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Bone-Penetrating Copper-Coordinated Nanoassembly Elicits Cuproptosis for Multimodal Cancer Therapy 骨穿透铜协同纳米组装引发多模式癌症治疗的铜分化
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c25793
Ding Tan, Yan Sun, Xudong Li, Ya Wang, Xianbin Sun, Haijun Chen, Yuxiang Lin, Yu Gao
Copper-based nanotherapeutics have emerged as a promising anticancer platform by simultaneously inducing cuproptosis and enabling multimodal therapy. However, their clinical application remains constrained by uncontrolled copper ion release, a complex tumor microenvironment (TME), and insufficient therapeutic penetration. To address these challenges, we developed a multifunctional nanoplatform (BCB) through the integration of baicalein–copper coordinated nanoparticles with a boron-dipyrromethene-derived photosensitizer. BCB exhibited a uniform spherical morphology with an average size of approximately 150 nm, excellent stability, TME-responsive release, and multiple catalytic functions, including peroxidase-like and photodynamic activities. Through synergistic chemodynamic and phototherapeutic actions, BCB effectively depleted glutathione, generated abundant reactive oxygen species, disrupted mitochondrial membrane potential, and triggered cuproptosis. In murine melanoma models, BCB plus light irradiation achieved a 75% cure rate, even at low doses. Moreover, BCB exhibited antimigratory properties and bone-penetrating capability, with selective accumulation in intramedullary tumor sites, highlighting its potential for treating bone-metastatic cancers. This multimodal nanoplatform represents a promising synergistic strategy for overcoming current therapeutic limitations in both primary and metastatic tumors.
铜基纳米疗法已成为一个有前途的抗癌平台,同时诱导铜沉积和实现多模式治疗。然而,它们的临床应用仍然受到铜离子释放不受控制、复杂的肿瘤微环境(TME)和治疗渗透不足的限制。为了解决这些问题,我们开发了一种多功能纳米平台(BCB),将黄芩素-铜配位纳米颗粒与硼-二吡咯烯衍生的光敏剂集成在一起。BCB具有均匀的球形形貌,平均尺寸约为150 nm,稳定性好,tme响应释放,具有多种催化功能,包括过氧化物酶和光动力活性。BCB通过化学动力学和光治疗作用的协同作用,有效地消耗谷胱甘肽,产生丰富的活性氧,破坏线粒体膜电位,引发铜变形。在小鼠黑色素瘤模型中,BCB加光照射即使在低剂量下也能达到75%的治愈率。此外,BCB具有抗迁移特性和穿骨能力,在髓内肿瘤部位选择性积累,突出了其治疗骨转移癌的潜力。这种多模态纳米平台代表了一种有希望的协同策略,可以克服目前原发性和转移性肿瘤的治疗局限性。
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引用次数: 0
A High-Strength Phase-Separated Underwater Adhesive with Self-Reinforcement in Dynamic Water. 一种高强度动态水中自增强相分离水下胶粘剂。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c24454
Weicheng Gao, Qianyu Wei, Yaning Wei, Leyun Peng, Lixia Long, Xin Hou, Sidi Li, Jin Zhao, Xubo Yuan

Adhesives with excellent adhesion properties are crucial for aquatic activities. However, natural dynamic water can lead to the loss of adhesive molecules and a reduction in adhesion strength. In this work, we propose a unique phase-separated underwater adhesive through the copolymerization of hydrophilic and hydrophobic monomers. The hydrophobic groups repel interfacial water, while the hydrophilic groups form strong bonds with substrates, endowing the adhesive with outstanding adhesion. Moreover, the adhesive exhibits unique self-reinforcing properties in dynamic water. The self-reinforcement is realized through dynamic water-accelerated phase separation kinetics of the adhesive. The dynamic water forms a dense surface of adhesive, reducing adhesive loss and increasing the bonding area. The adhesion strength in dynamic water significantly increases, reaching 1.97-fold of that in static water. In addition, the adhesive demonstrates excellent adaptability and maintains strong adhesion in various water environments. Benefiting from its linear structure and good solubility, the adhesive exhibits recyclability and erasability, which promotes sustainable chemistry and utility. The recycled adhesive retains 95% of its original adhesive strength without obvious damage. The adhesive demonstrates practicality and accessibility in applications such as tube repair and leakage sealing. Overall, this work provides insights into the design and preparation of novel self-reinforcing underwater adhesives.

