chuying Ouyang,Hong Li,Liping Wang
{"title":"A Non-Concentrated Gradient-Solvation Electrolyte Enables a High-Voltage Lithium Metal Battery with 447.6 Wh Kg-1.","authors":"Hao Wang,Dong Yan,Hongyu Liu,Shuai Li,Xiaobin Niu,Chuying Ouyang,Hong Li,Liping Wang","doi":"10.1002/adma.202509760","DOIUrl":"https://doi.org/10.1002/adma.202509760","url":null,"abstract":"High-voltage lithium (Li) metal batteries (LMBs) emerge as a pivotal strategy for achieving high energy density applications. However, the electrolyte instability leading to inferior rate performance and short lifespan remains to be addressed. In this study, a new non-concentrated gradient-solvation electrolyte by solvent polarity discrepancy is developed. A highly donor-capable ether forms the Li⁺-solvated core through strong ion-dipole interactions, while a weakly donating carbonate creates the shell structure. Such a gradient-solvation structure enables the electrolyte with a high oxidation voltage (4.6 V vs. Li/Li+) and rapid Li+-desolvated kinetic. Consequently, the electrolyte facilitates the LiNi0.8Co0.1Mn0.1O2 (NCM811)||Li cells to attain a specific capacity of 165.8 mAh g-1 at 5C, alongside 1000 stable cycles at 1C charge/3C discharge with 66% capacity retention. Even under lean conditions (N/P = 1.5, electrolyte: 20 µL), NCM811||Li cell still maintains 97.5% capacity retention over 100 cycles. Furthermore, a 3.2 Ah pouch cell achieves a specific energy density of 447.6 Wh kg-¹ with stable cycling. These findings highlight the promise of gradient-solvation electrolytes for high-voltage LMBs applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"26 1","pages":"e2509760"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488201","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}
引用次数: 0
Inflammation-Activatable Nanoscavengers for Sustainable Cell-Free DNA Capture and Cleavage. 可炎症激活的纳米复合物用于可持续的无细胞DNA捕获和切割。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202504557
Mengyuan Yin,Chenglong Ge,Yang Zhou,Renxiang Zhou,Yiyao Yang,Yu Qian,Jianyin He,Jingrui Shen,Lichen Yin
{"title":"Inflammation-Activatable Nanoscavengers for Sustainable Cell-Free DNA Capture and Cleavage.","authors":"Mengyuan Yin,Chenglong Ge,Yang Zhou,Renxiang Zhou,Yiyao Yang,Yu Qian,Jianyin He,Jingrui Shen,Lichen Yin","doi":"10.1002/adma.202504557","DOIUrl":"https://doi.org/10.1002/adma.202504557","url":null,"abstract":"Cell-free DNA (cfDNA) scavenging using cationic materials represents a promising therapeutic modality for autoimmune diseases (AIDs) such as inflammatory bowel disease (IBD). This approach, however, suffers from critical issues of binding saturation for cfDNA and risk of re-exposure of the captured cfDNA. Herein, an inflammation-activatable nanoscavenger integrating both cfDNA capture and cleavage functions is constructed from dendrimer-templated, charge- and conformation-transformable polypeptides with Cyclen-Zn complexes conjugated on the backbone termini. At neutral pH, the polypeptides containing both cis-aconitic acid and guanidine side chains adopt negative charges and random-coiled conformation, thus featuring long blood circulation and high accumulation to the inflamed intestinal tissue. Inside the mildly acidic inflammatory microenvironment, the polypeptides transform to the positively charged α-helices due to removal of the cis-aconitic acid groups, thus enabling robust cfDNA capture through electrostatic attraction, salt bridging, and spatial confinement within the cavity between adjacent rod-like helices. Subsequently, the exposed Cyclen-Zn endows the nanoscavenger with DNase-like activity to cleave the captured cfDNA, allowing sustainable cfDNA capture and scavenging. In consequence, the nanoscavenger efficiently inhibits TLR9 activation and restores immune homeostasis in IBD mice. This study proposes an enlightened strategy for sustainable cfDNA scavenging, and it renders a promising modality for AIDs treatment.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"9 1","pages":"e2504557"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488197","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}
