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Dual-Field Amplification via Nanotip-Engineered Catalysts for Efficient Spin-State and Ion Regulation in Aluminum–Sulfur Batteries 铝硫电池中高效自旋态和离子调节的纳米尖端催化剂双场放大
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c16319
Xingjun Liu,Jinghan Wang,Jiqiang Zhan,Qixin Wang,Xiaojing Lin,Hongpeng Li,Hongsen Li
Modulating the electronic structure of catalysts through external magnetic fields is a promising strategy for enhancing electrocatalytic activity, which has been successfully demonstrated in the oxygen evolution reaction (OER), zinc-air batteries and lithium–sulfur batteries. However, conventional magnetic regulation approaches typically focus solely on spin-state modulation, neglecting the ion transport limitations in practical systems. Additionally, existing permanent magnets and ferromagnetic additives generate magnetic fields with limited intensity and nonuniform directionality, restricting their effectiveness. Herein, we propose a tip-enhanced magnetic-electric dual-field strategy by rationally designing ferromagnetic NiCo2O4 catalysts with nanotip architectures to address long-standing kinetic bottlenecks in aluminum–sulfur (Al–S) batteries. Finite element analysis demonstrates that the high-curvature tips significantly amplify local electric and magnetic fields by approximately 4.2- and 2.6-fold, respectively, under an external field. Moreover, the induced spin-state transition of Ni3+ to high-spin (HS) states enhances d-p orbital hybridization with polysulfide intermediates, effectively lowering reaction barriers. This dual enhancement synergistically promotes ion transport via magnetohydrodynamic (MHD) effects, leading to substantially reduced voltage hysteresis and markedly improved electrochemical performance, delivering a high reversible capacity of 513 mAh g–1 after 700 cycles in Al–S batteries. By integrating geometric field amplification with spin-state modulation, this work presents a highly efficient and scalable strategy for approach to designing high-performance catalysts for advanced Al–S batteries.
通过外加磁场调节催化剂的电子结构是提高电催化活性的一种很有前途的策略,这种策略已在析氧反应(OER)、锌空气电池和锂硫电池中得到了成功的证明。然而,传统的磁调节方法通常只关注自旋态调制,而忽略了实际系统中离子输运的限制。此外,现有的永磁体和铁磁添加剂产生的磁场强度有限,方向性不均匀,限制了它们的有效性。本文提出了一种尖端增强的磁电双场策略,通过合理设计具有纳米尖端结构的铁磁性NiCo2O4催化剂来解决铝硫(Al-S)电池长期存在的动力学瓶颈。有限元分析表明,在外加磁场作用下,高曲率尖端将局部电场和磁场分别放大约4.2倍和2.6倍。此外,Ni3+诱导的自旋态向高自旋态的转变增强了与多硫化物中间体的d-p轨道杂化,有效地降低了反应势垒。这种双重增强通过磁流体动力学(MHD)效应协同促进离子传输,从而大大降低了电压滞后,显著提高了电化学性能,在700次循环后,Al-S电池的可逆容量高达513 mAh g-1。通过将几何场放大与自旋态调制相结合,本研究为设计先进Al-S电池的高性能催化剂提供了一种高效且可扩展的策略。
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引用次数: 0
In Situ Redox-Omics Decoding of Nanoparticle–Protein Corona Interactions Drives the Mitochondrial Metabolic-Immunological Mechanism in Microglia 纳米颗粒-蛋白电晕相互作用的原位氧化还原组学解码驱动小胶质细胞线粒体代谢-免疫机制
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c21740
Ze-Kun Chen,Ming Yu,Zhong-Yao Li,Ling-Li Zheng,Ji-Chao Zhang,Ting-Ting Liu,Zhuo Yang,Ling Li,Zhi-Yuan Lu,Tian-Tian Wei,Hua Wang,Bo Han,Wei Yu,Peng-Fei Tu,Ke-Wu Zeng
Nanoparticle–protein corona interactions critically determine biological responses but remain poorly characterized in living systems due to the lack of noninvasive analytical tools. In this study, we developed a redox-omics strategy that facilitated the in situ mapping of corona composition by tracking cysteine thiol oxidation markers induced by nanoparticles. As a research tool, we synthesized natural-organic-matter-derived carbon dots (nCDs) with dual superoxide dismutase/catalase-mimetic activity. A global redox-omics analysis identified 104 proteins that demonstrated significant redox reactions in response to treatment with nCDs. In particular, we found that nCDs specifically induced a conformational change in isocitrate dehydrogenase 1 (IDH1) by selectively reversing the oxidation of cysteine 269 (Cys269). In the mechanism, the site-specific reduction in cysteine 269 (Cys269) triggered a conformational switch of IDH1 that restored mitochondrial α-ketoglutarate flux and NADPH homeostasis, thereby blocking cytosolic mitochondrial DNA (mtDNA) leakage and subsequent cGAS-STING-driven neuroinflammation. Crucially, the nCDs-mediated metabolic checkpoint control inhibited the pro-inflammatory (M1) phenotypes of microglia, thereby achieving therapeutic efficacy in both zebrafish and murine ischemic stroke models, without inducing detectable toxicity. Collectively, we developed a label-free platform enabling in situ decoding of protein corona interactions via redox-sensitive cysteine profiling, eliminating the need for nanoparticle surface modifications.
