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Superior Energy-Storage Performance Enabled by Machine Learning Accelerated Composition Design for Lead-Free Antiferroelectrics 机器学习加速了无铅反铁电体的成分设计,实现了卓越的储能性能
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/smll.202514461
Feng Li, Liang Sun, Zongyuan Zhang, Xuan Wang, He Qi, Yannan Bin, Jia-Ze Li, Yacheng Yang, Yonghao Xu, Siyu Chen, Mingsheng Long, Lei Shan, Li-Feng Zhu, Chunchang Wang, Jiwei Zhai
Development of high-performance lead-free AgNbO3 (AN)-based antiferroelectrics (AFEs) have emerged as promising candidate for high-power energy-storage capacitors. Routine trial-and-error method in enhancing energy-storage density (Wrec) and efficiency (η) encounters great challenges since extensive latent space are explored for composition screening. Using machine learning (ML) algorithms, a two-layer stacking framework termed as SS-PAN (stacking strategy for predicting AN-based ceramics) is proposed here for designing high-performance AN-based AFEs. This framework achieves a high R2 score of 0.82 through cross validation and outperforms individual ML model. The predicted composition represented by Li0.01Ag0.99Nb0.5Ta0.5O3, possesses a quasi-linear P-E loop and an ultrahigh Wrec of 16.6 J cm−3 and η of 92.6% with an excellent figure of merit of 224.3 J cm−3 is achieved at electric field of 108 kV mm−1 in MLCC. Based on SHapley Additive exPlanations analysis, high prediction accuracy is enabled by precisely selecting features of tolerance factor and electron affinity of B-site element. Notably, local structure for Li0.01Ag0.99Nb0.5Ta0.5O3 composition is thoroughly decoded by STEM and DFT calculations, where highly polar short-range antiferroelectric nanodomains with strong localized dipole moments are induced by Li/Ta co-doping. This work imparts a potent potential of data-driven methodology for seeking emergent relaxor AFEs for advanced dielectric capacitor applications.
高性能无铅AgNbO3 (AN)基反铁电体(AFEs)已成为大功率储能电容器的有前途的候选材料。常规的试错法在提高能量存储密度(Wrec)和效率(η)方面遇到了巨大的挑战,因为在成分筛选方面探索了广阔的潜在空间。本文利用机器学习(ML)算法,提出了一种称为SS-PAN(预测人工智能陶瓷的堆叠策略)的双层堆叠框架,用于设计高性能的基于人工智能的人工智能陶瓷。该框架通过交叉验证获得了0.82的高R2分数,优于单个ML模型。在MLCC中,在108 kV mm−1电场下,Li0.01Ag0.99Nb0.5Ta0.5O3具有准线性P-E环,超高的Wrec为16.6 J cm−3,η为92.6%,优良的品质系数为224.3 J cm−3。在SHapley Additive explanation分析的基础上,通过精确选择b位元件的容差因子和电子亲和特性,实现了较高的预测精度。值得注意的是,通过STEM和DFT计算彻底解码了Li0.01Ag0.99Nb0.5Ta0.5O3成分的局部结构,其中Li/Ta共掺杂诱导出具有强局域偶极矩的高极性短程反铁电纳米畴。这项工作赋予了数据驱动方法的强大潜力,用于寻找先进介质电容器应用的紧急弛豫afe。
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引用次数: 0
Scalable Ionogel Film with Enhanced Thermal Conductivity for High-Efficiency Passive Cooling via Sorption–Radiation Balance 通过吸附-辐射平衡,可扩展的电离凝胶膜具有增强的导热性,用于高效被动冷却
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1021/acsami.5c22701
Mingzhao Yang, Jipeng Luo, Peixia Qi, Hongya Li, Jialin Deng, Yongchen Song, Lunxiang Zhang, Quan Shi
Passive cooling, particularly those combining evaporative and radiative mechanisms, has attracted growing interest due to its low energy requirements for powering electronic devices and integrated systems. However, complex fabrication, low thermal conductivity, and inherent trade-offs between competing cooling mechanisms hinder their potential for commercial application. To address these challenges, we combine hexagonal boron nitride (hBN) with 1-ethyl-3-methylimidazolium acetate (Emim Ac, EA) ionic liquid and fabricate an ionic composite film via a facile, scalable solvent evaporation method. This approach eliminates the need for specialized equipment and intricate steps in traditional cooling materials. The composite film achieves synergistic passive cooling by simultaneously leveraging the evaporative and radiative mechanisms. The incorporation of hBN significantly enhances thermal conductivity to 0.51 W·m–1·K–1, representing a 200% improvement over conventional materials such as silica gel and MOFs. The optimized film structure demonstrates a high-water sorption capacity (0.55 g/g) and an exceptional desorption enthalpy (1307 J/g), enabling efficient evaporative cooling. Furthermore, the film demonstrates a low desorption temperature of 40 °C and remarkable flexibility, making it suitable for diverse thermal management applications. Practical tests verify its effectiveness, lowering the temperature of computer CPUs by more than 5 °C within 8 min and reducing the temperature of photovoltaic (PV) cells by up to 10 °C. By integrating thermal conduction, water evaporation, and thermal radiation, this work presents a high-performance, zero-energy-consumption cooling strategy with broad applicability in electronics and energy systems.