具有优异粘附性能的胶粘剂对水生活动至关重要。然而,天然的动态水会导致粘接分子的损失和粘接强度的降低。在这项工作中,我们提出了一种独特的相分离水下粘合剂,通过亲水性和疏水性单体共聚。疏水基团排斥界面水,而亲水基团与底物形成牢固的键,使粘合剂具有出色的附着力。此外,该胶粘剂在动态水中表现出独特的自增强性能。胶粘剂的自增强是通过动态水加速相分离动力学实现的。动态水形成致密的胶粘剂表面,减少了胶粘剂损失,增加了粘接面积。在动水中黏附强度显著提高,达到静水中的1.97倍。此外,该胶粘剂具有优异的适应性,在各种水环境中都能保持较强的附着力。由于其线性结构和良好的溶解性,该胶粘剂具有可回收性和可擦除性,促进了可持续化学和实用。回收后的胶粘剂保持原有粘接强度的95%,无明显损伤。该粘合剂在管道修复和泄漏密封等应用中具有实用性和可及性。总的来说,这项工作为新型自增强水下粘合剂的设计和制备提供了见解。
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引用次数: 0
Acoustic-Driven Enhancement of Photocarrier Separation in a Reconfigurable WSe2 Homojunction. 可重构WSe2同质结中光载流子分离的声驱动增强。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c24273
Xuan Deng, Chao Dou, Yan Wang, Haoyue Lu, Ruoyao Sun, Yueying Li, Jing Liu

Two-dimensional transition-metal dichalcogenide (TMD) homojunctions are promising for optoelectronic applications but are fundamentally limited by inefficient carrier separation, even under reverse bias. Here, we introduce surface acoustic wave (SAW) technology as an efficient means to enhance photocarrier dissociation via strain-mediated electron-phonon interactions. To experimentally validate this approach, we constructed a hybrid acoustooptic platform by integrating a LiNbO3 substrate with interdigitated transducers onto a SiO2/Si chip. A reconfigurable WSe2 homojunction─fabricated on an hexagonal boron nitride (h-BN) intermediate layer and dynamically tunable via UV-assisted doping to form junctions with tailored built-in potentials─served as the functional device. Under SAW excitation propagating from LiNbO3 into the device stack, the homojunction exhibits a 30% photocurrent enhancement at 550 nm illumination, outperforming conventional reverse-bias operation at nearly an order-of-magnitude lower voltage, while maintaining a rectification ratio of >103 and negligible dark-current variation. Mechanistic studies reveal that the SAW induces a type-I band modulation in the nonpiezoelectric heterostructure, creating energy barriers that suppress recombination and substantially improve electron-hole separation. This work demonstrates SAW as an effective strategy for enhancing the optoelectronic performance in homojunctions and provides a scalable platform for acoustooptic applications in nonpiezoelectric low-dimensional systems.