纳米粒子-蛋白质电冠相互作用对生物反应起着至关重要的作用,但由于缺乏无创分析工具,在生命系统中仍然缺乏表征。在这项研究中,我们开发了一种氧化还原组学策略,通过跟踪纳米颗粒诱导的半胱氨酸硫醇氧化标记物,促进了电晕组成的原位定位。作为研究工具,我们合成了具有双超氧化物歧化酶/模拟过氧化氢酶活性的天然有机物衍生碳点(nCDs)。一项全球氧化还原组学分析发现,104种蛋白质在非传染性疾病治疗中表现出显著的氧化还原反应。特别是,我们发现nCDs通过选择性逆转半胱氨酸269 (Cys269)的氧化,特异性地诱导异柠檬酸脱氢酶1 (IDH1)的构象变化。在其机制中,半胱氨酸269 (Cys269)的位点特异性减少触发IDH1的构象开关,恢复线粒体α-酮戊二酸通量和NADPH稳态,从而阻断细胞质线粒体DNA (mtDNA)泄漏和随后的cgas - sting驱动的神经炎症。至关重要的是,ncds介导的代谢检查点控制抑制了小胶质细胞的促炎(M1)表型,从而在斑马鱼和小鼠缺血性卒中模型中实现了治疗效果,而没有引起可检测到的毒性。总的来说,我们开发了一个无标签的平台,通过氧化还原敏感的半胱氨酸谱分析来原位解码蛋白质电冕相互作用,从而消除了纳米颗粒表面修饰的需要。
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引用次数: 0
Astrocyte-Targeted Nanotherapeutics Modulate Iron Homeostasis in Cerebral Amyloid Angiopathy by Restoring the Astrocytic Trafficking Hub Function 星形胶质细胞靶向纳米疗法通过恢复星形胶质细胞运输枢纽功能调节脑淀粉样血管病中的铁稳态
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c16884
Lingling Zhou,Yanjun Xu,Peng Yang,Jia Zhou,Mingkang Wang,Yixian Li,Xiyu Yang,Xuan Liu,Tianying Wang,Cui Yao,Kang Qian,Jing Wu,Yongkang Mu,Wenxian Du,Yuehua Li,Qizhi Zhang
Cerebral amyloid angiopathy (CAA) is increasingly prevalent, and it is characterized by frequent recurrence and complex etiology. Aberrant ceruloplasmin (Cp) localization at the astrocytic endfeet, coupled with oxidative stress-induced dysregulation of iron regulatory proteins, is a central trigger of the iron dyshomeostasis that drives CAA progression. However, therapeutic strategies that specifically target iron transport regulation in astrocytes remain lacking. Here, we develop lattice-expanded Au/CeO2 with strong antioxidant capacity validated by DFT calculations. Its mesoporous architecture enables the loading of the phospholipase C inhibitor ET-18-OCH3, and further DAG peptide conjugation yields the astrocyte-targeted, biocompatible, and pluripotent nanomedicine DACe@ET. This nanoplatform stabilizes Cp at the astrocytic endfeet and restores the expression of DMT1 and FPN1. By suppressing anomalous Fe2+ influx while promoting efficient efflux and subsequent extracellular oxidation to nontoxic Fe3+, DACe@ET reestablishes a closed-loop Fe2+ export–oxidation system and restores iron homeostasis. In 3 × Tg mice, DACe@ET reduces cerebral iron deposition, decreases amyloid-β burden, attenuates neurodegeneration, and improves cognitive performance. This work demonstrates that restoring astrocytic iron trafficking hub function can serve as an effective therapeutic strategy for CAA, highlighting DACe@ET as a promising disease-modifying therapy with potential applicability to other neurological disorders marked by iron dyshomeostasis while establishing a foundation for future translational research.