被动冷却,特别是结合蒸发和辐射机制的被动冷却,由于其为电子设备和综合系统供电的低能量需求而引起了越来越多的兴趣。然而,复杂的制造、低导热性以及相互竞争的冷却机制之间的内在权衡阻碍了它们的商业应用潜力。为了解决这些问题,我们将六方氮化硼(hBN)与1-乙基-3-甲基咪唑醋酸盐(Emim Ac, EA)离子液体结合起来,通过简单、可扩展的溶剂蒸发方法制备了离子复合膜。这种方法消除了传统冷却材料中对专用设备和复杂步骤的需要。复合薄膜通过同时利用蒸发和辐射机制实现协同被动冷却。hBN的掺入显著提高了导热系数,达到0.51 W·m-1·K-1,比硅胶和mof等传统材料提高了200%。优化后的膜结构具有较高的吸水能力(0.55 g/g)和优异的解吸焓(1307 J/g),可实现高效的蒸发冷却。此外,该薄膜具有40°C的低解吸温度和卓越的灵活性,适用于各种热管理应用。实际测试验证了它的有效性,在8分钟内将计算机cpu的温度降低了5°C以上,将光伏电池的温度降低了10°C。通过整合热传导、水蒸发和热辐射,这项工作提出了一种高性能、零能耗的冷却策略,在电子和能源系统中具有广泛的适用性。
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引用次数: 0
First-principles study on effective hydrogen adsorption and gas sensing on WSe2 surface by Pt modification and GaN heterojunction construction Pt修饰和GaN异质结构建对WSe2表面有效氢吸附和气敏的第一性原理研究
IF 6.7 2区 材料科学 Q2 CHEMISTRY, PHYSICAL Pub Date : 2026-02-10 DOI: 10.1016/j.apsusc.2026.166288
Li Ye, Yongchao Liang, Wenqiang Li, Qian Chen, Jian Xiong
Achieving effective adsorption and sensing of H2 has become one of the most challenging and difficult tasks for maintaining a sustainable environment. The first-principles density functional theory was used for exploring the adsorption and sensing properties of H2, CO, HCN, CH4, and NH3 gas molecules on the Pt-WSe2 and GaN/WSe2 structures. By conducting calculations, the most stable adsorption configuration was identified. To begin with, the adsorption properties indicated that all gas molecules were physically adsorbed onto the WSe2 substrate. Furthermore, the Pt atoms were stably anchored at the S(H) site on the surface of WSe2, resulted in an increase of 0.33 eV in the adsorption energy for H2. The density of states further confirms that this modification alters the electronic properties of WSe2, thereby enhancing its adsorption performance. Finally, the GW surface in the WSe2/GaN heterostructure significantly enhanced the adsorption energy of H2 to −2.048 eV and improved the adsorption performance for CO, HCN, CH4, and NH3 molecules. Recovery times at room temperature were calculated for multiple configurations, predicting ultra-high selectivity and favorable recovery times for Pt-WSe2 toward all four gases except CH4. The adsorption mechanism is controlled by the changes in conductivity caused by charge transfer. These theoretical studies provide the theoretical basis for the practical application of monolayer WSe2 in hydrogen sensing and gas adsorption.
