Yuwei Qiu,Linfa Li,Lei Liang,Chaojie Yu,Fanglian Yao,Jin Zhou,Hong Zhang,Junjie Li
Achieving robust adhesion and seamless electrical integration between hydrogels and biological tissues remains a formidable challenge in tissue engineering and bioelectronics. Herein, we report a photothermal-mediated bioadhesion strategy for atraumatic yet tough tissue adhesion and an integrated electrical interface. By molecularly engineering functionalized polyaniline derivatives as bridging polymers, we achieved photothermally controlled tissue penetration, enabling the spontaneous formation of covalent-topological interactions between tissue and hydrogel. In contrast to conventional bioadhesives that depend primarily on surface interactions, our strategy employs tissue-penetrating conducting polymers to form a three-dimensional interlocking network. This integrated system forms highly efficient electrical pathways across the tissue-hydrogel interface, significantly reducing interfacial impedance and enabling effective interfacial electrical integration. Through in vitro and in vivo validation, we demonstrate the strategy's dual capability for high-precision electrophysiological monitoring and electrocoupling therapy in myocardial infarction. This bioadhesion strategy offers a simple and universal paradigm for bioelectronic and regenerative medicine.
{"title":"Photothermal-Mediated Topological-Covalent Tissue Adhesives: Synchronizing Robust Integration with Electrically Coupled Biointerfaces.","authors":"Yuwei Qiu,Linfa Li,Lei Liang,Chaojie Yu,Fanglian Yao,Jin Zhou,Hong Zhang,Junjie Li","doi":"10.1021/acsnano.5c14247","DOIUrl":"https://doi.org/10.1021/acsnano.5c14247","url":null,"abstract":"Achieving robust adhesion and seamless electrical integration between hydrogels and biological tissues remains a formidable challenge in tissue engineering and bioelectronics. Herein, we report a photothermal-mediated bioadhesion strategy for atraumatic yet tough tissue adhesion and an integrated electrical interface. By molecularly engineering functionalized polyaniline derivatives as bridging polymers, we achieved photothermally controlled tissue penetration, enabling the spontaneous formation of covalent-topological interactions between tissue and hydrogel. In contrast to conventional bioadhesives that depend primarily on surface interactions, our strategy employs tissue-penetrating conducting polymers to form a three-dimensional interlocking network. This integrated system forms highly efficient electrical pathways across the tissue-hydrogel interface, significantly reducing interfacial impedance and enabling effective interfacial electrical integration. Through in vitro and in vivo validation, we demonstrate the strategy's dual capability for high-precision electrophysiological monitoring and electrocoupling therapy in myocardial infarction. This bioadhesion strategy offers a simple and universal paradigm for bioelectronic and regenerative medicine.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"20 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145752769","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}
Ligand elimination from fully protected gold nanoclusters (AuNCs) to expose the metal core can induce high reactivity in catalytic reactions such as carbon dioxide reduction. However, there have been almost no reports of the preparation of partially ligand-eliminated species with controlled number and positions of removed ligands. Herein, we demonstrate regioselective single-ligand elimination of the thiolate-protected Au25 cluster anion [Au25(SR)18]− (SR = thiolate) to form [Au25(SR)17]0 through the protonation of an SR ligand with a Bro̷nsted acid. The number of eliminated SR ligands was experimentally confirmed through 1H nuclear magnetic resonance spectroscopy and electrospray ionization–mass spectrometry measurements. In contrast to the behavior of anionic [Au25(SR)18]−, the absence of SR elimination from the oxidized cluster ([Au25(SR)18]0) highlights the oxidation state-dependent reactivity of ligand elimination. The oxidation of [Au25(SR)18]− occurs in the Au13 core, so the contrasting reactivities of [Au25(SR)18]− and [Au25(SR)18]0 suggest the regioselective elimination of the Au13 core-bound SR ligand. The effects of the SR ligand on the reactivity of [Au25(SR)18]− reveal the importance of the electronic state of the Au13 core in regulating the SR-elimination reactivity. The similar trends were also confirmed in the reaction of other AuNCs bearing different Au core structures, and these electronic state-controlled reactivities of AuNCs have a resemblance with those of molecular transition metal complexes. The precisely controlled ligand elimination from AuNCs will facilitate the design of finely tuned Au-based catalysts with high reactivity and durability.