脑淀粉样血管病(Cerebral amyloid angiopathy,简称CAA)越来越普遍,其特点是复发频繁、病因复杂。星形细胞端足异常的铜蓝蛋白(Cp)定位,加上氧化应激诱导的铁调节蛋白失调,是驱动CAA进展的铁平衡失调的中心触发因素。然而,专门针对星形胶质细胞铁转运调节的治疗策略仍然缺乏。在这里,我们开发了晶格扩展的Au/CeO2,具有很强的抗氧化能力,经DFT计算验证。它的介孔结构允许装载磷脂酶C抑制剂ET-18-OCH3,进一步的DAG肽偶联产生星形胶质细胞靶向,生物相容性和多能纳米药物DACe@ET。该纳米平台稳定星形细胞端足的Cp,恢复DMT1和FPN1的表达。通过抑制异常的Fe2+内流,同时促进有效的外排和随后的细胞外氧化为无毒的Fe3+, DACe@ET重建了一个闭环Fe2+输出氧化系统,恢复铁稳态。在3 × Tg小鼠中,DACe@ET减少脑铁沉积,减少淀粉样蛋白-β负担,减轻神经变性,提高认知能力。这项工作表明,恢复星形胶质细胞铁转运枢纽功能可以作为CAA的有效治疗策略,强调DACe@ET是一种有前途的疾病修饰疗法,可能适用于其他以铁平衡失调为特征的神经系统疾病,同时为未来的转化研究奠定基础。
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引用次数: 0
Mechanism for Borophene Phase Transition on Substrate 硼罗芬在衬底上的相变机理
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c17811
Maolin Yu,Yangming Gui,Zhiqiang Zhao,Jidong Li,Xu Guo,Zhuhua Zhang
Borophene on the mostly used Ag(111) substrate undergoes a perplexing transition from the v1/6 to the v1/5 phases as temperature increases, but the underlying mechanism remains elusive, hindering fine control over borophene synthesis. Here, we propose that the phase transition is driven by a critical synergy between in-plane migration of boron atoms and their sinking into the substrate. Ab initio calculations show that atoms in the v1/6 phase can migrate to form patches with higher coordination numbers, where atoms are easier to sink into the substrate. Atomic sinking further promotes boron migration, locally nucleating v1/5 domains that eventually expand into a perfect sheet via iterative sinkings and migrations. This temperature-driven, stepwise transition is substantiated by machine-learning-assisted molecular dynamics simulations with an enhanced sampling technique. Moreover, our simulations rationalize the experimental temperature window for synthesizing a series of intermixed v1/6 and v1/5 phases. These findings can inform experimental efforts to achieve structure- and layer-controllable borophene synthesis.
随着温度的升高,常用的Ag(111)衬底上的硼罗芬经历了从v1/6相到v1/5相的复杂转变,但其基本机制尚不清楚,阻碍了对硼罗芬合成的精细控制。在这里,我们提出相变是由硼原子平面内迁移和沉入衬底之间的关键协同作用驱动的。从头计算表明,v1/6相的原子可以迁移形成配位数更高的贴片,原子更容易沉入衬底。原子下沉进一步促进硼迁移,局部成核v1/5结构域,最终通过迭代下沉和迁移扩展成完美的薄片。这种温度驱动的逐步转变通过机器学习辅助的分子动力学模拟和增强的采样技术得到证实。此外,我们的模拟合理化了合成一系列混合的v1/6和v1/5相的实验温度窗。这些发现可以为实现结构和层控硼罗芬合成的实验工作提供信息。
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引用次数: 0
Effect of Stoichiometry in Mo-Based Ordered Double Transition Metal Carbide MXenes on Solid Lubrication and Tribo-Film Formation mo基有序双过渡金属碳化物MXenes化学计量学对固体润滑和摩擦膜形成的影响
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c18644
Dario Zambrano,Bo Wang,Beichen Duan,Javier Marqués Henríquez,Paulina Valenzuela,William Gacitúa,Markus Varga,Manel Rodríguez-Ripoll,Krutarth Kiran Kamath,Brian C. Wyatt,Babak Anasori,Andreas Rosenkranz
MXenes have emerged as promising solid lubricants due to their layered structure, tunable chemistry, and ability to form mechanically robust, wear-resistant tribo-films. However, most studies have focused on single-metal MXenes such as Ti3C2Tx, Ti3CNTx, or V2CTx, leaving multimetal MXenes largely unexplored. Here, we present a comprehensive tribological and mechanochemical evaluation of ordered double-transition metal Mo2TiC2Tx and Mo2Ti2C3Tx coatings under dry sliding in ambient conditions. Using nanoindentation mapping, X-ray photoelectron spectroscopy, Raman spectroscopy, and electron microscopy, we demonstrate that Mo2Ti2C3Tx tends to form dense, chemically stabilized, and mechanically robust tribo-layers thus maintaining a low and stable coefficient of friction (∼0.1) and wear rate (∼0.1 × 10–3 mm3/N·m) under a contact pressure of 0.55 GPa. These tribolayers exhibit improved mechanical properties (hardness ∼ 4.2 GPa; Young’s modulus ∼ 103 GPa), along with increased carbide retention and reduced surface oxidation. In contrast, Mo2TiC2Tx coatings display a less favorable behavior, resulting in a higher COF (∼0.5), greater wear rate (∼1.3 × 10–3 mm3/N·m), and the formation of thinner, chemically degraded tribo-layers under comparable conditions. Mo2Ti2C3Tx exhibited the best tribological and mechanical performance under comparable conditions, clearly outperforming Ti3C2Tx, Ti3CNTx, and Mo2TiC2Tx. Our study introduces Mo-based MXenes as an emerging frontier in solid lubrication and the importance of MXene structure and composition in their tribo-layer evolution and stress accommodation mechanisms.
