Chuang Yuan,Hongli Li,Yunlong Gao,Rui Zeng,Zichao Luo,Xinyu Yang
Sepsis accounts for 20% of global mortality, largely driven by dysregulated hyperactivation of macrophages that disrupts immune homeostasis. Current anti-inflammatory strategies often compromise pathogen clearance and exacerbate immunosuppression. Precisely targeting hyperactivated macrophages while preserving antimicrobial function represents a promising therapeutic approach. Through high-throughput screening of 390 kinase inhibitors in hyperactivated macrophages, we identified the polo-like kinase 1 (PLK1) inhibitor GSK461364 as a potent modulator of hyperactivation. However, its clinical translation is limited by dose-dependent cytotoxicity and systemic toxicity. To address this, we engineered mannose-functionalized nanoparticles (Nano-PLK1in) for targeted combinatorial delivery of the inhibitor and glutathione to hyperactive macrophages. These nanoparticles significantly enhanced cellular uptake, approximately 2-fold, in both murine and human hyperactivated macrophages. The triple-action Nano-PLK1in platform enables: (i) precision inhibition of the caspase-11 pathway via PLK1 blockade, (ii) reactivation of redox homeostasis through glutathione-mediated mitochondrial protection, and (iii) preservation of antimicrobial capacity without broad immunosuppression. In murine models of sepsis, Nano-PLK1in markedly improved survival by 50% compared to free drug, along with a 41.8% reduction in coagulopathy and a 28.9-54.3% decrease in ALT/creatinine levels reflecting multiorgan protection, and enhanced bacterial clearance. By integrating precision macrophage reprogramming with effective pathogen eradication, our nanoscale engineering strategy surmounts the efficacy-toxicity trade-off of conventional therapies, highlighting its translational promise for sepsis treatment.
{"title":"An Engineered Triple-Functional Nanoplatform for Effective Sepsis Therapy via Macrophage-Targeted Polo-like Kinase 1 Inhibition.","authors":"Chuang Yuan,Hongli Li,Yunlong Gao,Rui Zeng,Zichao Luo,Xinyu Yang","doi":"10.1021/acsnano.5c20947","DOIUrl":"https://doi.org/10.1021/acsnano.5c20947","url":null,"abstract":"Sepsis accounts for 20% of global mortality, largely driven by dysregulated hyperactivation of macrophages that disrupts immune homeostasis. Current anti-inflammatory strategies often compromise pathogen clearance and exacerbate immunosuppression. Precisely targeting hyperactivated macrophages while preserving antimicrobial function represents a promising therapeutic approach. Through high-throughput screening of 390 kinase inhibitors in hyperactivated macrophages, we identified the polo-like kinase 1 (PLK1) inhibitor GSK461364 as a potent modulator of hyperactivation. However, its clinical translation is limited by dose-dependent cytotoxicity and systemic toxicity. To address this, we engineered mannose-functionalized nanoparticles (Nano-PLK1in) for targeted combinatorial delivery of the inhibitor and glutathione to hyperactive macrophages. These nanoparticles significantly enhanced cellular uptake, approximately 2-fold, in both murine and human hyperactivated macrophages. The triple-action Nano-PLK1in platform enables: (i) precision inhibition of the caspase-11 pathway via PLK1 blockade, (ii) reactivation of redox homeostasis through glutathione-mediated mitochondrial protection, and (iii) preservation of antimicrobial capacity without broad immunosuppression. In murine models of sepsis, Nano-PLK1in markedly improved survival by 50% compared to free drug, along with a 41.8% reduction in coagulopathy and a 28.9-54.3% decrease in ALT/creatinine levels reflecting multiorgan protection, and enhanced bacterial clearance. By integrating precision macrophage reprogramming with effective pathogen eradication, our nanoscale engineering strategy surmounts the efficacy-toxicity trade-off of conventional therapies, highlighting its translational promise for sepsis treatment.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"87 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495094","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}
Precise control of light-matter interactions is a cornerstone of next-generation technologies, from ultrasensitive biosensing and single-molecule tracking to the development of adaptive metamaterials. While small, symmetric nanostructures are well-understood, micrometer-scale plasmonic Janus particles (pJPs), comprising dielectric cores with thin metallic caps, exhibit complex optical properties due to their asymmetric structure. Despite widespread applications in active matter research, their orientation-dependent scattering properties remain largely unexplored. We introduce Fourier plane tomographic spectroscopy for simultaneous four-dimensional characterization of scattering from individual micrometer-scale particles across wavelength, incident angle, and scattering angle. Combining measurements with finite-element simulations, we identify discrete spectral markers in visible and near-infrared regions that evolve predictably with cap orientation. Spherical-harmonics decomposition reveals that these markers arise from three distinct multipolar modes up to fifth order: axial-propagating transverse-electric, transverse-propagating transverse-electric, and transverse-propagating axial-electric, with retardation-induced splitting. We observe progressive red-shifts and line width narrowing of higher-order resonances, demonstrating curvature's influence on mode dispersion. Orientation-specific scattering patterns exhibit polarization-dependent features enabling optical tracking of particle rotation. Beyond pJPs, this methodology establishes a general framework for characterizing asymmetric nanostructures of diverse material combinations and geometries, offering a toolkit for designing orientation-responsive nanoantennas, reconfigurable metasurfaces, active colloidal systems with tailored light-matter interactions, and high-precision optical tracking of particle rotation.