实现氢气的有效吸附和传感已成为维持可持续环境的最具挑战性和最困难的任务之一。利用第一性原理密度泛函理论研究了Pt-WSe2和GaN/WSe2结构对H2、CO、HCN、CH4和NH3气体分子的吸附和传感性能。通过计算,确定了最稳定的吸附构型。首先,吸附性质表明所有气体分子都被物理吸附到WSe2底物上。Pt原子稳定锚定在WSe2表面的S(H)位点,使WSe2对H2的吸附能提高了0.33 eV。态密度进一步证实了这种修饰改变了WSe2的电子性质,从而提高了其吸附性能。最后,WSe2/GaN异质结构中的GW表面显著提高了H2的吸附能至−2.048 eV,提高了对CO、HCN、CH4和NH3分子的吸附性能。计算了多种构型在室温下的回收时间,预测了Pt-WSe2对除CH4外的所有四种气体的超高选择性和有利的回收时间。吸附机理受电荷转移引起的电导率变化控制。这些理论研究为单层WSe2在氢气传感和气体吸附方面的实际应用提供了理论基础。
{"title":"First-principles study on effective hydrogen adsorption and gas sensing on WSe2 surface by Pt modification and GaN heterojunction construction","authors":"Li Ye, Yongchao Liang, Wenqiang Li, Qian Chen, Jian Xiong","doi":"10.1016/j.apsusc.2026.166288","DOIUrl":"https://doi.org/10.1016/j.apsusc.2026.166288","url":null,"abstract":"Achieving effective adsorption and sensing of H<sub>2</sub> has become one of the most challenging and difficult tasks for maintaining a sustainable environment. The first-principles density functional theory was used for exploring the adsorption and sensing properties of H<sub>2</sub>, CO, HCN, CH<sub>4</sub>, and NH<sub>3</sub> gas molecules on the Pt-WSe<sub>2</sub> and GaN/WSe<sub>2</sub> structures. By conducting calculations, the most stable adsorption configuration was identified. To begin with, the adsorption properties indicated that all gas molecules were physically adsorbed onto the WSe<sub>2</sub> substrate. Furthermore, the Pt atoms were stably anchored at the S(H) site on the surface of WSe<sub>2</sub>, resulted in an increase of 0.33 eV in the adsorption energy for H<sub>2</sub>. The density of states further confirms that this modification alters the electronic properties of WSe<sub>2</sub>, thereby enhancing its adsorption performance. Finally, the GW surface in the WSe<sub>2</sub>/GaN heterostructure significantly enhanced the adsorption energy of H<sub>2</sub> to −2.048 eV and improved the adsorption performance for CO, HCN, CH<sub>4</sub>, and NH<sub>3</sub> molecules. Recovery times at room temperature were calculated for multiple configurations, predicting ultra-high selectivity and favorable recovery times for Pt-WSe<sub>2</sub> toward all four gases except CH<sub>4</sub>. The adsorption mechanism is controlled by the changes in conductivity caused by charge transfer. These theoretical studies provide the theoretical basis for the practical application of monolayer WSe<sub>2</sub> in hydrogen sensing and gas adsorption.","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"1 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2026-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146146144","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
Ligand-Free MgCO3 Nanoclusters Catalyze Nucleophilic Alcohol Addition Reactions 无配体MgCO3纳米团簇催化亲核醇加成反应
IF 9.5 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1021/acsami.5c21329
Lluís Martínez-Belenguer, Kateřina Zítová, Jose Pedro Cerón-Carrasco, Belén Lerma-Berlanga, Antonio Leyva-Pérez
Subnano and nanometric metal clusters are ultrasmall aggregates in which most atoms are exposed on the surface, directly interacting with reactants and enabling highly efficient catalysis. However, metal carbonate clusters have been barely prepared and used in catalysis. Here, we report the synthesis of ultrasmall, ligand-free MgCO3 clusters formed via CO2 capture with MgCl2, with an average composition of [MgCO3]5·3H2O. These clusters exhibit catalytic activity in various nucleophilic alcohol addition reactions, showing a 5-fold enhancement compared to bulk MgCO3 and CaCO3–triethylamine clusters. These results pave the way for synthesis of ultrasmall alkaline metal carbonate clusters beyond Ca, which can be employed as efficient catalysts in organic synthesis.
