Advanced Materials最新文献_第5页

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

Extracellular Matrix Topography Drives Adrenergic to Mesenchymal Transition in Neuroblastoma. 细胞外基质地形驱动神经母细胞瘤肾上腺素能向间充质转化。

IF 27.4 1区材料科学

Advanced Materials Pub Date : 2025-06-25 DOI: 10.1002/adma.202501526

Antonios Chronopoulos, Chandra Kaladhar Vemula, Vic Zamloot, Ivan Chavez, Rebekah Kennedy, Woochan Kim, Devon Bell, Yuanzhong Pan, Babak Moghimi, Jangho Kim, Shahab Asgharzadeh, JinSeok Park

{"title":"Extracellular Matrix Topography Drives Adrenergic to Mesenchymal Transition in Neuroblastoma.","authors":"Antonios Chronopoulos, Chandra Kaladhar Vemula, Vic Zamloot, Ivan Chavez, Rebekah Kennedy, Woochan Kim, Devon Bell, Yuanzhong Pan, Babak Moghimi, Jangho Kim, Shahab Asgharzadeh, JinSeok Park","doi":"10.1002/adma.202501526","DOIUrl":"https://doi.org/10.1002/adma.202501526","url":null,"abstract":"<p><p>Neuroblastoma (NB), the most common extracranial solid tumor in children, exhibits intra-tumoral heterogeneity with two interconvertible identities: adrenergic (ADRN) and mesenchymal (MES). Compared to ADRN cells, MES cells exhibit phenotypes associated with metastasis and therapy resistance. Thus, the transition from ADRN to MES may contribute to poor clinical outcomes, necessitating further investigation into this ADRN-to-MES transition (AMT) to improve clinical responses. The extracellular matrix (ECM), a critical component of the tumor microenvironment (TME), provides structural support and delivers mechanical signals that influence oncogenic processes. This research demonstrates that high-risk NB tumors contain more topographically aligned ECM fibers than low-risk NB tumors. Using nano-fabricated biomaterials designed to mimic the aligned ECM, ECM topography is revealed to drive AMT through transcriptional and epigenetic changes, accompanied by enhanced MES phenotypic features. Furthermore, ECM topography is shown to stimulate Rho-associated kinase and YAP signaling pathways, which mediate ECM-driven reprogramming. These findings introduce ECM-driven AMT as a novel mechanism in NB progression and provide insights into TME-targeted therapeutic strategies aimed at suppressing MES cells to improve clinical outcomes in NB.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":" ","pages":"e2501526"},"PeriodicalIF":27.4,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144482643","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

Unlocking the Potential of MOFs Anodes via Solid-State Corrosion Prelithiation for High-Energy Li-Ion Batteries. 通过固态腐蚀预锂化释放高能锂离子电池mof阳极的潜力。

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-06-25 DOI: 10.1002/adma.202507962

Huanhao Lei,Jinning Zuo,Jia Lu,Ziqiang Ma,Yuke Wang,Wangqi Dai,Xinyu Cheng,Huikang Xia,Zhengwen Fu

{"title":"Unlocking the Potential of MOFs Anodes via Solid-State Corrosion Prelithiation for High-Energy Li-Ion Batteries.","authors":"Huanhao Lei,Jinning Zuo,Jia Lu,Ziqiang Ma,Yuke Wang,Wangqi Dai,Xinyu Cheng,Huikang Xia,Zhengwen Fu","doi":"10.1002/adma.202507962","DOIUrl":"https://doi.org/10.1002/adma.202507962","url":null,"abstract":"Pristine metal-organic frameworks (MOFs) with their excellent cycling stability and high capacity are considered as promising next-generation anode materials for advanced high-performance lithium-ion batteries. Despite extensive efforts to improve initial Coulombic efficiency (ICE) via electrochemical prelithiation, the fundamental processes governing transition metals (TMs) dissolution and associated degradation mechanisms in MOFs-based full cells remain unclear. In this study, crystalline cobalt-nickel bimetallic metal-organic frameworks CoNix-MOF (CoNix-Benzene dicarboxylic MOFs), specifically derived from benzene dicarboxylic (BDC) ligands, are selected as the target material for investigation. A solid-state corrosion (SSC) strategy for prelithiating MOFs anodes with corrosion of lithium metal is proposed for the first time. The full cell with prelithiated MOFs anode achieves an energy density of 493 Wh kg-1 and demonstrates superior cycling stability with 83.3% capacity retention after 240 cycles at 0.2 C. The SSC prelithiation strategy effectively passivates Co/Ni nanoparticles, reducing Ni dissolution percentage by an order of magnitude (from 15.32% to 1.16%), which is identified as the key factor underpinning the enhanced full cell performance. This study underscores the practical applicability of MOFs-based anodes prelithiated by the SSC strategy for achieving high-energy-density and long-cycling lithium-ion batteries.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"39 1","pages":"e2507962"},"PeriodicalIF":29.4,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478904","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