{"title":"Fourier Plane Tomographic Spectroscopy Reveals Orientation-Dependent Multipolar Plasmon Modes in Micrometer-Scale Janus Particles.","authors":"Felix H Patzschke, Frank Cichos","doi":"10.1021/acsnano.6c01771","DOIUrl":"https://doi.org/10.1021/acsnano.6c01771","url":null,"abstract":"<p><p>Precise control of light-matter interactions is a cornerstone of next-generation technologies, from ultrasensitive biosensing and single-molecule tracking to the development of adaptive metamaterials. While small, symmetric nanostructures are well-understood, micrometer-scale plasmonic Janus particles (pJPs), comprising dielectric cores with thin metallic caps, exhibit complex optical properties due to their asymmetric structure. Despite widespread applications in active matter research, their orientation-dependent scattering properties remain largely unexplored. We introduce Fourier plane tomographic spectroscopy for simultaneous four-dimensional characterization of scattering from individual micrometer-scale particles across wavelength, incident angle, and scattering angle. Combining measurements with finite-element simulations, we identify discrete spectral markers in visible and near-infrared regions that evolve predictably with cap orientation. Spherical-harmonics decomposition reveals that these markers arise from three distinct multipolar modes up to fifth order: axial-propagating transverse-electric, transverse-propagating transverse-electric, and transverse-propagating axial-electric, with retardation-induced splitting. We observe progressive red-shifts and line width narrowing of higher-order resonances, demonstrating curvature's influence on mode dispersion. Orientation-specific scattering patterns exhibit polarization-dependent features enabling optical tracking of particle rotation. Beyond pJPs, this methodology establishes a general framework for characterizing asymmetric nanostructures of diverse material combinations and geometries, offering a toolkit for designing orientation-responsive nanoantennas, reconfigurable metasurfaces, active colloidal systems with tailored light-matter interactions, and high-precision optical tracking of particle rotation.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":16.0,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502705","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}
Micro/nanomotors hold promise for remote manipulation in complex biological environments. However, integrating robust barrier penetration, real-time tracking, and effective theranostics within a motor system remains a formidable translational challenge. Here, we engineer sequential magneto-actuated and optically imageable biohybrid micromotors (BAMs) for precise tumor therapy. BAMs consist of two components, magnetospirillum bacteria (AMB-1), enabling autonomous tumor tropism via hypoxia-driven chemotaxis and magnetic navigation under external fields, and extracellularly biomineralized Ag2S quantum dots, serving as near-infrared (NIR)-II fluorescence imaging agents and photothermal converters. In vivo studies demonstrate that BAMs can migrate to the hypoxic core of the tumors through the synergistic effect of hypoxia-targeting chemotaxis and magnetic actuation, which can be monitored via NIR-II fluorescence imaging. Moreover, as a photothermal therapeutic agent, BAMs effectively induce tumor cell apoptosis and suppress tumor growth through photothermal conversion. This innovative BAMs platform not only overcomes passive diffusion but also provides precise theranostics through integrated magnetic guidance, NIR-II imaging, and photothermal therapy, showcasing the promise of biohybrid systems.