由于其层状结构、可调节的化学性质以及形成机械坚固、耐磨的摩擦膜的能力,MXenes已成为有前途的固体润滑剂。然而,大多数研究都集中在单金属MXenes上,如Ti3C2Tx、Ti3CNTx或V2CTx,而对多金属MXenes的探索很大程度上是未知的。在此,我们对有序双过渡金属Mo2TiC2Tx和Mo2Ti2C3Tx涂层在干滑动环境下进行了全面的摩擦学和力学评价。利用纳米压痕图、x射线光电子能谱、拉曼光谱和电子显微镜,我们证明了Mo2Ti2C3Tx倾向于形成致密、化学稳定、机械坚固的摩擦层,从而在0.55 GPa的接触压力下保持低而稳定的摩擦系数(~ 0.1)和磨损率(~ 0.1 × 10-3 mm3/N·m)。这些摩擦层表现出改善的机械性能(硬度~ 4.2 GPa;杨氏模量~ 103 GPa),以及增加的碳化物保留和减少的表面氧化。相比之下,Mo2TiC2Tx涂层表现出不太有利的行为,导致更高的COF(~ 0.5),更高的磨损率(~ 1.3 × 10-3 mm3/N·m),并且在相同条件下形成更薄的化学降解摩擦层。在同等条件下,Mo2Ti2C3Tx表现出最佳的摩擦学和力学性能,明显优于Ti3C2Tx、Ti3CNTx和Mo2TiC2Tx。本研究介绍了mo基MXene作为固体润滑领域的新兴前沿,以及MXene结构和组成在摩擦层演化和应力调节机制中的重要性。
{"title":"Effect of Stoichiometry in Mo-Based Ordered Double Transition Metal Carbide MXenes on Solid Lubrication and Tribo-Film Formation","authors":"Dario Zambrano,Bo Wang,Beichen Duan,Javier Marqués Henríquez,Paulina Valenzuela,William Gacitúa,Markus Varga,Manel Rodríguez-Ripoll,Krutarth Kiran Kamath,Brian C. Wyatt,Babak Anasori,Andreas Rosenkranz","doi":"10.1021/acsnano.5c18644","DOIUrl":"https://doi.org/10.1021/acsnano.5c18644","url":null,"abstract":"MXenes have emerged as promising solid lubricants due to their layered structure, tunable chemistry, and ability to form mechanically robust, wear-resistant tribo-films. However, most studies have focused on single-metal MXenes such as Ti3C2Tx, Ti3CNTx, or V2CTx, leaving multimetal MXenes largely unexplored. Here, we present a comprehensive tribological and mechanochemical evaluation of ordered double-transition metal Mo2TiC2Tx and Mo2Ti2C3Tx coatings under dry sliding in ambient conditions. Using nanoindentation mapping, X-ray photoelectron spectroscopy, Raman spectroscopy, and electron microscopy, we demonstrate that Mo2Ti2C3Tx tends to form dense, chemically stabilized, and mechanically robust tribo-layers thus maintaining a low and stable coefficient of friction (∼0.1) and wear rate (∼0.1 × 10–3 mm3/N·m) under a contact pressure of 0.55 GPa. These tribolayers exhibit improved mechanical properties (hardness ∼ 4.2 GPa; Young’s modulus ∼ 103 GPa), along with increased carbide retention and reduced surface oxidation. In contrast, Mo2TiC2Tx coatings display a less favorable behavior, resulting in a higher COF (∼0.5), greater wear rate (∼1.3 × 10–3 mm3/N·m), and the formation of thinner, chemically degraded tribo-layers under comparable conditions. Mo2Ti2C3Tx exhibited the best tribological and mechanical performance under comparable conditions, clearly outperforming Ti3C2Tx, Ti3CNTx, and Mo2TiC2Tx. Our study introduces Mo-based MXenes as an emerging frontier in solid lubrication and the importance of MXene structure and composition in their tribo-layer evolution and stress accommodation mechanisms.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"161 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139000","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
Ultrasmall Platinum Nanoclusters Modulating Dysregulated Reactive Oxide Species and Immunity for Psoriasis Therapy and Prevention 超小铂纳米团簇调节失调的活性氧化物和免疫对银屑病的治疗和预防
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c18716
Kang Liu,Suqing Feng,Xingyu Zhu,Yaru Wang,Wengang Liu,Ting Feng,Haiguang Zhu,Yong Liu,Junlong Geng,Jianping Xie,Xun Yuan