亚纳米和纳米金属簇是一种超小的聚集体,其中大多数原子暴露在表面,直接与反应物相互作用,实现高效催化。然而,金属碳酸盐簇很少被制备并用于催化。在这里,我们报道了用MgCl2捕获CO2形成的超小的,无配体的MgCO3簇的合成,其平均组成为[MgCO3]5·3H2O。这些团簇在各种亲核醇加成反应中表现出催化活性,与散装MgCO3和caco3 -三乙胺团簇相比,表现出5倍的增强。这些结果为超小碱性金属碳酸盐簇的合成铺平了道路,该簇可作为有机合成中的高效催化剂。
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引用次数: 0
Design principles for fluoroethylene carbonate additive–electrode compatibility in nanoporous sugarcane bagasse-based hard carbon sodium ion anodes 纳米多孔蔗渣基硬碳钠离子阳极中氟碳酸乙烯添加剂-电极相容性的设计原则
IF 11.9 2区 材料科学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2026-02-10 DOI: 10.1039/d5ta09846g
Jiahan Fu, Sheng Li, Chaofan Luo, Honglin Hu, Tianshun Xiong, Xin Li, Junyou Yang, Guangwei Huang, Jianfang Li, Yubo Luo, Canhuang Zhang
Nanopore sodium storage underpins the characteristic low-voltage plateau in hard carbon (HC) anodes. Yet, the interfacial impact of electrolyte additives on this confined process remains largely elusive. Herein, we unveil a pore-blocking mechanism in sugarcane bagasse-based hard carbon (SuHC) induced by fluoroethylene carbonate (FEC), a widely used solid electrolyte interphase (SEI) forming additive. Using a combination of electrochemical analysis, spectroscopy, electron microscopy, and density functional theory, we demonstrate that FEC decomposition induces NaF-rich deposits in near-surface pore domains and pore-entrance regions, which impede Na+ intercalation and suppress the low-voltage plateau. High-resolution transmission electron microscopy (HRTEM) reveals NaF-matching crystallites in subsurface regions close to particle edges. This interfacial chemistry drives a mechanistic shift from diffusion-dominated intercalation to surface-limited capacitive storage. Our findings highlight the critical importance of additive–structure compatibility and offer design principles for tailoring electrolyte formulations for nanoporous carbon anodes in next-generation SIBs.
纳米孔钠存储支撑了硬碳(HC)阳极的低压平台特性。然而,电解质添加剂对这一受限过程的界面影响在很大程度上仍然难以捉摸。在此,我们揭示了一种被广泛使用的固体电解质界面(SEI)形成添加剂氟碳酸乙烯(FEC)诱导的甘蔗甘蔗渣基硬碳(SuHC)的孔阻塞机制。结合电化学分析、光谱学、电子显微镜和密度泛函理论,我们证明FEC分解在近表面孔域和孔入口区域诱导富naf沉积,这阻碍了Na+的嵌入并抑制了低压平台。高分辨率透射电子显微镜(HRTEM)显示,在靠近颗粒边缘的亚表面区域有与naf匹配的晶体。这种界面化学驱动了从扩散主导的插层到表面限制电容存储的机制转变。我们的研究结果强调了添加剂-结构相容性的重要性,并为下一代sib中纳米多孔碳阳极的定制电解质配方提供了设计原则。
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引用次数: 0
Self-Assembled Carrier-Free Nanomedicines Potentiate Chemo-Photothermal Immunotherapy by Overcoming Prostaglandin E2-Mediated Immunosuppression 自组装无载体纳米药物通过克服前列腺素e2介导的免疫抑制来增强化学光热免疫治疗
IF 13.3 2区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/smll.202512540
Xiaoliang Deng, Lina Wu, Boxin Chen, Xiaohui Tang, Shiying Xu, Yinxing Huang, Fan Pan, Jun Lu, Xianquan Feng
Inflammation plays a pivotal role in fostering an immunosuppressive tumor microenvironment, which diminishes tumor immunogenic cell death (ICD) and subsequently promotes tumor recurrence and metastasis. The COX-2/PGE2 signaling axis has been identified as a crucial regulator in the establishment of immunosuppressive conditions. Herein, this work developed an excipient-free nanomedicine (IPC NPs) via non-covalent self-assembly, integrating indocyanine green and paclitaxel (dual ICD inducers) with celecoxib (COX-2/PGE2 inhibitor) for combined chemo-photothermal therapy with anti-inflammatory effects. The IPC NPs displayed monodisperse characteristics with optimal near-infrared responsiveness, significantly enhancing tumor tissue permeation while demonstrating synergistic chemo-photothermal cytotoxicity against triple-negative breast cancer (TNBC). Notably, IPC NPs-encapsulated celecoxib effectively remodeled the tumor inflammatory microenvironment by attenuating therapy-induced inflammatory responses, thereby potentiating ICD. This triple therapy regimen promoted dendritic cell maturation, enhanced cytotoxic T lymphocyte infiltration into tumor tissues, and upregulated effector memory T cell populations in TNBC. These immunomodulatory effects substantially ameliorated the immunosuppressive tumor microenvironment, leading to significant inhibition of primary tumor growth and metastasis. Collectively, this work presents a novel carrier-free nanotherapeutic strategy that synergistically combines chemo-photothermal-inflammatory suppression therapy, offering a promising approach for TNBC.