{"title":"Engineered Magnetobacterial Microrobots with Tunable Self-Mineralization for Precise Imaging-Guided Photothermal Therapy.","authors":"Hui Ran,Lishan Zhang,Yicheng Ye,Ning Zhong,Yuanyuan Wang,Bingquan Huang,Yuejun Jiang,Xue Yang,Qiuyun Wei,Hao Tian,Fei Peng,Yingfeng Tu","doi":"10.1021/acsnano.5c19758","DOIUrl":"https://doi.org/10.1021/acsnano.5c19758","url":null,"abstract":"Micro/nanomotors hold promise for remote manipulation in complex biological environments. However, integrating robust barrier penetration, real-time tracking, and effective theranostics within a motor system remains a formidable translational challenge. Here, we engineer sequential magneto-actuated and optically imageable biohybrid micromotors (BAMs) for precise tumor therapy. BAMs consist of two components, magnetospirillum bacteria (AMB-1), enabling autonomous tumor tropism via hypoxia-driven chemotaxis and magnetic navigation under external fields, and extracellularly biomineralized Ag2S quantum dots, serving as near-infrared (NIR)-II fluorescence imaging agents and photothermal converters. In vivo studies demonstrate that BAMs can migrate to the hypoxic core of the tumors through the synergistic effect of hypoxia-targeting chemotaxis and magnetic actuation, which can be monitored via NIR-II fluorescence imaging. Moreover, as a photothermal therapeutic agent, BAMs effectively induce tumor cell apoptosis and suppress tumor growth through photothermal conversion. This innovative BAMs platform not only overcomes passive diffusion but also provides precise theranostics through integrated magnetic guidance, NIR-II imaging, and photothermal therapy, showcasing the promise of biohybrid systems.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"14 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502242","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}
Al current collectors are widely adopted in nonaqueous batteries because of their low cost, high conductivity, and low density, yet their deployment in aqueous congeners (i.e., Zn-ion batteries) is largely precluded by concurrent issues of surface passivation and electrolyte-driven corrosion. Here, an on-site N-doped carbon-skinned Al current collector (NC@Al) is developed to resolve this longstanding dilemma. Enabled by an ultrafast Joule heating process, elevated temperature carbonization could be completed in seconds without thermally deforming the Al substrate, which renders a dense and continuous double-sided NC overlayer, affording favorable interfacial adhesion. Combined theoretical calculations and experimental diagnostics verify the NC overlayer simultaneously helps suppress the Al passivation-corrosion issue and promote uniform Zn deposition. As a result, symmetric cells based on NC@Al exhibit durable cycling beyond 3500 h at 0.5 mA cm-2/0.25 mAh cm-2. When paired with an iodine cathode, our constructed pouch cells with an active material loading of 25 mg cm-2 sustain stable operation for 1000 cycles under a stringent N/P ratio of 1.77. Technoeconomic analysis further highlights the energy-efficiency advantage of our route in practical manufacturing. This work establishes a strategy for employing commercially available Al current collector materials toward aqueous batteries.