二维过渡金属二硫化物(TMD)同质结在光电应用中很有前景,但从根本上受到低效载流子分离的限制,即使在反向偏压下也是如此。在这里,我们介绍了表面声波(SAW)技术作为一种有效的手段,通过应变介导的电子-声子相互作用来增强光载流子的解离。为了实验验证这种方法,我们将LiNbO3衬底与交叉换能器集成到SiO2/Si芯片上,构建了一个混合声光平台。在六方氮化硼(h-BN)中间层上制备了一种可重构的WSe2同质结,并可通过紫外光辅助掺杂进行动态调整,形成具有定制内置电位的结,这是一种功能器件。在从LiNbO3传播到器件堆叠的SAW激发下,在550 nm照明下,同结显示出30%的光电流增强,在几乎低一个数量级的电压下优于传统的反向偏置操作,同时保持bbb103的整流比和可忽略的暗电流变化。机理研究表明,SAW在非压电异质结构中诱导i型带调制,产生抑制复合的能量势垒,并显著改善电子-空穴分离。这项工作证明了声表面波是提高同质结光电性能的有效策略,并为非压电低维系统中的声光应用提供了一个可扩展的平台。
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引用次数: 0
In-Situ CuNPs Reduction on MXene for High-Thermal-Conductivity Composite Films with Exceptional EMI Shielding and Photothermal Conversion. 具有优异EMI屏蔽和光热转换的高导热复合薄膜在MXene上的原位CuNPs还原。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c25592
Xianjin Yang, Enxiang Jiao, Xuehai Zhang, Ke Zhang, Anbang Sun, Yanwei Zhao, Huimin Wang, Zheng Cao, Peng Lv, Haijun Zhang, Hongwang Shen, Fulai Zhao

The rapid advancement of 5G communication technology necessitates enhanced performance in electromagnetic interference (EMI) shielding and thermal management materials. We fabricated multifunctional nacre-like MXene@CuNPs(MSC)composite films via intermittent filtration and in situ reduction. The resulting composite film exhibited a high in-plane thermal conductivity of 47.6 W m-1 K-1 and demonstrated superior thermal management capability in heat dissipation tests. Containing 3.1 wt % Cu and with a thickness of 0.04 mm, the film achieved an average EMI shielding effectiveness (SE) of 64 dB within the X-band (8.2-12.4 GHz). Calculations based on the effective medium theory (EMT) elucidated the critical role of Cu nanoparticles (CuNPs) in establishing an efficient thermal conduction network. Owing to the CuNPs acting as thermal bridges, the interfacial thermal resistance within the composite film decreased by 35.6%. Furthermore, the MSC composite films exhibited rapid-response photothermal behavior. Upon irradiation with a light power density of 200 mW cm-2, the surface temperature of the MSC3.1 film rapidly reached 101 °C. The outstanding performance of this composite film underscores the broad application potential of Cu-modified MXene in electronic devices and related fields.

5G通信技术的快速发展需要提高电磁干扰(EMI)屏蔽和热管理材料的性能。我们通过间歇过滤和原位还原法制备了多功能纳米样MXene@CuNPs(MSC)复合膜。所制备的复合薄膜具有47.6 W m-1 K-1的高面内导热系数,在散热测试中表现出优异的热管理能力。该薄膜含有3.1 wt %的Cu,厚度为0.04 mm,在x波段(8.2-12.4 GHz)内实现了64 dB的平均EMI屏蔽效能(SE)。基于有效介质理论(EMT)的计算阐明了Cu纳米颗粒(CuNPs)在建立高效热传导网络中的关键作用。由于CuNPs的热桥作用,复合膜内的界面热阻降低了35.6%。此外,MSC复合膜表现出快速响应的光热行为。当光功率密度为200 mW cm-2时,MSC3.1薄膜的表面温度迅速达到101℃。该复合膜的优异性能凸显了cu修饰MXene在电子器件及相关领域的广泛应用潜力。
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引用次数: 0
Leveraging 3D Printing-Induced Spherulitic Topographical and Biochemical Cues on Polyether Ether Ketone/Hydroxyapatite/Magnesium Orthosilicate Composites for Orthopedic Applications 利用3D打印诱导的聚醚醚酮/羟基磷灰石/正硅酸镁复合材料的球形地形和生化线索用于骨科应用
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c22456
Praveen Jeyachandran, Lionel Yan Jin Lee, Si Jian Hui, Balamurugan Vellayappan, Jerry Ying Hsi Fuh, James Thomas Patrick Decourcy Hallinan, A. Senthil Kumar, Naresh Kumar
A prime focus in orthopedic research is to promote osseointegration, while improving the functionality of implantable biomaterials. Surface topographic features have been shown to influence cell–biomaterial interactions, thereby facilitating cell adhesion, proliferation, and growth. However, a key challenge lies in inducing such topographical cues through existing biofabrication technologies. This study presents a newer strategy to leverage existing 3D printing (3DP) technology, promoting topographical cues manifested as microscopic spherulitic crystals integrated with nanoscopic lamellas on printed surfaces. Poly ether–ether–ketone (PEEK) composites reinforced with hydroxyapatite (HAp) and magnesium orthosilicate (Mg2SiO4) are printed using droplet-based 3D printing (3DP) technology, wherein the printing parameters are tailored to induce a network of spherulitic topographical cues in conjunction with biochemical cues arising from exposed bioactive fillers. Human osteosarcoma (Saos-2) cells are used to investigate the synergistic influence of the topographical and biochemical cues on the cell–material biological interactions. The composites exhibit hydrophilic surfaces with enhanced surface energy, promoting cellular adhesion and the formation of numerous filopodia, indicating an active engagement with spherulitic topographies. Composite surfaces featuring spherulitic topographical and biochemical cues foster a conducive environment, augmenting the cytocompatibility and osteogenic capabilities. Furthermore, process optimization not only improves the mechanical performance of the composites but also enhances their damping capabilities, a critical attribute for implant applications. This approach demonstrates that engineered spherulitic-topographical cues, in conjunction with biochemical cues, can mimic lamellar bone morphology, yielding improved biological and dynamic mechanical responses and highlighting their potential for personalized orthopedic implant applications.