Psoriasis is a chronic inflammatory skin disease that affects millions worldwide. Current treatments are often limited by side effects and high relapse rates. This study introduces an ultrasmall platinum-nanocluster-based artificial enzyme (Pt NE) for effective psoriasis therapy and relapse prevention. Pt NEs exhibit multienzyme mimetic activities─superoxide dismutase, catalase, and glutathione peroxidase-like─with an overall antioxidant capacity 5-fold greater than Au or Cu analogues. Their superior skin penetration (69.93% and 14.27% higher than Au and Cu NEs, respectively) enables efficient reactive oxygen species scavenging and modulation of the inflammatory microenvironment. In vivo, Pt NEs achieve complete psoriatic symptom remission, comparable to a commercial calcipotriol/betamethasone ointment but without steroid-associated adverse effects. Mechanistically, Pt NEs modulate immunity by downregulating pro-inflammatory genes and upregulating genes related to proliferation inhibition and apoptosis. Excellent biocompatibility was observed, with no detectable organ damage or systemic toxicity. This work proposes a safe, effective, and cost-efficient nanotherapeutic strategy with strong potential for clinical translation in psoriasis management.
牛皮癣是一种慢性炎症性皮肤病,影响着全世界数百万人。目前的治疗方法往往受到副作用和高复发率的限制。本研究介绍了一种基于铂纳米簇的超小人工酶(Pt NE),用于有效治疗银屑病和预防复发。Pt NEs具有多酶模拟活性──超氧化物歧化酶、过氧化氢酶和谷胱甘肽过氧化物酶样──其总体抗氧化能力比Au或Cu类似物高5倍。它们优越的皮肤穿透性(分别比Au和Cu NEs高69.93%和14.27%)能够有效清除活性氧并调节炎症微环境。在体内,Pt NEs可以完全缓解银屑病症状,与市售的钙化三醇/倍他米松软膏相当,但没有类固醇相关的不良反应。在机制上,Pt NEs通过下调促炎基因和上调与增殖抑制和细胞凋亡相关的基因来调节免疫。观察到良好的生物相容性,无可检测到的器官损伤或全身毒性。这项工作提出了一种安全、有效、成本效益高的纳米治疗策略,在牛皮癣的临床治疗中具有很强的潜力。
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引用次数: 0
Ultralow-Temperature Synthesis of Two-Dimensional Anisotropic FeOCl and Quasi-One-Dimensional Moiré Superlattices 二维各向异性FeOCl和准一维莫尔条纹超晶格的超低温合成
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-09 DOI: 10.1021/acsnano.5c19178
Zemin Zheng,Jiuxiang Dai,Ang Li,Meng Gao,Yuanyuan Qiu,Xingxing Zhang,Zhitong Jin,Mo Cheng,Hongshuai Cao,Qingqing Ji,Wu Zhou,Teng Yang,Lin Zhou
Two-dimensional (2D) materials, with an atomic thickness and exceptional properties, hold great promise for next-generation devices and flexible electronics. However, these applications face integration challenges due to high-temperature synthesis and transfer-induced degradation. Here, we demonstrate the ultralow-temperature growth of high-quality 2D FeOCl, enabling its direct integration into heterostructures and flexible substrates. The synthesized 2D FeOCl exhibits high crystallinity, uniformity, and intrinsic structural and optical anisotropy. Using this method, we synthesized FeOCl-based vertical heterostructures on both layered 2D MoS2 and nonlayered 2D Fe3O4. The heterostructures exhibit highly ordered quasi-one-dimensional moiré superlattices and anisotropic second harmonic generation (SHG) patterns. Theoretical calculations attribute these properties to anisotropic charge redistribution at the interfaces. This work establishes a versatile low-temperature platform for synthesizing and integrating 2D materials, providing both a pathway for polarization-sensitive optoelectronics and spintronic devices and a scalable synthetic route to explore emergent one-dimensional (1D) quantum physics.