铝集流器由于其低成本、高导电性和低密度而被广泛应用于非水电池中，但由于表面钝化和电解质驱动的腐蚀问题，它们在水电池（即锌离子电池）中的应用在很大程度上被排除在外。在这里，一个现场n掺杂碳皮铝电流收集器（NC@Al）被开发来解决这个长期存在的难题。通过超快焦耳加热工艺，可以在几秒钟内完成高温碳化，而不会使Al衬底发生热变形，从而形成致密连续的双面NC覆层，提供良好的界面附着力。理论计算和实验诊断相结合，验证了NC覆盖层同时有助于抑制Al钝化腐蚀问题和促进均匀Zn沉积。因此，基于NC@Al的对称电池在0.5 mA cm-2/0.25 mAh cm-2下表现出超过3500小时的持久循环。当与碘阴极配对时，我们构建的活性材料负载为25 mg cm-2的袋状电池在严格的N/P比为1.77的条件下可稳定运行1000次。技术经济分析进一步强调了我们的路线在实际制造中的节能优势。这项工作建立了一种将市售铝集流材料用于水性电池的策略。
{"title":"Overcoming Passivation-Corrosion Dilemma of Al Current Collector for Aqueous Zn Battery.","authors":"Zixiang Meng,Yuhan Zou,Jiashu Chen,Yongbiao Mu,Yan Li,Yuyuan Wang,Qian Liu,Yuyang Yi,Lin Zeng,Guangping Zheng,Shixue Dou,Jingyu Sun","doi":"10.1021/acsnano.6c02382","DOIUrl":"https://doi.org/10.1021/acsnano.6c02382","url":null,"abstract":"Al current collectors are widely adopted in nonaqueous batteries because of their low cost, high conductivity, and low density, yet their deployment in aqueous congeners (i.e., Zn-ion batteries) is largely precluded by concurrent issues of surface passivation and electrolyte-driven corrosion. Here, an on-site N-doped carbon-skinned Al current collector (NC@Al) is developed to resolve this longstanding dilemma. Enabled by an ultrafast Joule heating process, elevated temperature carbonization could be completed in seconds without thermally deforming the Al substrate, which renders a dense and continuous double-sided NC overlayer, affording favorable interfacial adhesion. Combined theoretical calculations and experimental diagnostics verify the NC overlayer simultaneously helps suppress the Al passivation-corrosion issue and promote uniform Zn deposition. As a result, symmetric cells based on NC@Al exhibit durable cycling beyond 3500 h at 0.5 mA cm-2/0.25 mAh cm-2. When paired with an iodine cathode, our constructed pouch cells with an active material loading of 25 mg cm-2 sustain stable operation for 1000 cycles under a stringent N/P ratio of 1.77. Technoeconomic analysis further highlights the energy-efficiency advantage of our route in practical manufacturing. This work establishes a strategy for employing commercially available Al current collector materials toward aqueous batteries.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"17 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495098","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}
Yi-Cheng Wang,Yan Liu,Chenyu Xu,Peng-Fei Sui,Yi Liu,Renfei Feng,Xiaolei Wang,Jing-Li Luo
The photoelectrochemical CO2 reduction reaction (PEC CO2RR) to syngas is of great significance for meeting the needs of the green chemical industry, and controlling the CO/H2 ratio is an important issue. However, the reliance on thin-film semiconductor photocathodes significantly limits the available fabrication methods, and some of the proposed schemes have not been able to precisely tune the CO/H2 ratio by indirectly regulating the electronic structure of active sites. In order to overcome the limitations of traditional fabrication methods, this work proposes a simple photodeposition method for loading Cu2-xTe onto 1% S-doped ZnTe/ZnO to regulate the oxidation state of Cu between +1 and +2 by precisely controlling the deposition light wavelength from violet to red. With shorter deposition light wavelengths, the photon energy increases, leading to a reduced valence state of Cu. As the Cu oxidation state decreases, the band structure of Cu2-xTe-ZnTe can be modulated, with the overall d-band center shifting toward the Fermi level. Besides, the electron density around the Cu active sites increases due to the shorter Cu-Cu bond, resulting in stabilized reaction intermediates and a faster charge transfer process, leading to higher CO selectivity with suppressed hydrogen evolution reaction. As a result, Cu@S-ZnTe/ZnO shows a tunable CO/H2 molar ratio ranging from 0.45 to 1.70 by adjusting the oxidation state of Cu, which can be precisely controlled by simply varying the deposition light wavelength with a specific filter. This demonstrates the great potential of the proposed photodeposition method and the resulting photoelectrocatalyst for practical PEC CO2RR applications.