{"title":"Protonation-Induced Single-Ligand Elimination of Thiolate-Protected Gold Nanoclusters","authors":"Wataru Suzuki, Ryo Takahata, Tomu Morigaki, Yuki Chiga, Tomokazu Umeyama, Toshiharu Teranishi","doi":"10.1021/acsnano.5c12415","DOIUrl":"https://doi.org/10.1021/acsnano.5c12415","url":null,"abstract":"Ligand elimination from fully protected gold nanoclusters (AuNCs) to expose the metal core can induce high reactivity in catalytic reactions such as carbon dioxide reduction. However, there have been almost no reports of the preparation of partially ligand-eliminated species with controlled number and positions of removed ligands. Herein, we demonstrate regioselective single-ligand elimination of the thiolate-protected Au<sub>25</sub> cluster anion [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>−</sup> (SR = thiolate) to form [Au<sub>25</sub>(SR)<sub>17</sub>]<sup>0</sup> through the protonation of an SR ligand with a Bro̷nsted acid. The number of eliminated SR ligands was experimentally confirmed through <sup>1</sup>H nuclear magnetic resonance spectroscopy and electrospray ionization–mass spectrometry measurements. In contrast to the behavior of anionic [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>−</sup>, the absence of SR elimination from the oxidized cluster ([Au<sub>25</sub>(SR)<sub>18</sub>]<sup>0</sup>) highlights the oxidation state-dependent reactivity of ligand elimination. The oxidation of [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>−</sup> occurs in the Au<sub>13</sub> core, so the contrasting reactivities of [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>−</sup> and [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>0</sup> suggest the regioselective elimination of the Au<sub>13</sub> core-bound SR ligand. The effects of the SR ligand on the reactivity of [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>−</sup> reveal the importance of the electronic state of the Au<sub>13</sub> core in regulating the SR-elimination reactivity. The similar trends were also confirmed in the reaction of other AuNCs bearing different Au core structures, and these electronic state-controlled reactivities of AuNCs have a resemblance with those of molecular transition metal complexes. The precisely controlled ligand elimination from AuNCs will facilitate the design of finely tuned Au-based catalysts with high reactivity and durability.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"9 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732526","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}
Qingli Cao,Lingbin Ye,Yun Gao,Haiping He,Zhizhen Ye,Xingliang Dai
Enlarged synthesis of monodisperse colloidal nanocrystals is essential for practical applications. However, the scalable synthesis of perovskite nanocrystals remains challenging due to the fast crystallization nature of perovskites, which allows for only an extremely short time window for mass and heat transfer. Specifically, the difficulties in the enlarged synthesis of ultrasmall and monodisperse CsPbBr3 nanocrystals are amplified, usually accompanied by the formation of nanoplate byproducts. Here, we demonstrate a multibranched ligand-assisted synthetic strategy to control the isotropic growth of ultrasmall CsPbBr3 nanocrystals in an enlarged synthesis. The multibranched ligand with large steric hindrance breaks the close alignment of alkylammonium cations at a specific facet during the nucleation stage, which synergistically suppresses anisotropic growth and extends the crystallization time window to several min. This allows for synthesis volumes up to 200 mL without compromising monodispersity and optical quality, which also avoids the generation of nanoplate byproducts. The enlarged-synthesized CsPbBr3 nanocrystals exhibit blue emission at 480 nm with a narrow full-width at half-maximum of 21 nm. Corresponding blue light-emitting diodes achieve an external quantum efficiency of 22.4% with great spectral stability and reproducibility. This work provides a solution for scalable preparation of ultrasmall nanocrystals and presents a generalizable ligand design approach for morphology control, facilitating the practical development of highly efficient perovskite optoelectronic devices.