引用次数: 0
Immobilization of H2O in Diffusion Channel of Metal-Organic Frameworks for Long-Term CO2 Capture from Humid Flue Gas. 金属-有机骨架扩散通道中水的固定化对湿烟气中CO2的长期捕集
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202410500
Yang Chen,Kaihua Wang,Jing-Hong Li,Yi Wang,Rui-Biao Lin,Xiao-Ming Chen,Jinping Li,Libo Li
{"title":"Immobilization of H2O in Diffusion Channel of Metal-Organic Frameworks for Long-Term CO2 Capture from Humid Flue Gas.","authors":"Yang Chen,Kaihua Wang,Jing-Hong Li,Yi Wang,Rui-Biao Lin,Xiao-Ming Chen,Jinping Li,Libo Li","doi":"10.1002/adma.202410500","DOIUrl":"https://doi.org/10.1002/adma.202410500","url":null,"abstract":"Utilizing physisorption for CO2 capture in humid flue gas presents challenges, with H2O molecules either damaging the adsorbent or competing with CO2 for adsorption, compromising long-term stability. Herein, a counter-intuitive strategy is proposed to address this issue by immobilizing H2O into metal-organic framework (TYUT-ATZ, TYUT = Taiyuan University of Technology, ATZ = 3-amino-1,2,4-triazole) as binding sites for CO2 capture from humid airflow. Through tailoring the -NH2 group numbers and pore sizes creates ingenious H2O sites, preserving CO2 adsorption space and enhancing CO2 adsorption interactions in 1D channels. The well-constructed TYUT-ATZ-β demonstrates a high CO2 adsorption capacity (62.7 cm3 cm-3) at 0.15 bar and outstanding CO2/N2 (15/85) selectivity (2031) at 298 K, while also exhibits the highest CO2/H2O uptake ratio in humid flue gas due to its excellent water stability and unique H2O site. Consequently, it shows top-performing CO2 enrichment ability with easy regeneration in long-term separation experiments (over 100 cycles) under high-humidity (75% RH). Gas adsorption isotherms, single-crystal analysis, selectivity calculations, and contrastive breakthrough experiments comprehensively validate this artful H2O immobilization strategy in MOFs for efficient CO2 capture in humid flue gas, satisfying the application requirements of high selectivity, rapid regeneration, and long-term stability.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"39 1","pages":"e2410500"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488204","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}
引用次数: 0
Halogen Ion-Mediated Hydrothermal Synthesis of Diverse MXenes with Tailored Heterostructures. 卤素离子介导的水热合成具有定制异质结构的多种MXenes。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202504586
Hanchen Xu,Hongwei Shou,Ziwei Yan,Kefu Zhu,Chuanqiang Wu,Wei Jiang,Zhanfeng Liu,Shiqiang Wei,Jialin Shi,Hassan Akhtar,Changda Wang,Li Song
{"title":"Halogen Ion-Mediated Hydrothermal Synthesis of Diverse MXenes with Tailored Heterostructures.","authors":"Hanchen Xu,Hongwei Shou,Ziwei Yan,Kefu Zhu,Chuanqiang Wu,Wei Jiang,Zhanfeng Liu,Shiqiang Wei,Jialin Shi,Hassan Akhtar,Changda Wang,Li Song","doi":"10.1002/adma.202504586","DOIUrl":"https://doi.org/10.1002/adma.202504586","url":null,"abstract":"Two-dimensional transition metal carbides and nitrides (MXenes) have attracted significant attention due to their exceptional physicochemical properties. Despite extensive studies, efficient methods for the production of MXenes with precise structural control still remain a challenge, thus hindering their potential in many specific applications. Herein, a halogen ion-mediated hydrothermal approach is proposed for the controllable preparation of diverse MXenes and their heterostructures with well-defined interfacial architectures, demonstrating its potential as a high-throughput synthesis strategy. As proof of concept, Mo2C can be synthesized on a gram scale by employing NH₄F in the hydrothermal etching process of Mo2Ga2C. Subsequently, this approach is applied to various