骨科研究的主要焦点是促进骨整合,同时提高可植入生物材料的功能。表面地形特征已被证明影响细胞-生物材料的相互作用,从而促进细胞粘附、增殖和生长。然而,一个关键的挑战在于通过现有的生物制造技术诱导这种地形线索。本研究提出了一种利用现有3D打印(3DP)技术的新策略,促进了在打印表面上表现为微观球晶与纳米片集成的地形线索。采用基于液滴的3D打印(3DP)技术打印羟基磷灰石(HAp)和正硅酸镁(Mg2SiO4)增强的聚醚醚酮(PEEK)复合材料,其中打印参数可定制,以诱导球形地形线索网络,并结合暴露的生物活性填料产生的生化线索。人类骨肉瘤(Saos-2)细胞被用来研究地形和生化线索对细胞-物质生物相互作用的协同影响。复合材料表现出具有增强表面能的亲水性表面,促进细胞粘附和大量丝状足的形成,表明其与球型地形积极参与。具有球形地形和生化特征的复合表面营造了有利的环境,增强了细胞相容性和成骨能力。此外,工艺优化不仅提高了复合材料的机械性能,还提高了它们的阻尼能力,这是植入应用的关键属性。该方法表明,工程球型地形线索与生化线索相结合,可以模拟板层骨形态,产生更好的生物和动态力学反应,并突出了它们在个性化骨科植入物应用中的潜力。
{"title":"Leveraging 3D Printing-Induced Spherulitic Topographical and Biochemical Cues on Polyether Ether Ketone/Hydroxyapatite/Magnesium Orthosilicate Composites for Orthopedic Applications","authors":"Praveen Jeyachandran, Lionel Yan Jin Lee, Si Jian Hui, Balamurugan Vellayappan, Jerry Ying Hsi Fuh, James Thomas Patrick Decourcy Hallinan, A. Senthil Kumar, Naresh Kumar","doi":"10.1021/acsami.5c22456","DOIUrl":"https://doi.org/10.1021/acsami.5c22456","url":null,"abstract":"A prime focus in orthopedic research is to promote osseointegration, while improving the functionality of implantable biomaterials. Surface topographic features have been shown to influence cell–biomaterial interactions, thereby facilitating cell adhesion, proliferation, and growth. However, a key challenge lies in inducing such topographical cues through existing biofabrication technologies. This study presents a newer strategy to leverage existing 3D printing (3DP) technology, promoting topographical cues manifested as microscopic spherulitic crystals integrated with nanoscopic lamellas on printed surfaces. Poly ether–ether–ketone (PEEK) composites reinforced with hydroxyapatite (HAp) and magnesium orthosilicate (Mg<sub>2</sub>SiO<sub>4</sub>) are printed using droplet-based 3D printing (3DP) technology, wherein the printing parameters are tailored to induce a network of spherulitic topographical cues in conjunction with biochemical cues arising from exposed bioactive fillers. Human osteosarcoma (Saos-2) cells are used to investigate the synergistic influence of the topographical and biochemical cues on the cell–material biological interactions. The composites exhibit hydrophilic surfaces with enhanced surface energy, promoting cellular adhesion and the formation of numerous filopodia, indicating an active engagement with spherulitic topographies. Composite surfaces featuring spherulitic topographical and biochemical cues foster a conducive environment, augmenting the cytocompatibility and osteogenic capabilities. Furthermore, process optimization not only improves the mechanical performance of the composites but also enhances their damping capabilities, a critical attribute for implant applications. This approach demonstrates that engineered spherulitic-topographical cues, in conjunction with biochemical cues, can mimic lamellar bone morphology, yielding improved biological and dynamic mechanical responses and highlighting their potential for personalized orthopedic implant applications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"301 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146116074","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Low-Temperature Ru-Ru Hybrid Bonding: Ar/H2 Plasma and NH4OH Synergistic Activation for Ultrahigh Density Interconnection. 低温Ru-Ru杂化键:Ar/H2等离子体和NH4OH协同活化的超高密度互连。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c23710