{"title":"Isotropic-Grown Ultrasmall CsPbBr3 Nanocrystals in an Enlarged Synthesis toward Efficient Blue Electroluminescence.","authors":"Qingli Cao,Lingbin Ye,Yun Gao,Haiping He,Zhizhen Ye,Xingliang Dai","doi":"10.1021/acsnano.5c15099","DOIUrl":"https://doi.org/10.1021/acsnano.5c15099","url":null,"abstract":"Enlarged synthesis of monodisperse colloidal nanocrystals is essential for practical applications. However, the scalable synthesis of perovskite nanocrystals remains challenging due to the fast crystallization nature of perovskites, which allows for only an extremely short time window for mass and heat transfer. Specifically, the difficulties in the enlarged synthesis of ultrasmall and monodisperse CsPbBr3 nanocrystals are amplified, usually accompanied by the formation of nanoplate byproducts. Here, we demonstrate a multibranched ligand-assisted synthetic strategy to control the isotropic growth of ultrasmall CsPbBr3 nanocrystals in an enlarged synthesis. The multibranched ligand with large steric hindrance breaks the close alignment of alkylammonium cations at a specific facet during the nucleation stage, which synergistically suppresses anisotropic growth and extends the crystallization time window to several min. This allows for synthesis volumes up to 200 mL without compromising monodispersity and optical quality, which also avoids the generation of nanoplate byproducts. The enlarged-synthesized CsPbBr3 nanocrystals exhibit blue emission at 480 nm with a narrow full-width at half-maximum of 21 nm. Corresponding blue light-emitting diodes achieve an external quantum efficiency of 22.4% with great spectral stability and reproducibility. This work provides a solution for scalable preparation of ultrasmall nanocrystals and presents a generalizable ligand design approach for morphology control, facilitating the practical development of highly efficient perovskite optoelectronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145746655","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}
Ou Wang,Heyu Wang,Yu Tang,Zhiheng Ma,Bao-Li An,Yongmei Zhao,Xiaohong Wang,Jiaqiang Xu
Accurate detection of acetone (C3H6O) is essential for both environmental monitoring and noninvasive diabetes diagnosis. High-entropy alloys (HEAs) have been demonstrated as effective catalysts to replace noble metals for enhancing the gas-sensing performance of semiconductor metal oxides. However, HEAs tend to agglomerate at high temperatures, which severely limits their long-term stability and performance. To address this issue, a PtFeCoNiCuSn HEA was developed as a functional sensitizer for SnO2-based C3H6O sensors. The existence of Sn in the HEA structure enhances the interaction of HEA with SnO2 and prevents agglomeration under high-temperature conditions (≥300 °C), leading to improved stability and catalytic activity for C3H6O detection. The PtFeCoNiCuSn-SnO2-300 sensor exhibited increased sensitivity than its Sn-free HEA counterpart, along with shorter response and recovery times (6.5 s/10.5 s) at a working temperature of 230 °C, a clear response (Ra/Rg = 4.59@2 ppm), and a low detection limit down to 4 ppb for C3H6O. Moreover, it demonstrated stable long-term stability, with no significant response degradation (σ = 0.056) observed over a 63-day continuous test. The enhanced performance is attributed to the synergistic effects of the HEA's multielement composition and strong metal-support interaction, which strengthens electronic interaction and the activation of surface oxygen species. This study provides a framework for enhancing the interaction between HEAs and semiconductor metal oxides to further improve the gas-sensing properties of the latter.
{"title":"Anchoring Sn-Containing High-Entropy Alloy PtFeCoNiCuSn on SnO2 for Improving Acetone Detection Ability.","authors":"Ou Wang,Heyu Wang,Yu Tang,Zhiheng Ma,Bao-Li An,Yongmei Zhao,Xiaohong Wang,Jiaqiang Xu","doi":"10.1021/acsnano.5c15097","DOIUrl":"https://doi.org/10.1021/acsnano.5c15097","url":null,"abstract":"Accurate detection of acetone (C3H6O) is essential for both environmental monitoring and noninvasive diabetes diagnosis. High-entropy alloys (HEAs) have been demonstrated as effective catalysts to replace noble metals for enhancing the gas-sensing performance of semiconductor metal oxides. However, HEAs tend to agglomerate at high temperatures, which severely limits their long-term stability and performance. To address this issue, a PtFeCoNiCuSn HEA was developed as a functional sensitizer for SnO2-based C3H6O sensors. The existence of Sn in the HEA structure enhances the interaction of HEA with SnO2 and prevents agglomeration under high-temperature conditions (≥300 °C), leading to improved stability and catalytic activity for C3H6O detection. The PtFeCoNiCuSn-SnO2-300 sensor exhibited increased sensitivity than its Sn-free HEA counterpart, along with shorter response and recovery times (6.5 s/10.5 s) at a working temperature of 230 °C, a clear response (Ra/Rg = 4.59@2 ppm), and a low detection limit down to 4 ppb for C3H6O. Moreover, it demonstrated stable long-term stability, with no significant response degradation (σ = 0.056) observed over a 63-day continuous test. The enhanced performance is attributed to the synergistic effects of the HEA's multielement composition and strong metal-support interaction, which strengthens electronic interaction and the activation of surface oxygen species. This study provides a framework for enhancing the interaction between HEAs and semiconductor metal oxides to further improve the gas-sensing properties of the latter.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"150 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728650","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}