Local Proton-Rich Solid Solution Catalyst with a Cluster-in-Cluster Structure for Anti-interference Seawater Splitting. 具有簇中簇结构的局部富质子固溶体催化剂的抗干扰海水分裂。

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-06-25 DOI: 10.1002/adma.202507080

Wenjie Shao,Zhenyu Xing,Mi Zhou,Rui Yan,Tian Ma,Bo Yin,Yi Wang,Chong Cheng,Shuang Li,Changsheng Zhao

{"title":"Local Proton-Rich Solid Solution Catalyst with a Cluster-in-Cluster Structure for Anti-interference Seawater Splitting.","authors":"Wenjie Shao,Zhenyu Xing,Mi Zhou,Rui Yan,Tian Ma,Bo Yin,Yi Wang,Chong Cheng,Shuang Li,Changsheng Zhao","doi":"10.1002/adma.202507080","DOIUrl":"https://doi.org/10.1002/adma.202507080","url":null,"abstract":"The poor proton coverage of electrocatalysts in neutral hydrogen evolution reaction (HER) and the incapacity to resist alkali hydroxides for seawater electrolysis have resulted in a large kinetics gap from acidic water splitting. Facing this challenge, a cluster-in-cluster solid solution catalyst with a proton-rich microenvironment and anti-interference interface composed of an amorphous hafnium oxide cluster penetrating in crystalline iridium cluster (HfOx-in-Ir SSC), is reported which can achieve superior activity for direct seawater splitting. The structure characterizations, in situ FT-IR and Raman, and theoretical calculations reveal that the HfOx clusters in the Ir cluster endow an interfacial proton-rich microenvironment by increasing the coverage and optimizing the adsorption of *H, thereby achieving a low overpotential of 30 mV in neutral electrolytes. Fascinating, the interfaces of HfOx-in-Ir SSC catalysts present abundant *H and OH* species and simultaneously superior anti-poison to Cl-/ClO- and anti-deposition to Mg(OH)2, eventually achieving an ultra-low overpotential of 117 mV at 10 mA cm-2 and excellent stability in seawater splitting.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"657 1","pages":"e2507080"},"PeriodicalIF":29.4,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478856","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

Ion-Framework Electrolyte Featured Zinc-Ion Transport for Solvent and Interphasial Co-Passivation. 具有锌离子传输的离子框架电解质用于溶剂和相间共钝化。

IF 29.4 1区材料科学

Advanced Materials Pub Date : 2025-06-25 DOI: 10.1002/adma.202503765

Jianze Feng,Xixian Li,Yunfa Dong,Yimou Wang,Weinan Zhao,Yuming Cui,Yuzhong Niu,Kai Liu,Zhongtao Li

{"title":"Ion-Framework Electrolyte Featured Zinc-Ion Transport for Solvent and Interphasial Co-Passivation.","authors":"Jianze Feng,Xixian Li,Yunfa Dong,Yimou Wang,Weinan Zhao,Yuming Cui,Yuzhong Niu,Kai Liu,Zhongtao Li","doi":"10.1002/adma.202503765","DOIUrl":"https://doi.org/10.1002/adma.202503765","url":null,"abstract":"The rapid application of zinc-ion (Zn2+) energy storage lacks favorable solvation structures to simultaneously form inert electrolyte environments and robust solid electrolyte interphase (SEI), which means that Zn2+ devices cannot synchronously against the side reactions, Zn dendrites and narrow electrochemical stability windows, further hindering their wide operative voltage window and ultra-long service life. Here, ion-framework electrolytes are designed by using large-sized inert-ammonium salts as the main solute. The ion framework, assembled from ultra-large solvation ion clusters containing large tetraethylammonium cations, large anions, and abundant solvents via electrostatic interactions, not only forms suitable channels for Zn2+ transport but also constrains free solvents to passivate their electrochemical activity, achieving an ultra-wide electrochemical stability window about 3.72 V. More importantly, the enrichment of the ion framework at Zn interface generates a homogenous SEI with the dense polymer-inorganic hybrid structure to passivate the interphasial chemistry, which eliminates the Zn dendrites and side reactions. Therefore, Zn anode using this electrolyte achieves the ultra-long cycling stability of 8,150 h, and Zn metal||activated carbon capacitors exhibit a high operative voltage (0-2.1 V) and ultra-long cycle life (≈170,000 cycles at 10 A g-1). This electrolyte design principle is promising for addressing the typical challenges in other metal-ion systems.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"20 1","pages":"e2503765"},"PeriodicalIF":29.4,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478898","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