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。
{"title":"Dual-Field Amplification via Nanotip-Engineered Catalysts for Efficient Spin-State and Ion Regulation in Aluminum–Sulfur Batteries","authors":"Xingjun Liu,Jinghan Wang,Jiqiang Zhan,Qixin Wang,Xiaojing Lin,Hongpeng Li,Hongsen Li","doi":"10.1021/acsnano.5c16319","DOIUrl":"https://doi.org/10.1021/acsnano.5c16319","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"31 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138996","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}
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.
{"title":"In Situ Redox-Omics Decoding of Nanoparticle–Protein Corona Interactions Drives the Mitochondrial Metabolic-Immunological Mechanism in Microglia","authors":"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","doi":"10.1021/acsnano.5c21740","DOIUrl":"https://doi.org/10.1021/acsnano.5c21740","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139085","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}
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.
{"title":"Astrocyte-Targeted Nanotherapeutics Modulate Iron Homeostasis in Cerebral Amyloid Angiopathy by Restoring the Astrocytic Trafficking Hub Function","authors":"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","doi":"10.1021/acsnano.5c16884","DOIUrl":"https://doi.org/10.1021/acsnano.5c16884","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"3 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138997","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}
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.
{"title":"Mechanism for Borophene Phase Transition on Substrate","authors":"Maolin Yu,Yangming Gui,Zhiqiang Zhao,Jidong Li,Xu Guo,Zhuhua Zhang","doi":"10.1021/acsnano.5c17811","DOIUrl":"https://doi.org/10.1021/acsnano.5c17811","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"241 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138998","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}
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.
{"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}
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.
{"title":"Ultrasmall Platinum Nanoclusters Modulating Dysregulated Reactive Oxide Species and Immunity for Psoriasis Therapy and Prevention","authors":"Kang Liu,Suqing Feng,Xingyu Zhu,Yaru Wang,Wengang Liu,Ting Feng,Haiguang Zhu,Yong Liu,Junlong Geng,Jianping Xie,Xun Yuan","doi":"10.1021/acsnano.5c18716","DOIUrl":"https://doi.org/10.1021/acsnano.5c18716","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"24 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139001","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}
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.
{"title":"Ultralow-Temperature Synthesis of Two-Dimensional Anisotropic FeOCl and Quasi-One-Dimensional Moiré Superlattices","authors":"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","doi":"10.1021/acsnano.5c19178","DOIUrl":"https://doi.org/10.1021/acsnano.5c19178","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"4 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139002","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}
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。
{"title":"Ultrafast Activity Tuning and Kilogram-Scale Synthesis of Fe–N–C Catalysts via Confinement-Engineered Joule Heating","authors":"Guobin Qin,Xiaoxiong Li,Danna Wu,Hai-Gang Lu,Gaoyi Han,Sheng Zhu,Yan Li","doi":"10.1021/acsnano.6c00048","DOIUrl":"https://doi.org/10.1021/acsnano.6c00048","url":null,"abstract":"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.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"36 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-02-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139037","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}
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.
{"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}
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.
{"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}