炎症在培养免疫抑制肿瘤微环境中起关键作用,从而减少肿瘤免疫原性细胞死亡(ICD),并随后促进肿瘤复发和转移。COX-2/PGE2信号轴已被确定为建立免疫抑制条件的关键调节因子。本研究通过非共价自组装开发了一种无赋形剂纳米药物(IPC NPs),将吲哚青绿和紫杉醇(双ICD诱导剂)与塞来昔布(COX-2/PGE2抑制剂)结合,用于具有抗炎作用的化学光热联合治疗。IPC NPs表现出单分散特性,具有最佳的近红外响应性,显著增强肿瘤组织渗透,同时显示出对三阴性乳腺癌(TNBC)的协同化学-光热细胞毒性。值得注意的是,IPC nps包封的塞来昔布通过减弱治疗诱导的炎症反应,有效地重塑了肿瘤炎症微环境,从而增强了ICD。这种三联治疗方案促进了树突状细胞的成熟,增强了细胞毒性T淋巴细胞向肿瘤组织的浸润,并上调了TNBC中的效应记忆T细胞群。这些免疫调节作用大大改善了免疫抑制的肿瘤微环境,从而显著抑制原发肿瘤的生长和转移。总的来说,这项工作提出了一种新的无载体纳米治疗策略,该策略协同结合了化学-光热-炎症抑制治疗,为TNBC提供了一种有希望的方法。
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引用次数: 0
Selenium oxide nanostructure-based electrodes for rapid and simultaneous electrochemical determination of oxalic and ascorbic acids in food matrices 用于食品基质中草酸和抗坏血酸快速同时电化学测定的氧化硒纳米结构电极
IF 6.7 3区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1039/d5nr04332h
Rania M. Needa, Hosny Ibrahim, Ahmed F. A. Youssef, Rabeay Y. A. Hassan
The development of nanostructured electrochemical platforms for rapid and selective sensing of coexisting biomolecules remains a key challenge in food analysis. Herein, selenium oxide nanostructures (SeO2NSs) were synthesized and integrated into carbon-based electrodes to enable the simultaneous electrochemical detection of ascorbic acid (AA) and oxalic acid (OA) in complex food matrices. Comprehensive morphological, structural, and electrochemical characterization studies confirmed the uniform distribution, high surface area, and excellent redox activity of the SeO2NSs. Under optimized chronoamperometric conditions, the SeO2NS-modified electrode exhibited wide linear response ranges of 5.0–550 µM for OA and 5.0–455 µM for AA, with low detection limits of 0.50 µM and 0.43 µM, respectively. The sensor demonstrated remarkable selectivity and stability against common interfering species, ensuring accurate quantification in real samples. Thus, the developed platform was successfully applied to the simultaneous determination of AA and OA in fresh fruits and vegetables (guava, spinach, and mango) and in beverages derived from coffee beans and tea leaves. This work highlights the potential of selenium oxide nanostructures as efficient electroactive materials for high-performance, cost-effective, and reliable electrochemical sensing in food-quality monitoring and safety assessment.