MXenes, including Ti3C2, V2C, and Nb4C3. Moreover, NH4X (X = Cl, Br, I) etchants combined with small-molecule intercalants enabled the targeted synthesis of MXene-based heterostructures, such as Mo2CTx@MoS2 featuring ≈15 nm amorphous MoS2 surface layers. Notable, the Mo2CTx(Br) heterostructure exhibited outstanding electrochemical stability, delivering a capacity of 465.5 mAh g⁻¹ after 300 cycles at 1 A g⁻¹, and achieving high coulombic efficiency of 99.8% during lithium-ion battery cycling. This work establishes a versatile and scalable platform for the synthesis of MXene-based materials, thus paving the way for accelerating their potential in various fields.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"141 1","pages":"e2504586"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488198","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}
引用次数: 0
Spin-polarized Acidic Water Electrolysis with Antenna-Reactor Plasmonic Electrocatalysts. 天线反应器等离子体电催化剂的自旋极化酸性电解。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-26 DOI: 10.1002/adma.202507658
Kyunghee Chae,Heejun Lee,Wen-Tse Huang,Jaehyun Son,Bertrand Pavageau,Tae-Hyun Kim,Seung-Eun Lee,Jeongwon Kim,Jooho Moon,Ru-Shi Liu,Joonho Bang,Dong Ha Kim
{"title":"Spin-polarized Acidic Water Electrolysis with Antenna-Reactor Plasmonic Electrocatalysts.","authors":"Kyunghee Chae,Heejun Lee,Wen-Tse Huang,Jaehyun Son,Bertrand Pavageau,Tae-Hyun Kim,Seung-Eun Lee,Jeongwon Kim,Jooho Moon,Ru-Shi Liu,Joonho Bang,Dong Ha Kim","doi":"10.1002/adma.202507658","DOIUrl":"https://doi.org/10.1002/adma.202507658","url":null,"abstract":"Water electrolysis, driven by renewable electricity, offers a sustainable path for hydrogen production. However, efficient bifunctional electrocatalysts are needed to overcome the high overpotentials of both the oxygen evolution reaction and hydrogen evolution reaction. To address this, a novel catalyst system is developed integrating plasmonic nanoreactors with chirality-induced spin selectivity. In this system, chiral Au nanoparticles act as antennae, while single-atom iridium serves as the catalytic reactor, achieving a 3.5 fold increase in reaction kinetics (at 1.57 V vs RHE) compared to commercial IrO2 catalysts and enhancing durability by over 4.8 times relative to conventional Pt/C || IrO2 systems. Density functional theory and operando X-ray absorption spectroscopy reveal that plasmon-driven spin alignment polarizes the Ir atom, significantly enhancing stability (>480 h at 100 mA cm-2) under acidic conditions. This work represents a major advance in spin polarization for plasmonic electrocatalysis, offering a new route to sustainable energy solutions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"46 1","pages":"e2507658"},"PeriodicalIF":29.4,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144488199","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}
引用次数: 0
Fukui Function-Engineered Gel Electrolytes: Thermodynamic/Kinetic-Synergistic Regulation for Long-Cycling Zinc Metal Batteries. 福井功能工程凝胶电解质:长循环锌金属电池的热力学/动力学协同调节。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-25 DOI: 10.1002/adma.202508722
Yiwen Zhang,Hao Zhuo,Peixian Lei,Dajiang Tang,Qiang Hu,Xiaoyang Du,Cai-Jun Zheng,Jia-Lin Yang,Zhen-Yi Gu,Jingxin Zhao,Silu Tao,Xing-Long Wu
{"title":"Fukui Function-Engineered Gel Electrolytes: Thermodynamic/Kinetic-Synergistic Regulation for Long-Cycling Zinc Metal Batteries.","authors":"Yiwen Zhang,Hao Zhuo,Peixian Lei,Dajiang Tang,Qiang Hu,Xiaoyang Du,Cai-Jun Zheng,Jia-Lin Yang,Zhen-Yi Gu,Jingxin Zhao,Silu Tao,Xing-Long Wu","doi":"10.1002/adma.202508722","DOIUrl":"https://doi.org/10.1002/adma.202508722","url":null,"abstract":"While traditional gel electrolytes address critical issues such as electrolyte leakage and dendrite growth in zinc metal batteries (ZMBs), their intrinsic inability to suppress the competing hydrogen evolution reaction (HER) remains a fundamental limitation. Herein, a Fukui