{"title":"Wavelength-Tailoring Copper Oxidation States for Tunable Photoelectrochemical Syngas Generation.","authors":"Yi-Cheng Wang,Yan Liu,Chenyu Xu,Peng-Fei Sui,Yi Liu,Renfei Feng,Xiaolei Wang,Jing-Li Luo","doi":"10.1021/acsnano.5c21792","DOIUrl":"https://doi.org/10.1021/acsnano.5c21792","url":null,"abstract":"The photoelectrochemical CO2 reduction reaction (PEC CO2RR) to syngas is of great significance for meeting the needs of the green chemical industry, and controlling the CO/H2 ratio is an important issue. However, the reliance on thin-film semiconductor photocathodes significantly limits the available fabrication methods, and some of the proposed schemes have not been able to precisely tune the CO/H2 ratio by indirectly regulating the electronic structure of active sites. In order to overcome the limitations of traditional fabrication methods, this work proposes a simple photodeposition method for loading Cu2-xTe onto 1% S-doped ZnTe/ZnO to regulate the oxidation state of Cu between +1 and +2 by precisely controlling the deposition light wavelength from violet to red. With shorter deposition light wavelengths, the photon energy increases, leading to a reduced valence state of Cu. As the Cu oxidation state decreases, the band structure of Cu2-xTe-ZnTe can be modulated, with the overall d-band center shifting toward the Fermi level. Besides, the electron density around the Cu active sites increases due to the shorter Cu-Cu bond, resulting in stabilized reaction intermediates and a faster charge transfer process, leading to higher CO selectivity with suppressed hydrogen evolution reaction. As a result, Cu@S-ZnTe/ZnO shows a tunable CO/H2 molar ratio ranging from 0.45 to 1.70 by adjusting the oxidation state of Cu, which can be precisely controlled by simply varying the deposition light wavelength with a specific filter. This demonstrates the great potential of the proposed photodeposition method and the resulting photoelectrocatalyst for practical PEC CO2RR applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"15 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147495101","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}
Harvesting freshwater and hydroenergy through evaporation from seawater simultaneously and efficiently is highly preferred for various applications but remains a challenge owing to mutually exclusive requirements: Efficient water-energy harvesting necessitates the presence of a thin water film on engineered evaporator surfaces to promote evaporation current, whereas efficient freshwater generation demands rapid bulk water transport. To decouple these originally conflicting requirements, we present a 3D modular architecture decorated with nanoscale channels that imparts rapid thin-film evaporation, enabling simultaneous and efficient cogeneration of water-electricity from seawater. The modular units endow the rapid transport of seawater in confined nanoscale channels and effective thin-film evaporation. Under 1 sun irradiation, the modular water-electricity cogenerator (MWEG) reaches a current density of 1.58 mA cm-2, power density of 1.2 W m-2, and high evaporation rate of 2.69 kg m-2 h-1. In addition, under an outdoor light concentration of up to 10 sun, the power density and evaporation rate of MWEG can be significantly increased to 4.3 W m-2 and 27.5 kg m-2 h-1, respectively. These performances demonstrate the vast potential of harnessing the evaporation of Earth's seawater to address shortages of both energy and water.
通过海水蒸发同时高效地收集淡水和水能是各种应用的首选，但由于相互排斥的要求，仍然存在挑战：高效的水能收集需要在工程蒸发器表面存在薄水膜以促进蒸发电流，而高效的淡水发电需要快速的大量水运输。为了解耦这些最初相互冲突的需求，我们提出了一种3D模块化架构，装饰有纳米级通道，可以使薄膜快速蒸发，同时有效地利用海水进行水电热电联产。模块化单元使海水在受限的纳米级通道中快速输送，并有效地蒸发薄膜。在1次太阳照射下，模块化水电联产机（MWEG）的电流密度为1.58 mA cm-2，功率密度为1.2 W m-2，蒸发速率高达2.69 kg m-2 h-1。此外，在室外光照浓度高达10太阳的情况下，MWEG的功率密度和蒸发速率可显著提高，分别达到4.3 W m-2和27.5 kg m-2 h-1。这些表现显示了利用地球海水蒸发来解决能源和水短缺问题的巨大潜力。
{"title":"Rapid Thin-Film Evaporation with Nanoscale Transport Empowers Efficient Water-Energy Harvesting from Seawater.","authors":"Meiwen Peng,Miao Wu,He Yang,Xinyu Zheng,Tianyi Wang,Rui Zhang,Bo Zhao,Lili Wang,Zhiqiang Liang,Tao Chen,Yinghui Sun,Zuankai Wang,Lin Jiang","doi":"10.1021/acsnano.5c22215","DOIUrl":"https://doi.org/10.1021/acsnano.5c22215","url":null,"abstract":"Harvesting freshwater and hydroenergy through evaporation from seawater simultaneously and efficiently is highly preferred for various applications but remains a challenge owing to mutually exclusive requirements: Efficient water-energy harvesting necessitates the presence of a thin water film on engineered evaporator surfaces to promote evaporation current, whereas efficient freshwater generation demands rapid bulk water transport. To decouple these originally conflicting requirements, we present a 3D modular architecture decorated with nanoscale channels that imparts rapid thin-film evaporation, enabling simultaneous and efficient cogeneration of water-electricity from seawater. The modular units endow the rapid transport of seawater in confined nanoscale channels and effective thin-film evaporation. Under 1 sun irradiation, the modular water-electricity cogenerator (MWEG) reaches a current density of 1.58 mA cm-2, power density of 1.2 W m-2, and high evaporation rate of 2.69 kg m-2 h-1. In addition, under an outdoor light concentration of up to 10 sun, the power density and evaporation rate of MWEG can be significantly increased to 4.3 W m-2 and 27.5 kg m-2 h-1, respectively. These performances demonstrate the vast potential of harnessing the evaporation of Earth's seawater to address shortages of both energy and water.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"92 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502439","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}