Luyao Yi, Jielong Gao, Zhengrong Yin, Cui Huang, Taolei Sun, Guanbin Gao, Zhengyi Fu, Zhaoyong Zou
Bacterial invasion compromises the inherent reparative capability of dentin, leading to caries progression. Designing an effective strategy to simultaneously restore the dentin structure and combat oral biofilms remains a great challenge. This study presents a single-step biomimetic approach that employs carboxyl-functionalized gold nanoparticles (AuNPs-COOH) as a noncollagenous protein analogue to generate nanoparticle-induced liquid precursor (NILP) for synergistic dentin regeneration and antibacterial therapy. The AuNPs-COOH stabilize amorphous calcium phosphate precursors and induce intrafibrillar mineralization, thereby restoring the hierarchical architecture and mechanical properties of dentin (elastic modulus: 24.42 GPa; hardness: 1.06 GPa), closely matching those of sound dentin (24.84 and 1.15 GPa, respectively) and surpassing conventional polymer-induced remineralization. The remineralized dentin exhibits dual antibacterial functionalities activated by near-infrared (NIR) light: photothermal effect and photodynamic generation of reactive oxygen species. This NIR-activated system significantly inhibits Streptococcus mutans biofilm formation in vitro, reducing biofilm biomass to 10–20% of control levels under both immediate and long-term conditions, and demonstrates robust antibacterial efficacy in vivo. Furthermore, the remineralized dentin exhibits excellent biocompatibility with dental pulp stem cells and minimal systemic toxicity in animal models. The AuNPs-COOH-mediated NILP system thus offers a synergistic strategy for functional dentin regeneration and caries prevention.
{"title":"Synergistic Antibacterial Remineralization: A Bioprocessing-Inspired Single-Step Nanoparticle-Induced Liquid Precursor Strategy for Functional Dentin Repair","authors":"Luyao Yi, Jielong Gao, Zhengrong Yin, Cui Huang, Taolei Sun, Guanbin Gao, Zhengyi Fu, Zhaoyong Zou","doi":"10.1021/acsnano.5c14982","DOIUrl":"https://doi.org/10.1021/acsnano.5c14982","url":null,"abstract":"Bacterial invasion compromises the inherent reparative capability of dentin, leading to caries progression. Designing an effective strategy to simultaneously restore the dentin structure and combat oral biofilms remains a great challenge. This study presents a single-step biomimetic approach that employs carboxyl-functionalized gold nanoparticles (AuNPs-COOH) as a noncollagenous protein analogue to generate nanoparticle-induced liquid precursor (NILP) for synergistic dentin regeneration and antibacterial therapy. The AuNPs-COOH stabilize amorphous calcium phosphate precursors and induce intrafibrillar mineralization, thereby restoring the hierarchical architecture and mechanical properties of dentin (elastic modulus: 24.42 GPa; hardness: 1.06 GPa), closely matching those of sound dentin (24.84 and 1.15 GPa, respectively) and surpassing conventional polymer-induced remineralization. The remineralized dentin exhibits dual antibacterial functionalities activated by near-infrared (NIR) light: photothermal effect and photodynamic generation of reactive oxygen species. This NIR-activated system significantly inhibits <i>Streptococcus mutans</i> biofilm formation <i>in vitro</i>, reducing biofilm biomass to 10–20% of control levels under both immediate and long-term conditions, and demonstrates robust antibacterial efficacy <i>in vivo</i>. Furthermore, the remineralized dentin exhibits excellent biocompatibility with dental pulp stem cells and minimal systemic toxicity in animal models. The AuNPs-COOH-mediated NILP system thus offers a synergistic strategy for functional dentin regeneration and caries prevention.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"7 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728703","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}
Siyu Meng, Huiping Du, Xiang Li, Xinmin Zheng, Pan Zhao, Zhang Yuan, Shaohui Huang, Yanli Zhao, Liangliang Dai