开发纳米结构电化学平台,快速和选择性地检测共存的生物分子,仍然是食品分析中的一个关键挑战。本文合成了氧化硒纳米结构(SeO2NSs)并将其集成到碳基电极中,以实现复杂食品基质中抗坏血酸(AA)和草酸(OA)的同时电化学检测。全面的形态、结构和电化学表征研究证实了SeO2NSs的均匀分布、高表面积和优异的氧化还原活性。在优化的时间电流条件下,seo2ns修饰电极对OA的线性响应范围为5.0 ~ 550µM,对AA的线性响应范围为5.0 ~ 455µM,检出限分别为0.50µM和0.43µM。该传感器对常见干扰物质表现出显著的选择性和稳定性,确保了实际样品的准确定量。因此,所建立的平台成功地应用于新鲜果蔬(番石榴、菠菜、芒果)和咖啡豆、茶叶饮料中AA和OA的同时测定。这项工作强调了氧化硒纳米结构作为高效电活性材料的潜力,在食品质量监测和安全评估中具有高性能、低成本和可靠的电化学传感。
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引用次数: 0
Engineering Liquid Metal Nanoparticles for Wearable Devices 工程液态金属纳米颗粒可穿戴设备
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1021/acsnano.5c18099
Yuxuan Chen, Zhiheng Zhang, Shan He, Guozhen Liu
Liquid metals (LMs) are emerging as highly promising materials for wearable devices owing to their exceptional properties, such as high electrical and thermal conductivity, biocompatibility, flexibility, and unique surface characteristics. Through surface engineering with ligands, polymers, and nanomaterials, LMs can be processed into stable bioinks with enhanced oxidation resistance, adhesion, and multifunctionality. These bioinks are further integrated into microneedle and patch-based wearables via fabrication strategies, including photolithography, micromolding, 3D printing, screen and inkjet printing, and direct writing. Such integration enables diverse biomedical applications, ranging from physiological signal monitoring and sweat or temperature sensing to wound healing, antibacterial therapy, and controlled drug delivery. Despite these advances, challenges remain in application maturity, long-term stability, biocompatibility, and scalable manufacturing. Accordingly, this review summarizes these challenges and outlines future directions for LM-based wearable biomedical devices.
液态金属(LMs)由于其优异的性能,如高导电性和导热性、生物相容性、柔韧性和独特的表面特性,正在成为可穿戴设备的极具前景的材料。通过配体、聚合物和纳米材料的表面工程,LMs可以被加工成稳定的生物墨水,具有增强的抗氧化性、附着力和多功能性。这些生物墨水通过光刻、微成型、3D打印、丝网和喷墨打印以及直接书写等制造策略,进一步集成到微针和贴片式可穿戴设备中。这样的集成使多种生物医学应用成为可能,从生理信号监测、汗液或温度传感到伤口愈合、抗菌治疗和控制药物输送。尽管取得了这些进步,但在应用成熟度、长期稳定性、生物相容性和可扩展制造方面仍然存在挑战。因此,本文总结了这些挑战,并概述了基于lm的可穿戴生物医学设备的未来发展方向。
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引用次数: 0
Proton Provision-Conversion-Spillover Cascade Programming on Dual Supported Pt Atoms for Robust Hydrogen Production 双支撑Pt原子上的质子供给-转换-溢出级联规划
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202522479
Mansheng Liao, Yuan Zhang, Qianyi Lin, Kaiming Liang, Yayun Hong, Lei Zhang
Rational proton engineering offers a powerful strategy for enhancing the hydrogen evolution reaction (HER) performance of single-atom catalysts (SACs). Notably, achieving concerted proton management across multiple reaction steps presents a highly efficient approach, yet it remains more challenging to implement than single-step regulation. Here, we propose a domino-type proton provision-conversion-spillover programming for Pt SACs in acidic HER, enabled by ultrathin porous nitrogen-doped carbon (main 1–2 atomic layers, sub-1 nm) encapsulated TiN nanowires with tips as dual-support tip-platform (Pt-NC1@TiN NWs). Experimental and theoretical results demonstrate that this platform triggers tip-distance-spillover domino effects to drive a proton cascade throughout HER. Specifically, NC1@TiN nanotips induce tip-enhanced effect that promotes interfacial proton accessibility. Concurrently, the short-distance Pt/TiN vertical coupling optimizes electronic modulation of unsaturated Pt-N2 sites to enhance their intrinsic activity. Exposed TiN sites function as hydrogen spillover centers to facilitate H2 desorption. Consequently, Pt-NC1@TiN NWs achieve a superior Pt mass activity of 153.5 A/mgPt@-100 mV, surpassing Pt/C by two orders of magnitude. Notably, it reaches 2 A/cm2 at low cell voltage of 1.75 V and sustains stable operation at 1 A/cm2 for 1200 h in proton exchange membrane water electrolyzer (PEMWE). This work indicates the potential of harnessing multi-step domino processes for advanced catalyst design.