二维(2D)材料具有原子厚度和特殊性能,对下一代设备和柔性电子产品具有很大的希望。然而,由于高温合成和转移诱导降解,这些应用面临集成挑战。在这里,我们展示了高质量二维FeOCl的超低温生长,使其能够直接集成到异质结构和柔性衬底中。合成的二维FeOCl具有较高的结晶度、均匀性以及固有的结构和光学各向异性。利用这种方法,我们在层状二维MoS2和非层状二维Fe3O4上合成了基于feocl的垂直异质结构。异质结构表现出高度有序的准一维莫尔条纹超晶格和各向异性二次谐波产生模式。理论计算将这些特性归因于界面上电荷的各向异性再分配。本工作为二维材料的合成和集成建立了一个多功能的低温平台,为极化敏感光电子和自旋电子器件提供了一条途径,并为探索新兴一维(1D)量子物理提供了一条可扩展的合成途径。
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引用次数: 0
Ultrafast Activity Tuning and Kilogram-Scale Synthesis of Fe–N–C Catalysts via Confinement-Engineered Joule Heating 基于焦耳加热的Fe-N-C催化剂的超快活性调谐和公斤级合成
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-08 DOI: 10.1021/acsnano.6c00048
Guobin Qin,Xiaoxiong Li,Danna Wu,Hai-Gang Lu,Gaoyi Han,Sheng Zhu,Yan Li
Atomically dispersed Fe–N–C catalysts with well-defined iron–nitrogen coordination exhibit fantastic promise for the oxygen reduction reaction (ORR). However, achieving their scalable synthesis while preventing iron aggregation and performance degradation remains a critical challenge. Here, we demonstrate a highly efficient confined flash Joule heating (CFJH) technique for the scalable and ultrafast synthesis of Fe–N–C catalysts. The coal-derived porous carbons are efficient in confining iron phthalocyanine (FePc) molecules, suppressing their migration and iron aggregation during ultrafast CFJH treatment. This process facilitates the conversion of FePc into atomically dispersed FeN4 sites embedded within a graphitization-enhanced carbon framework. Mechanistic studies reveal that, compared to an FePc precursor, these integrated FeN4 sites exhibit a shifted rate-determining step with optimized adsorption/desorption of oxygen intermediates, leading to a reduced energy barrier for efficient 4e– oxygen reduction. The resulting catalyst exhibits impressive ORR activity in alkaline media with a high half-wave potential (0.90 V vs RHE) and remarkable durability (94.5% retention over 100 h). The assembled zinc-air battery delivers a peak power density of 277.6 mW cm–2 and sustains stable operation for over 900 h, outperforming the Pt/C + IrO2 benchmark. Scalable production is achieved at a rate of 0.5 kg h–1, establishing a facile and industrially viable route for synthesizing high-performance atomically dispersed catalysts.
具有明确的铁氮配位的原子分散Fe-N-C催化剂在氧还原反应(ORR)中表现出良好的应用前景。然而,在防止铁聚集和性能下降的同时实现可扩展的合成仍然是一个关键的挑战。在这里,我们展示了一种高效的限制闪蒸焦耳加热(CFJH)技术,用于可扩展和超快合成Fe-N-C催化剂。在超快CFJH处理过程中,煤衍生多孔碳能有效地限制酞菁铁(FePc)分子,抑制其迁移和铁聚集。这一过程有助于将FePc转化为嵌入石墨化增强碳框架内的原子分散的FeN4位点。机理研究表明,与FePc前驱体相比,这些集成的FeN4位点表现出一个移位的速率决定步骤,优化了氧中间体的吸附/解吸,从而降低了有效还原4e -氧的能量垒。所得催化剂在碱性介质中表现出令人印象深刻的ORR活性,具有高半波电位(0.90 V vs RHE)和显着的耐久性(100小时内保持率为94.5%)。组装的锌空气电池提供277.6 mW cm-2的峰值功率密度,并保持超过900小时的稳定运行,优于Pt/C + IrO2基准。在0.5 kg h-1的速率下实现了规模化生产,为合成高性能原子分散催化剂建立了一条简单可行的工业路线。
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引用次数: 0
Dynamic Simulation Assists Insights into the Deafness Prevention of a Self-Assembly Pd Nanozyme with Intrinsic Targeting 动态模拟有助于深入了解具有内在靶向的自组装Pd纳米酶的耳聋预防
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-08 DOI: 10.1021/acsnano.5c19608
Qin Huo,Guanrun Wang,Yanmei Mo,Guohui Nie,Bin Zhang
With aging increases the possibility of body impairment, deafness prevention remains a major unmet clinical challenge, largely due to the lack of effective therapeutics capable of targeting cochlear hair cells (HCs) across the blood–labyrinth barrier (BLB). Here, we report a precisely structured palladium-polyoxometalate coordinated antioxidant nanoagent (Pd single-atom nanozyme, Pd SAN), which demonstrates superior antioxidative enzyme-like capacity and robust biosafety. With identical Pd1–O4 coordinating sites and controllable size, Pd SAN effectively penetrates the BLB, accumulates within the cochlea, and