In the originally published article, Figure 5E contained an error inadvertently. Specially, the invasion images of control and MA-PEI groups were mistakenly used. To ensure the accuracy of the data, we provide the corrected Figure 5E and its corresponding quantitative analysis (Figure 5H) below. Figure 5. (E) Microscopy images and quantitative analysis (H) of the wound healing, migration and invasion assays of B16F10 cells after coculturing with MDSCs plus different treatments for 24 h. P values were determined by unpaired Student’s t test (two-tailed), ***p < 0.001. Data are represented as mean ± SD (n = 4 biologically independent samples). Scale bars: 100 μm for E. Also, in Figure S26E and Figure S30, the invasion image of MA-PEI group and the HMGB 1 image of Saline group were mistakenly used, respectively. The corrected Figure S26E and its corresponding quantitative analysis (Figure S26H), and the corrected Figure S30 are shown in the corrected Supporting Information. The complete corrected Supporting Information is provided here. These corrections do not affect the conclusions of our publication, and no changes to the article text are required. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.5c19444. Additional experimental procedures; NMR spectra; GPC curves; FTIR spectra; gel retardation assay; UV–vis spectra; size distributions; DLS analysis; fluorescence correlation spectroscopy; agarose gel electrophoreses; cytotoxicity assay; tumor penetration images; CLSM images; quantification analysis of FAM fluorescence; Western blot analysis; survival of 4T1 cells; gating and classifying strategies; flow cytometry profiles; phenotype and quantitative analysis; typical cytokine concentrations; concentrations of IL-6, IL-12, and TNF-α; microscopy images and quantitative analysis; FCM detection; representative FCM plots; IFC images; in vivo uptake effect; weight change curves; representative histological images; biodistribution; and pharmacokinetics (PDF) Correction to “An Adjuvant Micelle-Based Multifunctional Nanosystem for Tumor Immunotherapy by Remodeling Three Types of Immunosuppressive Cells” 2 views 0 shares 0 downloads Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. This article has not yet been cited by other publications.
{"title":"Correction to “An Adjuvant Micelle-Based Multifunctional Nanosystem for Tumor Immunotherapy by Remodeling Three Types of Immunosuppressive Cells”","authors":"Siyu Meng, Huiping Du, Xiang Li, Xinmin Zheng, Pan Zhao, Zhang Yuan, Shaohui Huang, Yanli Zhao, Liangliang Dai","doi":"10.1021/acsnano.5c19444","DOIUrl":"https://doi.org/10.1021/acsnano.5c19444","url":null,"abstract":"In the originally published article, Figure 5E contained an error inadvertently. Specially, the invasion images of control and MA-PEI groups were mistakenly used. To ensure the accuracy of the data, we provide the corrected Figure 5E and its corresponding quantitative analysis (Figure 5H) below. Figure 5. (E) Microscopy images and quantitative analysis (H) of the wound healing, migration and invasion assays of B16F10 cells after coculturing with MDSCs plus different treatments for 24 h. P values were determined by unpaired Student’s <i>t</i> test (two-tailed), ***<i>p</i> < 0.001. Data are represented as mean ± SD (<i>n</i> = 4 biologically independent samples). Scale bars: 100 μm for E. Also, in Figure S26E and Figure S30, the invasion image of MA-PEI group and the HMGB 1 image of Saline group were mistakenly used, respectively. The corrected Figure S26E and its corresponding quantitative analysis (Figure S26H), and the corrected Figure S30 are shown in the corrected Supporting Information. The complete corrected Supporting Information is provided here. These corrections do not affect the conclusions of our publication, and no changes to the article text are required. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsnano.5c19444. Additional experimental procedures; NMR spectra; GPC curves; FTIR spectra; gel retardation assay; UV–vis spectra; size distributions; DLS analysis; fluorescence correlation spectroscopy; agarose gel electrophoreses; cytotoxicity assay; tumor penetration images; CLSM images; quantification analysis of FAM fluorescence; Western blot analysis; survival of 4T1 cells; gating and classifying strategies; flow cytometry profiles; phenotype and quantitative analysis; typical cytokine concentrations; concentrations of IL-6, IL-12, and TNF-α; microscopy images and quantitative analysis; FCM detection; representative FCM plots; IFC images; in vivo uptake effect; weight change curves; representative histological images; biodistribution; and pharmacokinetics (PDF) Correction\u0000to “An Adjuvant Micelle-Based Multifunctional\u0000Nanosystem for Tumor Immunotherapy by Remodeling Three Types of Immunosuppressive\u0000Cells” <span> 2 </span><span> views </span> <span> 0 </span><span> shares </span> <span> 0 </span><span> downloads </span> Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. This article has not yet been cited by other publications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"158 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729221","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}
Yeonji Kim, Seung Won Lee, Jihye Jang, Woojoong Kim, Guangtao Zan, Seokyeong Lee, Taebin Kim, Gwanho Kim, Jaemin Yoo, Jung Hun Lee, Kaiying Zhao, Tae Hyun Park, Kyuho Lee, Hayeon Jeong, Jin Woo Oh, Jong Woong Park, Shengyou Li, Mark C. Hersam, Cheolmin Park