Jingbo Qin,Yi Cheng,Jayathilake Malinda,Yufeng Zhao,James M Tour,Jian Lin
Flash Joule heating (FJH) presents an attractive method to decompose per- and polyfluoroalkyl substances (PFAS) but suffers from an optimization challenge due to its complex reaction dynamics. In this study, we introduce a data-driven workflow that includes a Human-Guided Bayesian Optimization (HGBO) algorithm and an interpretable multibranch neural network (MBNN) to understand and optimize PFAS removal from soil. The HGBO algorithm incorporates expert intuition into the optimization cycle via a probabilistic acquisition strategy to enhance efficiency. In two iterations, HGBO improves the PFAS removal efficiency by 60%, outperforming vanilla BO and human-centered optimization. The results are well interpreted by SHapley additive expansion (SHAP) values and partial dependence analysis (PDA) to quantify feature significance and interactions. An interpretable MBNN is then developed to quantify the contributions of functional groups in various PFAS to the FJH degradation mechanism, which is further validated by density functional theory calculations. Seamless integration of HGBO and interpretable MBNN in one data-driven workflow not only accelerates experimental optimization but also provides interpretability, enabling more informed experimental decisions in complex chemical synthesis with limited data.
{"title":"Accelerate Flash Removal of PFAS from Soil by Human-Guided Bayesian Optimization and Interpretable Machine Learning.","authors":"Jingbo Qin,Yi Cheng,Jayathilake Malinda,Yufeng Zhao,James M Tour,Jian Lin","doi":"10.1021/acsnano.5c20063","DOIUrl":"https://doi.org/10.1021/acsnano.5c20063","url":null,"abstract":"Flash Joule heating (FJH) presents an attractive method to decompose per- and polyfluoroalkyl substances (PFAS) but suffers from an optimization challenge due to its complex reaction dynamics. In this study, we introduce a data-driven workflow that includes a Human-Guided Bayesian Optimization (HGBO) algorithm and an interpretable multibranch neural network (MBNN) to understand and optimize PFAS removal from soil. The HGBO algorithm incorporates expert intuition into the optimization cycle via a probabilistic acquisition strategy to enhance efficiency. In two iterations, HGBO improves the PFAS removal efficiency by 60%, outperforming vanilla BO and human-centered optimization. The results are well interpreted by SHapley additive expansion (SHAP) values and partial dependence analysis (PDA) to quantify feature significance and interactions. An interpretable MBNN is then developed to quantify the contributions of functional groups in various PFAS to the FJH degradation mechanism, which is further validated by density functional theory calculations. Seamless integration of HGBO and interpretable MBNN in one data-driven workflow not only accelerates experimental optimization but also provides interpretability, enabling more informed experimental decisions in complex chemical synthesis with limited data.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"2004 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502243","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}
Magneto-ionics-as the voltage-driven control of magnetic properties through ionic motion and redox processes-offers a promising route toward energy-efficient spintronic devices. Exchange bias, being the unidirectional anisotropy arising from interfacial coupling between antiferromagnets and ferromagnets, plays a central role in spintronics. Here, we demonstrate reversible, room-temperature magneto-ionic generation, suppression, and modulation of exchange bias within a 50 nm-thick antiferromagnetic, magneto-ionically active NiCoO layer. Instead of relying on field cooling to set exchange bias, an applied magnetic field during the growth promotes alignment of the antiferromagnetic spin sublattices, producing a preferential unidirectional orientation. Gating drives oxygen-ion migration along columnar grain boundaries, partially reducing NiCoO and forming ferromagnetic NiCo clusters that couple to the antiferromagnetic matrix. The exchange bias can be controlled by tuning the Ni/Co ratio, which adjusts the Néel temperature, and by varying the actuation time and voltage amplitude which control ferromagnetic cluster size. Micromagnetic simulations reveal that the exchange bias originates from the interfacial uncompensated spins exhibiting partial ferromagnetic-like behavior. This single-layer approach, together with the voltage-controlled formation and tuning of exchange bias without heat treatments, simplifies fabrication and offers a framework for low-power antiferromagnetic spintronic devices.