Yufei Bai, Jia Yang, Xinze Li, Qiushi Kang, Ziyang Xiu, Tadatomo Suga, Chenxi Wang

Ruthenium (Ru) has emerged as a promising next-generation metal for ultrahigh-density interconnects, offering superior electrical performance and electromigration resistance at submicrometre dimensions, and thus is a strong candidate to replace Cu in future very-large-scale integration (VLSI) technologies. However, enabling Ru/dielectric hybrid bonding at low temperatures remains exceedingly challenging. The intrinsically high melting point of Ru(∼2334 °C) and its extremely low diffusion coefficient (∼1 × 10-70 m2·s-1) typically necessitate high-temperature, high-pressure thermal compression bonding. In parallel, hydrophilic bonding with dielectric materials such as SiO2 must be achieved while suppressing Ru surface oxidation. In this study, we introduce a synergistic surface-activation strategy─Ar/H2 plasma treatment followed by immersion in NH4OH─that enables robust Ru-Ru bonding at 250 °C without oxidation. Moreover, the activated surfaces yield a 20% reduction in Ru surface resistance. This approach generates abundant -OH and -NH2 functional groups on the Ru surface, promoting interfacial reactions and the formation of a void-free interface. Intriguingly, the bond strengths exceeded 12 MPa after 1000 thermal cycles between -45 °C and +125 °C. This synergistic activation route provides a viable pathway for low-temperature Ru/dielectric hybrid bonding with high reliability. The demonstrated bonding performance underscores Ru potential as a Cu replacement in BEOL interconnects and establishes a foundation for metal/dielectric hybrid bonding in forthcoming high-density integration technologies.

钌(Ru)已经成为一种有前途的下一代超高密度互连金属,在亚微米尺寸上提供卓越的电性能和电迁移电阻,因此是未来超大规模集成电路(VLSI)技术中取代Cu的有力候选者。然而,在低温下实现Ru/介电杂化键仍然非常具有挑战性。Ru固有的高熔点(~ 2334°C)和极低的扩散系数(~ 1 × 10-70 m2·s-1)通常需要高温高压热压键合。同时,必须在抑制Ru表面氧化的同时实现与介电材料(如SiO2)的亲水性键合。在这项研究中,我们引入了一种协同表面活化策略──Ar/H2等离子体处理,然后浸泡在NH4OH中──使Ru-Ru在250°C下无氧化地形成坚固的键合。此外,活化表面可使Ru表面阻力降低20%。该方法在Ru表面生成丰富的-OH和-NH2官能团,促进界面反应,形成无空隙界面。有趣的是,在-45°C和+125°C之间进行1000次热循环后,结合强度超过了12 MPa。这种协同活化途径为低温高可靠性的Ru/介电杂化键合提供了一条可行的途径。所展示的键合性能强调了Ru作为BEOL互连中Cu替代品的潜力,并为即将到来的高密度集成技术中的金属/介电混合键合奠定了基础。
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引用次数: 0
A Hybrid Bilayer Design to Control Lithium Nucleation and Dendrite Growth in Lithium Metal Batteries. 控制锂金属电池中锂成核和枝晶生长的混合双层设计。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c23307
Ashwin P V, Supriya Sau, Novotna Seal, Amreen Bano, Sagar Mitra