protects HCs from neomycin-induced damage. Mechanistically, Pd SAN inhibits ferroptosis by preserving glutathione redox balance, reducing lipid peroxidation, stabilizing lysosomal membranes, and maintaining Fe2+ homeostasis. Notably, dynamic simulation demonstrates that Pd SAN shows comparable binding affinity to critical HC proteins (Prestin, Myo7a) as superoxide dismutase (SOD), and functionally suppresses neomycin-induced ferroptosis with equal or greater efficacy. In vivo experiments confirm that Pd SAN prevents auditory threshold shifts and mitigates cochlear structural injury, underscoring its translational potential. This study not only reveals that lysosomal damage–iron metabolism dysregulation–oxidative stress is a key axis driving aminoglycoside ototoxicity, but also establishes Pd SAN whose structure can be accurately deciphered with mass spectroscopy as an innovatively designed cochlea-targeting antioxidant nanomaterial with strong potential for clinical translation in deafness prevention.
随着年龄的增长,身体损伤的可能性增加,耳聋预防仍然是一个主要的未满足的临床挑战,主要是由于缺乏有效的治疗方法能够跨越血液迷宫屏障(BLB)靶向耳蜗毛细胞(hc)。在这里,我们报道了一种精确结构的钯-多金属氧酸盐协同抗氧化纳米剂(Pd单原子纳米酶,Pd SAN),它具有优异的抗氧化酶样能力和强大的生物安全性。Pd - SAN具有相同的Pd1-O4配位位点和可控制的大小,可有效穿透BLB,在耳蜗内蓄积,保护hc免受新霉素引起的损伤。从机制上讲,Pd - SAN通过保持谷胱甘肽氧化还原平衡、减少脂质过氧化、稳定溶酶体膜和维持Fe2+稳态来抑制铁下垂。值得注意的是,动态模拟表明Pd - SAN与关键HC蛋白(Prestin, Myo7a)的结合亲和力与超氧化物歧化酶(SOD)相当,并且在功能上抑制新霉素诱导的铁凋亡具有相同或更高的功效。体内实验证实,Pd - SAN可防止听阈值移位,减轻耳蜗结构损伤,强调其翻译潜力。本研究不仅揭示了溶酶体损伤-铁代谢失调-氧化应激是驱动氨基糖苷耳毒性的关键轴,而且还建立了一种结构可通过质谱准确破译的Pd SAN,作为一种创新设计的耳蜗靶向抗氧化纳米材料,在耳聋预防方面具有很强的临床转化潜力。
{"title":"Dynamic Simulation Assists Insights into the Deafness Prevention of a Self-Assembly Pd Nanozyme with Intrinsic Targeting","authors":"Qin Huo,Guanrun Wang,Yanmei Mo,Guohui Nie,Bin Zhang","doi":"10.1021/acsnano.5c19608","DOIUrl":"https://doi.org/10.1021/acsnano.5c19608","url":null,"abstract":"With aging increases the possibility of body impairment, deafness prevention remains a major unmet clinical challenge, largely due to the lack of effective therapeutics capable of targeting cochlear hair cells (HCs) across the blood–labyrinth barrier (BLB). Here, we report a precisely structured palladium-polyoxometalate coordinated antioxidant nanoagent (Pd single-atom nanozyme, Pd SAN), which demonstrates superior antioxidative enzyme-like capacity and robust biosafety. With identical Pd1–O4 coordinating sites and controllable size, Pd SAN effectively penetrates the BLB, accumulates within the cochlea, and protects HCs from neomycin-induced damage. Mechanistically, Pd SAN inhibits ferroptosis by preserving glutathione redox balance, reducing lipid peroxidation, stabilizing lysosomal membranes, and maintaining Fe2+ homeostasis. Notably, dynamic simulation demonstrates that Pd SAN shows comparable binding affinity to critical HC proteins (Prestin, Myo7a) as superoxide dismutase (SOD), and functionally suppresses neomycin-induced ferroptosis with equal or greater efficacy. In vivo experiments confirm that Pd SAN prevents auditory threshold shifts and mitigates cochlear structural injury, underscoring its translational potential. This study not only reveals that lysosomal damage–iron metabolism dysregulation–oxidative stress is a key axis driving aminoglycoside ototoxicity, but also establishes Pd SAN whose structure can be accurately deciphered with mass spectroscopy as an innovatively designed cochlea-targeting antioxidant nanomaterial with strong potential for clinical translation in deafness prevention.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139036","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
In Situ Observation of Triple-Phase Interface during Electrocatalytic CO2 Reduction 电催化CO2还原过程中三相界面的原位观察