{"title":"Voltage-Driven Generation of Ferromagnetism in a Magneto-Ionically Active Antiferromagnet Enabling Room-Temperature Exchange Bias.","authors":"Simone Privitera,Zheng Ma,Hugo Gómez-Torres,Aitor Arredondo-López,Maciej Oskar Liedke,Eric Hirschmann,Andreas Wagner,Huan Tan,Pau Solsona,Alberto Quintana,Thiago Dias,Diane Gouéré,Elmer Monteblanco,Dafiné Ravelosona,Nuria Del-Valle,Carles Navau,Aitor Lopeandia,Jordi Sort,Enric Menéndez","doi":"10.1021/acsnano.5c19864","DOIUrl":"https://doi.org/10.1021/acsnano.5c19864","url":null,"abstract":"Magneto-ionics-as the voltage-driven control of magnetic properties through ionic motion and redox processes-offers a promising route toward energy-efficient spintronic devices. Exchange bias, being the unidirectional anisotropy arising from interfacial coupling between antiferromagnets and ferromagnets, plays a central role in spintronics. Here, we demonstrate reversible, room-temperature magneto-ionic generation, suppression, and modulation of exchange bias within a 50 nm-thick antiferromagnetic, magneto-ionically active NiCoO layer. Instead of relying on field cooling to set exchange bias, an applied magnetic field during the growth promotes alignment of the antiferromagnetic spin sublattices, producing a preferential unidirectional orientation. Gating drives oxygen-ion migration along columnar grain boundaries, partially reducing NiCoO and forming ferromagnetic NiCo clusters that couple to the antiferromagnetic matrix. The exchange bias can be controlled by tuning the Ni/Co ratio, which adjusts the Néel temperature, and by varying the actuation time and voltage amplitude which control ferromagnetic cluster size. Micromagnetic simulations reveal that the exchange bias originates from the interfacial uncompensated spins exhibiting partial ferromagnetic-like behavior. This single-layer approach, together with the voltage-controlled formation and tuning of exchange bias without heat treatments, simplifies fabrication and offers a framework for low-power antiferromagnetic spintronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"15 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147502244","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}
Yein Kim, Minsub Um, Subeom Shin, Hochan Song, Young Ran Park, Jonghee Yang
The ligand-assisted reprecipitation (LARP)-based synthetic approach has gained attention as a promising method for scalable synthesis of perovskite nanocrystals (PNCs) with outstanding optoelectronic functionalities. However, such distinct synthetic features of the LARP method involve an intrinsic limitation in realizing red-color emissions from I-rich compositions. Herein, we explore the LARP synthesis space of CsPb(BrxI1–x)3 PNCs via a high-throughput robotic synthesis platform integrating machine learning (ML) algorithms, not only allowing for understanding the role of each chemical variable from the multidimensional synthesis space but also refining the bespoke synthesis landscape of PNCs with target functionalities. It is found that ligand ratios as well as the selection of antisolvents dynamically contribute to synthesizing I-rich CsPbX3 PNCs, where their delicate and dedicated adjustments are required depending on the Br-to-I ratios. Furthermore, a disparity between the latent feature in ML-refined synthesis space and the manifested functionality space is identified, where the colloidal nature in the precursor state is found to colligate the bespoke synthesizability and functionality control of the LARP-PNCs. This data-driven approach enables the rational synthetic designs of CsPbX3 PNCs, as well as the fundamental relationship between the synthesis and functionality space.