Despite the significant progress in the development of ionic junctions of two types of ionic conductors for ionic current rectification, reminiscent to electronic p- and n-type junctions, stimuli-responsive ionic junctions wherein stimuli reversibly control current rectification are seldom demonstrated. Here, we present a near-infrared (NIR)-responsive ionic junction and its application as a switchable logic gate. The NIR- responsive ionic junction is developed with a bilayer of ionoelastomers: liquid-free ionic conductors with mobile cations (p-type) and anion counterions (n-type) mixed with NIR-responsive 2D MXene (Ti3C2Tx) nanosheets sandwiched between two liquid metal electrodes. The study revealed that two types of MXene with positive and negative surface potentials incorporated into p- and n-type ionoelastomers, respectively, facilitated the diffusion of mobile ions. This resulted in an enhanced current rectification of an ionic diode. The rectification of an ionic junction is further increased upon NIR exposure to the device due to the photothermal energy conversion of MXene. A facile control of the rectification ratio with both exposure time and power of NIR enabled the development of a switchable ionic logic gate. Herein, the AND-to-OR gate transition was reversibly manipulated by NIR exposure and device cooling programmed to the two ionic junctions in series.
{"title":"Near-Infrared Responsive Ionoelastomer Junction Enabling Switchable Ionic Logic Gate","authors":"Yeonji Kim, Seung Won Lee, Jihye Jang, Woojoong Kim, Guangtao Zan, Seokyeong Lee, Taebin Kim, Gwanho Kim, Jaemin Yoo, Jung Hun Lee, Kaiying Zhao, Tae Hyun Park, Kyuho Lee, Hayeon Jeong, Jin Woo Oh, Jong Woong Park, Shengyou Li, Mark C. Hersam, Cheolmin Park","doi":"10.1021/acsnano.5c13433","DOIUrl":"https://doi.org/10.1021/acsnano.5c13433","url":null,"abstract":"Despite the significant progress in the development of ionic junctions of two types of ionic conductors for ionic current rectification, reminiscent to electronic p- and n-type junctions, stimuli-responsive ionic junctions wherein stimuli reversibly control current rectification are seldom demonstrated. Here, we present a near-infrared (NIR)-responsive ionic junction and its application as a switchable logic gate. The NIR- responsive ionic junction is developed with a bilayer of ionoelastomers: liquid-free ionic conductors with mobile cations (p-type) and anion counterions (n-type) mixed with NIR-responsive 2D MXene (Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>) nanosheets sandwiched between two liquid metal electrodes. The study revealed that two types of MXene with positive and negative surface potentials incorporated into p- and n-type ionoelastomers, respectively, facilitated the diffusion of mobile ions. This resulted in an enhanced current rectification of an ionic diode. The rectification of an ionic junction is further increased upon NIR exposure to the device due to the photothermal energy conversion of MXene. A facile control of the rectification ratio with both exposure time and power of NIR enabled the development of a switchable ionic logic gate. Herein, the AND-to-OR gate transition was reversibly manipulated by NIR exposure and device cooling programmed to the two ionic junctions in series.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"29 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729202","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 formation of complex nanoscale architectures through molecular self-assembly remains a fundamental challenge in materials science and biology. Brochosomes─nanostructured granules produced by the Malpighian tubules of leafhoppers─exhibit diverse morphologies driven by molecular-level variations in their protein constituents. Inspired by this natural system, a droplet microfluidic platform is developed that adapts principles observed in leafhopper Malpighian tubules, using amphiphilic block copolymers to generate brochosome-like particles. By tuning the ratio of hydrophobic and hydrophilic domains and the molecular weight of the block copolymers, the interfacial tension of oil-in-water droplets is modulated to control particle diameter, pore geometry, and wall thickness, producing five distinct brochosome architectures that fall within the range observed in leafhoppers. The resulting particles range from 390 nm to 2 μm in diameter, with pore sizes between 30 and 130 nm. Self-assembly of the block copolymers and interfacial tension-driven morphogenesis enable high-throughput synthesis exceeding 105 particles per second. The synthetic brochosomes exhibit broadband and omnidirectional antireflection across the ultraviolet and visible spectrum, comparable to natural brochosomes. This platform provides a scalable route to the fabrication of bioinspired micro- and nanostructures and elucidates how molecular design governs morphological evolution, with potential applications in optical coatings, pigments, camouflage materials, and biomedicine.