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2026-02-08 DOI: 10.1021/acsnano.5c19098
Zezhong Xie,Jinli Yu,Hao Yang,Jian Chen,Muzi Yang,Mingyang Li,Kun Wang,Qiushi Wang,Kai-Hang Ye,Gangfeng Ouyang
The solid–liquid–gas triple-phase interface in the CO2 electro-reduction reaction (CO2RR) is pivotal for determining catalytic activity and selectivity, as it influences both the kinetics and thermodynamics of the reactions. However, observing this interface in situ is challenging because it forms at the interface among the solid catalyst, the flowing electrolyte, and the turbulent CO2. To address the issues, we achieved unobstructed in situ Raman observations at the microscale by developing a straightforward catalyst-integrated gas diffusion electrode (GDE). This monolithic GDE, featuring a biomimetic hydrophobic structure, fully releases the triple-phase interface─an essential prerequisite for enabling the in situ detection. Characterizations reveal that the microenvironment at the triple-phase interface significantly enhances multicarbon (C2+) selectivity. Furthermore, using advanced in situ 3D Raman tomography, we successfully visualized the spatial distribution of the triple-phase interface with high precision. The integration of in situ Raman spectroscopy with computational modeling has provided invaluable insights into the evolution of species within the microenvironment, elucidating a high local pH and rapid CO2 mass transfer at the triple-phase interface.
在CO2电还原反应(CO2RR)中,固液气三相界面是决定催化活性和选择性的关键,因为它影响反应的动力学和热力学。然而,原位观察该界面具有挑战性,因为它形成于固体催化剂、流动电解质和湍流CO2之间的界面。为了解决这些问题,我们通过开发一种直接的催化剂集成气体扩散电极(GDE),在微观尺度上实现了无阻碍的原位拉曼观测。这种单片GDE具有仿生疏水结构,完全释放三相界面,这是实现原位检测的必要先决条件。表征表明,三相界面微环境显著提高了多碳(C2+)的选择性。此外,利用先进的原位三维拉曼层析成像技术,我们成功地实现了三相界面空间分布的高精度可视化。原位拉曼光谱与计算模型的集成为微环境中物种的进化提供了宝贵的见解,阐明了高局部pH值和三相界面上快速的CO2传质。
{"title":"In Situ Observation of Triple-Phase Interface during Electrocatalytic CO2 Reduction","authors":"Zezhong Xie,Jinli Yu,Hao Yang,Jian Chen,Muzi Yang,Mingyang Li,Kun Wang,Qiushi Wang,Kai-Hang Ye,Gangfeng Ouyang","doi":"10.1021/acsnano.5c19098","DOIUrl":"https://doi.org/10.1021/acsnano.5c19098","url":null,"abstract":"The solid–liquid–gas triple-phase interface in the CO2 electro-reduction reaction (CO2RR) is pivotal for determining catalytic activity and selectivity, as it influences both the kinetics and thermodynamics of the reactions. However, observing this interface in situ is challenging because it forms at the interface among the solid catalyst, the flowing electrolyte, and the turbulent CO2. To address the issues, we achieved unobstructed in situ Raman observations at the microscale by developing a straightforward catalyst-integrated gas diffusion electrode (GDE). This monolithic GDE, featuring a biomimetic hydrophobic structure, fully releases the triple-phase interface─an essential prerequisite for enabling the in situ detection. Characterizations reveal that the microenvironment at the triple-phase interface significantly enhances multicarbon (C2+) selectivity. Furthermore, using advanced in situ 3D Raman tomography, we successfully visualized the spatial distribution of the triple-phase interface with high precision. The integration of in situ Raman spectroscopy with computational modeling has provided invaluable insights into the evolution of species within the microenvironment, elucidating a high local pH and rapid CO2 mass transfer at the triple-phase interface.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"45 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138941","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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ACS Nano
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