Lithium metal batteries have gained renewed attention after a recent surge in high-energy battery systems. Lithium metal, known for its exceptional specific capacity and voltage, suffers from dendrite formation, which affects the cell performance and poses a severe safety threat, like internal short circuits and thermal runaway. Artificial solid electrolyte (ASEI) has emerged as an effective strategy to guide uniform lithium deposition, but only a few studies have explored the correlation between the interfacial kinetics and the nucleation behavior at the molecular level. In our work, we developed an inorganic-organic hybrid bilayer protective coating on the lithium anode, enabling over 1000 h of Li/Li symmetric cell cycling at 0.5 mA/cm2 (0.5 mAh/cm2) with low overpotentials. The impact of this bilayer on the nucleation behavior has been addressed using chronoamperometric studies and a modified SEI model based on S-H classical nucleation. Ab initio molecular dynamics (AIMD) simulations revealed the role of bilayer components in homogenizing the lithium flux by decreasing the coordination number of lithium ions and promoting lateral growth. These led to a relatively uniform lithium deposition morphology with better capacity retention of more than 80% after 80 cycles for protected lithium (p-Li)/NMC-622 half-cells cycled at 1.7 C with a high loading of 23 mg/cm2. Our findings establish the importance of interface engineering in controlling the nucleation kinetics of lithium deposition for the development of high-voltage lithium metal batteries.

锂金属电池在最近高能电池系统的激增后重新引起了人们的关注。锂金属以其特殊的比容量和电压而闻名,但由于树突的形成,会影响电池的性能,并造成严重的安全威胁,如内部短路和热失控。人工固体电解质(ASEI)已成为指导均匀锂沉积的有效策略,但在分子水平上探索界面动力学与成核行为之间的关系的研究很少。在我们的工作中,我们在锂阳极上开发了一种无机-有机杂化双层保护涂层,使锂/锂对称电池在0.5 mA/cm2 (0.5 mAh/cm2)下以低过电位循环超过1000小时。这种双分子层对成核行为的影响已经通过计时电流研究和基于S-H经典成核的改进SEI模型得到了解决。从头算分子动力学(AIMD)模拟揭示了双层组分通过降低锂离子配位数和促进横向生长来均匀锂通量的作用。这导致了相对均匀的锂沉积形态,保护锂(p-Li)/NMC-622半电池在1.7 C高负载23 mg/cm2下循环80次后容量保持率超过80%。我们的研究结果表明,界面工程在控制锂沉积成核动力学方面对高压锂金属电池的发展具有重要意义。
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引用次数: 0
Detection and Modulation of Gap States at the Grain Boundaries of Monolayer WS2. 单层WS2晶界间隙态的检测与调制。
IF 8.2 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-05 DOI: 10.1021/acsami.5c24211
Fateme Yekefalah, Albert Minj, Ankit Nalin Mehta, Thomas Nuytten, Pawan Kumar, Claudia Fleischmann, Ingrid De Wolf

In this work, an in-depth correlated study of the impact of grain boundaries on the excitonic and electronic properties of monolayer WS2 is reported. Signatures of defect- and strain-induced gap states are detected and studied in the vicinity of the grain boundaries using tip-enhanced photoluminescence, Kelvin probe force microscopy, and conductive atomic force microscopy. These gap states demonstrate a trap-like behavior for the free excitons, resulting in the radiative recombination of the localized excitonic states at room temperature. The trapping behavior is also detected for the free carriers, indicated by the abundance of fixed charges at the grain boundaries. The carrier trapping is corroborated through (tip-enhanced) photoluminescence spectroscopy at the grain boundaries, particularly after photoinjection of carriers. Comparison of the photoluminescence response acquired under ambient and high vacuum indicates the high reactivity of these defect sites and physisorption of ambient species. The ambient molecules seemingly passivate the defect sites and locally modulate the layer properties.