{"title":"Morphogenesis and High-Throughput Nanomanufacturing of Synthetic Brochosomes Inspired by a Leafhopper","authors":"Jinsol Choi, Tak-Sing Wong","doi":"10.1021/acsnano.5c12763","DOIUrl":"https://doi.org/10.1021/acsnano.5c12763","url":null,"abstract":"The formation of complex nanoscale architectures through molecular self-assembly remains a fundamental challenge in materials science and biology. Brochosomes─nanostructured granules produced by the Malpighian tubules of leafhoppers─exhibit diverse morphologies driven by molecular-level variations in their protein constituents. Inspired by this natural system, a droplet microfluidic platform is developed that adapts principles observed in leafhopper Malpighian tubules, using amphiphilic block copolymers to generate brochosome-like particles. By tuning the ratio of hydrophobic and hydrophilic domains and the molecular weight of the block copolymers, the interfacial tension of oil-in-water droplets is modulated to control particle diameter, pore geometry, and wall thickness, producing five distinct brochosome architectures that fall within the range observed in leafhoppers. The resulting particles range from 390 nm to 2 μm in diameter, with pore sizes between 30 and 130 nm. Self-assembly of the block copolymers and interfacial tension-driven morphogenesis enable high-throughput synthesis exceeding 10<sup>5</sup> particles per second. The synthetic brochosomes exhibit broadband and omnidirectional antireflection across the ultraviolet and visible spectrum, comparable to natural brochosomes. This platform provides a scalable route to the fabrication of bioinspired micro- and nanostructures and elucidates how molecular design governs morphological evolution, with potential applications in optical coatings, pigments, camouflage materials, and biomedicine.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"158 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729204","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}
Thai D Luong,Nick Martel,James Rae,Harriet P Lo,Ye-Wheen Lim,Yeping Wu,Kerrie-Ann McMahon,Haolan Sun,Nicholas L Fletcher,Kristofer J Thurecht,Angus P R Johnston,Nicholas Ariotti,Thomas E Hall,Robert G Parton
Targeted nanoparticles have the potential to revolutionize therapeutics for medical applications. Here, we demonstrate the utility of a flexible precision nanovesicle delivery system for functional delivery of DNA, RNA, proteins, and drugs into target cells. Nanovesicles generated by the membrane sculpting protein caveolin, termed caveospheres, can be loaded with RNA, DNA, proteins, or drugs postsynthesis or incorporate genetically encoded cargo proteins during production without the need for protein purification. Functionalized, fluorescently labeled caveospheres form a modular system that shows high stability in biological fluids and specific uptake by target-positive cells and can deliver proteins, drugs, DNA, and mRNA directly to the cytoplasm and nuclei of only the target cells. The negligible level of off-target transduction and uniform levels of targeted expression demonstrate advantages of the system over lipid-mediated gene delivery. Caveospheres can also be engineered to mimic viral particles by displaying the SARS-CoV-2-RBD protein, enabling the targeted delivery to human bronchial epithelial cells. We demonstrate their application as a targeted transfection system for cells in culture and critically, their efficacy in precision tumor killing in vivo.