function-guided molecular engineering approach is proposed to develop a gel electrolyte (HG-3TP) with higher Gibbs free energy of HER (ΔGHER). The reduced electrophilic Fukui function inhibits Zn electron extraction while participating in Zn2⁺ solvation to decrease free water activity. Simultaneously, attenuated nucleophilic Fukui function creates an inert barrier on Zn anodes, raising H⁺ desorption energy and lowering proton diffusion. These synergistic effects suppress the Volmer/Heyrovsky step, significantly increasing ΔGHER and inhibiting HER. Meanwhile, optimized interfacial energetics facilitate uniform Zn plating/stripping while maintaining cathode compatibility. As a result, Zn batteries with HG-3TP exhibit excellent long-term cycling stability, achieving 4,000 h in Zn||Zn symmetric cells and maintaining operation for 710 h at 60 °C, while demonstrating 83.5% capacity retention over 11 000 cycles in Zn||VO2 full cells. This work establishes a thermodynamics-kinetics orchestrated paradigm through Fukui function-guided electrolyte design, advancing ultrastable ZMBs for scalable energy storage.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"248 1","pages":"e2508722"},"PeriodicalIF":29.4,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478903","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}
引用次数: 0
Unraveling the Impact of Electrosorbed Ions on the Scaling Behavior of Fast-Charging Dynamics of Nanoporous Electrodes Toward Digital Design of Iontronic Devices. 揭示电吸附离子对纳米孔电极快速充电动力学尺度行为的影响,面向电子器件的数字化设计。
IF 29.4 1区 材料科学
Advanced Materials Pub Date : 2025-06-25 DOI: 10.1002/adma.202506177
Jinsha Liao,Peiyao Wang,Wen-Jie Jiang,Xiaoyang Du,Jefferson Zhe Liu,Dan Li
{"title":"Unraveling the Impact of Electrosorbed Ions on the Scaling Behavior of Fast-Charging Dynamics of Nanoporous Electrodes Toward Digital Design of Iontronic Devices.","authors":"Jinsha Liao,Peiyao Wang,Wen-Jie Jiang,Xiaoyang Du,Jefferson Zhe Liu,Dan Li","doi":"10.1002/adma.202506177","DOIUrl":"https://doi.org/10.1002/adma.202506177","url":null,"abstract":"Electrolyte-filled nanoporous electrodes with fast-charging capability are critical for advanced energy storage and iontronic devices. However, experiments and simulations consistently show that increasing electrode thickness degrades performance by limiting ion access to effective electrode/electrolyte interfaces, especially under fast-charging conditions. While often attributed to sluggish ion transport, the underlying mechanisms and the quantitative link between thickness and performance remain unclear due to complex pore structures and nanoconfined ion dynamics. Here, using multilayered graphene membranes as a model system, modified Poisson-Nernst-Planck simulations with experiments are combined to reveal how electrosorbed ions reshape local electrical and chemical potentials, particularly as the surface-to-volume ratio increases with reduced pore size. It is shown that electrosorbed ions substantially influence the scaling behavior of capacitance across electrode thicknesses, causing marked deviations from classical transmission line models as pores approach nanometric dimensions. Despite the complexity introduced by nanoconfinement, introducing a correction factor enables capacitance-scan rate relationships to collapse into a unified curve across various electrode architectures, allowing computationally efficient design of high-performance fast-charging electrochemical and iontronic devices. This work highlights the unique role of 2D nanomaterials as a versatile platform for bridging experiments and theory to address long-standing challenges in ion transport dynamics.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"13 1","pages":"e2506177"},"PeriodicalIF":29.4,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478905","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}
引用次数: 0
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