本文报道了晶界对单层WS2的激子和电子特性影响的深入相关研究。利用尖端增强光致发光、开尔文探针力显微镜和导电原子力显微镜,在晶界附近检测和研究了缺陷和应变引起的间隙状态的特征。这些间隙态对自由激子表现出类似陷阱的行为,导致局域激子态在室温下的辐射重组。自由载流子的捕获行为也被检测到,由晶界处固定电荷的丰度表示。通过(尖端增强)在晶界处的光致发光光谱证实了载流子捕获,特别是在载流子光注入后。通过比较环境真空和高真空条件下的光致发光响应,可以看出这些缺陷位点具有较高的反应活性和环境物质的物理吸附性。周围的分子似乎钝化了缺陷部位并局部调节了层的性质。
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引用次数: 0
Thermo-Regenerable Anion-Exchange Composites for the Removal of Diclofenac and Ibuprofen 热再生阴离子交换复合材料去除双氯芬酸和布洛芬
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsami.5c21493
Shanshan Xu, Rui Li, Chendong Shuang, Zhao Wang, Yang Yu, Rong Ji, Qing Zhou, Aimin Li, Tao Hou
Anion-exchange resins (AER) are widely applied in water treatment, although their chemical-intensive regeneration remains a bottleneck for the consumption of chemicals and generation of wastes. This study presents a thermo-regenerable AER composite (TR@AER) prepared via the interpenetration of poly(acrylic acid-co-acrylamide) (p(AA-co-AM)) within the AER matrix. TR@AER exhibits thermoresponsive hydrophilicity and surface charge, evidenced by a decrease in contact angle from 88.1° (25 °C) to 76.7° (50 °C) and a drop in ζ-potential from +36.9 mV (25 °C) to +31.1 mV (50 °C). In situ variothermal FTIR and molecular dynamics simulations reveal that this dual response is triggered by the dissociation of hydrogen bonds between −COOH and −CONH2 groups in p(AA-co-AM). The dissociation simultaneously drives the hydrophobic-to-hydrophilic transition and deprotonation of −COOH groups in p(AA-co-AM), which subsequently interact with quaternary ammonium (−NR3+) moieties of AER and alter surface charge characteristics. This enables a switchable adsorption and desorption of organic contaminants. At 25 °C, TR@AER rapidly adsorbs diclofenac and ibuprofen through synergistic electrostatic and hydrophobic interactions. Heating to 50 °C disrupts these interactions, significantly enhancing desorption. The desorption efficiency correlates with p(AA-co-AM) content in TR@AER. At the optimal p(AA-co-AM) loading (26–37 wt%), diclofenac desorption reached 92.2% and ibuprofen desorption reached 96.0% at 50 °C, representing 1.7- and 1.8-fold that of 25 °C, respectively. By circumventing chemical-intensive regeneration protocols, this work highlights an innovative strategy for stimuli-responsive adsorbent design with excellent regeneration capabilities.
阴离子交换树脂(AER)在水处理中得到了广泛的应用,尽管其化学物质密集的再生仍然是化学品消耗和废物产生的瓶颈。本研究提出了一种热再生的AER复合材料(TR@AER),通过在AER基体中插入聚丙烯酸-共丙烯酰胺(p(AA-co-AM))制备。TR@AER表现出热响应性亲水性和表面电荷,接触角从88.1°(25°C)下降到76.7°(50°C), ζ电位从+36.9 mV(25°C)下降到+31.1 mV(50°C)。原位变温FTIR和分子动力学模拟表明,这种双重反应是由p(AA-co-AM)中- COOH和- CONH2基团之间的氢键解离引起的。解离同时驱动p(AA-co-AM)中- COOH基团的亲疏转变和去质子化,这些基团随后与AER的季铵(- NR3+)部分相互作用并改变表面电荷特征。这使得有机污染物的可切换吸附和解吸。在25℃下,TR@AER通过静电和疏水的协同作用快速吸附双氯芬酸和布洛芬。加热到50°C会破坏这些相互作用,显著增强解吸。解吸效率与TR@AER中p(AA-co-AM)含量有关。在最佳p(AA-co-AM)负载(26-37 wt%)下,双氯芬酸和布洛芬在50℃下的解吸率分别为92.2%和96.0%,分别是25℃下的1.7倍和1.8倍。通过规避化学密集再生方案,这项工作强调了具有出色再生能力的刺激响应吸附剂设计的创新策略。