{"title":"Understanding Synthesis Space in Ligand-Assisted Reprecipitated CsPb(BrxI1–x)3 Perovskite Nanocrystals","authors":"Yein Kim, Minsub Um, Subeom Shin, Hochan Song, Young Ran Park, Jonghee Yang","doi":"10.1021/acsnano.6c00180","DOIUrl":"https://doi.org/10.1021/acsnano.6c00180","url":null,"abstract":"The ligand-assisted reprecipitation (LARP)-based synthetic approach has gained attention as a promising method for scalable synthesis of perovskite nanocrystals (PNCs) with outstanding optoelectronic functionalities. However, such distinct synthetic features of the LARP method involve an intrinsic limitation in realizing red-color emissions from I-rich compositions. Herein, we explore the LARP synthesis space of CsPb(Br<sub><i>x</i></sub>I<sub>1–<i>x</i></sub>)<sub>3</sub> PNCs via a high-throughput robotic synthesis platform integrating machine learning (ML) algorithms, not only allowing for understanding the role of each chemical variable from the multidimensional synthesis space but also refining the bespoke synthesis landscape of PNCs with target functionalities. It is found that ligand ratios as well as the selection of antisolvents dynamically contribute to synthesizing I-rich CsPbX<sub>3</sub> PNCs, where their delicate and dedicated adjustments are required depending on the Br-to-I ratios. Furthermore, a disparity between the latent feature in ML-refined synthesis space and the manifested functionality space is identified, where the colloidal nature in the precursor state is found to colligate the bespoke synthesizability and functionality control of the LARP-PNCs. This data-driven approach enables the rational synthetic designs of CsPbX<sub>3</sub> PNCs, as well as the fundamental relationship between the synthesis and functionality space.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"18 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496249","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}
Lucas Liberal, Rafael Battistella Nadas, Gustavo H. R. Soares, Frederico B. Sousa, Maria Clara Godinho, Gabriel Marques Jacobsen, Takashi Taniguchi, Kenji Watanabe, Marcio Daldin Teodoro, Ado Jorio, Leonardo Cristiano Campos
Two-dimensional (2D) semiconductors such as monolayer WSe2 have attracted significant interest for their quantum properties and potential as scalable single-photon emitters. However, conventional microphotoluminescence (μ-PL) techniques are fundamentally limited by optical diffraction, hindering access to critical nanoscale features such as strain gradients and localized quantum confinement. In this study, we utilize tip-enhanced photoluminescence (NanoPL) with a spatial resolution of ≈10 nm to directly image the emission landscape of monolayer WSe2 on top of nanopillars at room temperature. Our results reveal two distinct localization regimes associated with leading theoretical models for single-photon activation and provide guidelines for deterministic nanoengineering of quantum light sources.
{"title":"Quantum Confinement Emissions in Strained Monolayer WSe2: A Nanoscale Approach to Single-Photon Emitters via Tip-Enhanced Techniques","authors":"Lucas Liberal, Rafael Battistella Nadas, Gustavo H. R. Soares, Frederico B. Sousa, Maria Clara Godinho, Gabriel Marques Jacobsen, Takashi Taniguchi, Kenji Watanabe, Marcio Daldin Teodoro, Ado Jorio, Leonardo Cristiano Campos","doi":"10.1021/acsnano.5c18642","DOIUrl":"https://doi.org/10.1021/acsnano.5c18642","url":null,"abstract":"Two-dimensional (2D) semiconductors such as monolayer WSe<sub>2</sub> have attracted significant interest for their quantum properties and potential as scalable single-photon emitters. However, conventional microphotoluminescence (μ-PL) techniques are fundamentally limited by optical diffraction, hindering access to critical nanoscale features such as strain gradients and localized quantum confinement. In this study, we utilize tip-enhanced photoluminescence (NanoPL) with a spatial resolution of ≈10 nm to directly image the emission landscape of monolayer WSe<sub>2</sub> on top of nanopillars at room temperature. Our results reveal two distinct localization regimes associated with leading theoretical models for single-photon activation and provide guidelines for deterministic nanoengineering of quantum light sources.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"12 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2026-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147492908","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}
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