{"title":"A Modular Encapsulation System for Precision Delivery of Proteins, Nucleic Acids, and Small Molecules.","authors":"Thai D Luong,Nick Martel,James Rae,Harriet P Lo,Ye-Wheen Lim,Yeping Wu,Kerrie-Ann McMahon,Haolan Sun,Nicholas L Fletcher,Kristofer J Thurecht,Angus P R Johnston,Nicholas Ariotti,Thomas E Hall,Robert G Parton","doi":"10.1021/acsnano.5c11452","DOIUrl":"https://doi.org/10.1021/acsnano.5c11452","url":null,"abstract":"Targeted nanoparticles have the potential to revolutionize therapeutics for medical applications. Here, we demonstrate the utility of a flexible precision nanovesicle delivery system for functional delivery of DNA, RNA, proteins, and drugs into target cells. Nanovesicles generated by the membrane sculpting protein caveolin, termed caveospheres, can be loaded with RNA, DNA, proteins, or drugs postsynthesis or incorporate genetically encoded cargo proteins during production without the need for protein purification. Functionalized, fluorescently labeled caveospheres form a modular system that shows high stability in biological fluids and specific uptake by target-positive cells and can deliver proteins, drugs, DNA, and mRNA directly to the cytoplasm and nuclei of only the target cells. The negligible level of off-target transduction and uniform levels of targeted expression demonstrate advantages of the system over lipid-mediated gene delivery. Caveospheres can also be engineered to mimic viral particles by displaying the SARS-CoV-2-RBD protein, enabling the targeted delivery to human bronchial epithelial cells. We demonstrate their application as a targeted transfection system for cells in culture and critically, their efficacy in precision tumor killing in vivo.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"148 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728652","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}
We investigate the excitonic properties of epitaxially grown WS2 monolayers, bilayers and multilayers on graphene using monochromatic electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope. This material system is particularly attractive for optoelectronic applications, as direct growth from the gas phase offers a scalable route to wafer-sized heterostructures. The combination of nanometer-scale spatial resolution and high spectral quality in EELS allows for a detailed analysis of layer-dependent excitonic features. To complement the experimental results, we perform ab initio simulations based on density functional theory and the Bethe-Salpeter equation. The experimental spectra reveal a systematic redshift of both A and B excitons at the K-valley─centered near 2.0 and 2.4 eV, respectively─as the number of WS2 layers increases. While such redshifts are often attributed to dielectric screening, our ab initio calculations show that the dominant contribution arises from a subtle lattice mismatch between the lower and upper WS2 layers. We trace this mismatch to the heteroepitaxial alignment of the first WS2 layer to the graphene substrate during the growth process. Our results highlight how nanoscale structural distortions in epitaxial 2D materials can strongly influence key excitonic properties, even in the absence of intentional strain or alloying. By combining nanometer-scale electron spectroscopy with advanced theory, we establish a direct link between atomic structure and excitonic response in realistic, nonidealized heterostructures. These findings underscore the importance of microscopic interface effects in the design and scalable fabrication of exciton-based optoelectronic devices.
{"title":"Excitons in Epitaxially Grown WS2 on Graphene: A Nanometer-Resolved Electron Energy Loss Spectroscopy and Density Functional Theory Study.","authors":"Max Bergmann,Jürgen Belz,Oliver Maßmeyer,Badrosadat Ojaghi Dogahe,Robin Günkel,Johannes Glowatzki,Andreas Beyer,Ivan Solovev,Jens-Christian Drawer,Martin Esmann,Sergej Pasko,Simonas Krotkus,Michael Heuken,Stefan Wippermann,Kerstin Volz","doi":"10.1021/acsnano.5c11994","DOIUrl":"https://doi.org/10.1021/acsnano.5c11994","url":null,"abstract":"We investigate the excitonic properties of epitaxially grown WS2 monolayers, bilayers and multilayers on graphene using monochromatic electron energy loss spectroscopy (EELS) in a scanning transmission electron microscope. This material system is particularly attractive for optoelectronic applications, as direct growth from the gas phase offers a scalable route to wafer-sized heterostructures. The combination of nanometer-scale spatial resolution and high spectral quality in EELS allows for a detailed analysis of layer-dependent excitonic features. To complement the experimental results, we perform ab initio simulations based on density functional theory and the Bethe-Salpeter equation. The experimental spectra reveal a systematic redshift of both A and B excitons at the K-valley─centered near 2.0 and 2.4 eV, respectively─as the number of WS2 layers increases. While such redshifts are often attributed to dielectric screening, our ab initio calculations show that the dominant contribution arises from a subtle lattice mismatch between the lower and upper WS2 layers. We trace this mismatch to the heteroepitaxial alignment of the first WS2 layer to the graphene substrate during the growth process. Our results highlight how nanoscale structural distortions in epitaxial 2D materials can strongly influence key excitonic properties, even in the absence of intentional strain or alloying. By combining nanometer-scale electron spectroscopy with advanced theory, we establish a direct link between atomic structure and excitonic response in realistic, nonidealized heterostructures. These findings underscore the importance of microscopic interface effects in the design and scalable fabrication of exciton-based optoelectronic devices.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"10 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728654","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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