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引用次数: 0
Morphology Control in PDVT-10/DTCP Hybrid Films via Meniscus-Guided Cooperative Crystallization for High-Performance OFETs 利用半月板引导协同结晶技术控制PDVT-10/DTCP杂化膜的形态
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-04 DOI: 10.1021/acsami.5c23619
Xiao-Yuan Lin, Dhananjay S. Nipate, Shih-Kang Chen, Mai Harada, U-Ser Jeng, Michal Kohout, Hong-Cheu Lin, Yasutaka Kitagawa, Tomoyuki Akutagawa, Wen-Ya Lee, Hsiu-Hui Chen
The meniscus-guided coating (MGC) method was used to prepare well-aligned films of hybrid systems composed of the conjugated polymer poly{3,6-dithiophen-2-yl-2,5-di(2-decyltetra-decyl)-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thienylenevinylene-2,5-yl} (PDVT-10) and a photoresponsive small molecule dopant, dithienylperfluorocyclopentene (DTCP), at various concentrations in their open-ring form (DTCP-o) or closed-ring (DTCP-c) form. The structures of the coated films were characterized with polarized optical microscopy (POM), grazing-incidence X-ray diffraction (GIXRD), and atomic force microscopy (AFM). The DTCP can undergo reversible isomerization between a more twisted open-ring form and a more conjugated closed-ring form under UV and visible light, respectively. Both DTCP isomers were found to function as morphology-modulating additives that facilitate cooperative crystallization, an effect attributed to enhanced solution-phase molecular association, which impacts the packing of the polymer film. Organic field-effect transistors (OFETs) were fabricated from these films. The DTCP-c doping progressively enhanced charge transport, reaching the highest mobility of 2.44 cm2 V−1 s−1 at 10 wt %. Notably, 3 wt % DTCP-o, typically considered insulating molecule, increased PDVT-10 mobility from 2.12 to 3.23 cm2 V−1 s−1. This improvement is suggested to arise from the combined effects of precise molecular alignment by the MGC method and a favorable HOMO–HOMO energy level alignment predicted by DFT, enabling cooperative charge transfer despite the nominally insulating nature of the open-ring form. The photoswitchable DTCP provides a unique opportunity to optically modulate frontier molecular orbital energy levels, thereby opening up an avenue for designing electronic devices such as photocontrollable OFETs.
采用半月板引导镀膜(MGC)方法制备了由共轭聚合物聚{3,6-二噻吩-2-基-2,5-二(2-癸基四癸基)-吡咯[3,4-c] -吡咯-1,4-二酮-噻吩-2,5-基}(PDVT-10)和光响应小分子掺杂剂二噻吩基全氟环戊烯(DTCP)以不同浓度的开环形式(DTCP-o)或闭环形式(DTCP-c)组成的排列良好的杂化体系薄膜。利用偏光显微镜(POM)、掠入射x射线衍射(GIXRD)和原子力显微镜(AFM)对涂层的结构进行了表征。在紫外光和可见光下,DTCP可以在更扭曲的开环形式和更共轭的闭环形式之间进行可逆异构化。研究发现,这两种DTCP异构体都可以作为形态调节添加剂,促进协同结晶,这一效应归因于增强的溶液相分子缔合,从而影响聚合物膜的填充。利用这些薄膜制备了有机场效应晶体管(ofet)。DTCP-c掺杂逐渐增强了电荷输运,在10 wt %时达到2.44 cm2 V−1 s−1的最高迁移率。值得注意的是,3 wt %的DTCP-o,通常被认为是绝缘分子,将PDVT-10的迁移率从2.12增加到3.23 cm2 V−1 s−1。这种改进被认为是由于MGC方法的精确分子定位和DFT预测的有利的HOMO-HOMO能级定位的共同作用,尽管开环形式名义上具有绝缘性质,但仍能实现电荷的协同转移。光开关DTCP为光调制前沿分子轨道能级提供了一个独特的机会,从而为设计光可控ofet等电子器件开辟了一条途径。
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