合理的质子工程为提高单原子催化剂的析氢反应性能提供了有力的策略。值得注意的是,实现跨多个反应步骤的协调质子管理是一种高效的方法,但实施起来仍然比单步调节更具挑战性。在这里,我们提出了一个多米诺骨式质子供应-转换-溢出编程,用于酸性HER中的Pt SACs,通过超薄多孔氮掺杂碳(主要1-2原子层,sub- 1nm)封装TiN纳米线,尖端作为双支撑尖端平台(Pt-NC1@TiN NWs)实现。实验和理论结果表明,该平台触发尖端距离溢出多米诺骨牌效应,驱动质子级联贯穿HER。具体来说,NC1@TiN纳米尖端诱导了尖端增强效应,促进了界面质子的可及性。同时,短距离Pt/TiN垂直耦合优化了不饱和Pt- n2位点的电子调制,增强了其固有活性。暴露的TiN位点作为氢溢出中心,促进H2的解吸。因此,Pt-NC1@TiN NWs的Pt质量活度达到153.5 a /mgPt@-100 mV,比Pt/C高出两个数量级。值得注意的是,它在1.75 V的低电池电压下达到2 A/cm2,并在质子交换膜水电解槽(PEMWE)中以1 A/cm2稳定运行1200小时。这项工作表明利用多步骤多米诺过程进行先进催化剂设计的潜力。
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引用次数: 0
Bioinspired Engineered Virus-Mimetic Vesicles for Enhanced Cytosolic Delivery of STING Agonists Into Dendritic Cells 生物启发工程病毒模拟囊泡增强STING激动剂进入树突状细胞的胞浆输送
IF 29.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-10 DOI: 10.1002/adma.202520019
Shi-Zhen Geng, Yaru Shi, Jinjin Yang, Yiwen Gao, Zhehao Zhang, Hao Wu, Pan-Miao Liu, Jinjin Shi, Yiling Yang, Jian-Jun Yang
Effective delivery to dendritic cells (DCs) is crucial for the clinical translation of STING agonists, however, current cyclic dinucleotide (CDN) therapies are hindered by inefficient cytosolic delivery and off-target activation-induced T cell exhaustion. Here, a high-fidelity, dengue virus-mimetic platform (CDN@VLP) is engineered to leverage natural tropism for precise cytosolic release in immature DCs. Compared to conventional lipid nanoparticles, CDN@VLP enhances DC-specific uptake by 1.9-fold while reducing non-specific T cell internalization in tumors by 14.8-fold, achieving comparable antitumor efficacy at one-fortieth the dose of free CDN. Systematic screening identifies an optimal VLP subtype that improves targeted accumulation in type 1 conventional DCs (cDC1s)—a subset essential for STING pathway activation—by 2.3-fold and amplifies durable type I interferon responses, resulting in a 12.8-fold increase in IFN-β production. Transcriptomic analysis further reveals that CDN@VLP promotes cDC1 recruitment into tumors by enhancing the secretion of key chemokines (XCL1, CCL4, and CCL5), suggesting an additional mechanism of action. By mimicking viral tropism, the CDN@VLP platform establishes a paradigm for precision STING activation, overcoming the trade-off between potency and specificity in cDC1-targeted immunotherapy.
有效递送到树突状细胞(dc)对于STING激动剂的临床翻译至关重要,然而,目前的环二核苷酸(CDN)治疗受到低效的细胞质递送和脱靶激活诱导的T细胞衰竭的阻碍。在这里,一个高保真度的登革热病毒模拟平台(CDN@VLP)被设计为利用自然趋向性在未成熟的树突状细胞中精确释放细胞质。与传统的脂质纳米颗粒相比,CDN@VLP将dc特异性摄取提高了1.9倍,同时将肿瘤中的非特异性T细胞内化降低了14.8倍,在游离CDN剂量的十分之一下达到相当的抗肿瘤效果。系统筛选确定了一种最佳的VLP亚型,该亚型可将1型常规dc (cDC1s) (STING通路激活所必需的子集)的靶向积累提高2.3倍,并放大持久的I型干扰素反应,从而使IFN-β的产生增加12.8倍。转录组学分析进一步揭示CDN@VLP通过增强关键趋化因子(XCL1、CCL4和CCL5)的分泌来促进cDC1向肿瘤募集,提示了另一种作用机制。通过模仿病毒的趋向性,CDN@VLP平台建立了精确STING激活的范例,克服了cdc1靶向免疫治疗中效力和特异性之间的权衡。
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