Hong Huy Tran, Zhenting Xiang, Min Jun Oh, Yuan Liu, Zhi Ren, Chider Chen, Nadasinee Jaruchotiratanasakul, James M. Kikkawa, Daeyeon Lee, Hyun Koo, Edward Steager
Microrobots are poised to transform biomedicine by enabling precise, noninvasive procedures. However, current magnetic microrobots, composed of solid monolithic particles, present fundamental challenges in engineering intersubunit interactions, limiting their collective effectiveness in navigating irregular biological terrains and confined spaces. To address this, we design hierarchically assembled microrobots with multiaxis mobility and collective adaptability by engineering the potential magnetic interaction energy between subunits to create stable, self-reconfigurable structures capable of carrying and protecting cargo internally. Using double emulsion templates and magnetic control techniques, we confine 10 nm iron oxide and 15 nm silica nanoparticles within the shell of 100 μm microcapsules that form multiunit robotic collectives. Unexpectedly, we find that asymmetric localization of iron oxide nanoparticles in the microcapsules enhances the intercapsule potential energy, creating stable connections under rotating magnetic fields without altering the magnetic susceptibility. These robotic microcapsule collectives exhibit emergent behaviors, self-reconfiguring into kinematic chain-like structures to traverse complex obstacles, arched confinements, and adhesive, rugged biological tissues that typically impede microscale systems. By harnessing these functions, we demonstrate targeted antifungal delivery using a localized biofilm model on mucosal tissues, showing effective killing ofCandida without binding or causing physical damage to host cells. Our findings show how hierarchical assembly can produce cargo-carrying microrobots with collective, self-adaptive mobility for traversing complex biological environments, advancing targeted delivery for biomedical applications.
{"title":"Robotic Microcapsule Assemblies with Adaptive Mobility for Targeted Treatment of Rugged Biological Microenvironments","authors":"Hong Huy Tran, Zhenting Xiang, Min Jun Oh, Yuan Liu, Zhi Ren, Chider Chen, Nadasinee Jaruchotiratanasakul, James M. Kikkawa, Daeyeon Lee, Hyun Koo, Edward Steager","doi":"10.1021/acsnano.4c11686","DOIUrl":"https://doi.org/10.1021/acsnano.4c11686","url":null,"abstract":"Microrobots are poised to transform biomedicine by enabling precise, noninvasive procedures. However, current magnetic microrobots, composed of solid monolithic particles, present fundamental challenges in engineering intersubunit interactions, limiting their collective effectiveness in navigating irregular biological terrains and confined spaces. To address this, we design hierarchically assembled microrobots with multiaxis mobility and collective adaptability by engineering the potential magnetic interaction energy between subunits to create stable, self-reconfigurable structures capable of carrying and protecting cargo internally. Using double emulsion templates and magnetic control techniques, we confine 10 nm iron oxide and 15 nm silica nanoparticles within the shell of 100 μm microcapsules that form multiunit robotic collectives. Unexpectedly, we find that asymmetric localization of iron oxide nanoparticles in the microcapsules enhances the intercapsule potential energy, creating stable connections under rotating magnetic fields without altering the magnetic susceptibility. These robotic microcapsule collectives exhibit emergent behaviors, self-reconfiguring into kinematic chain-like structures to traverse complex obstacles, arched confinements, and adhesive, rugged biological tissues that typically impede microscale systems. By harnessing these functions, we demonstrate targeted antifungal delivery using a localized biofilm model on mucosal tissues, showing effective killing of<i>Candida</i> without binding or causing physical damage to host cells. Our findings show how hierarchical assembly can produce cargo-carrying microrobots with collective, self-adaptive mobility for traversing complex biological environments, advancing targeted delivery for biomedical applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"15 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968327","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}
Kai Huang, Kartik Samanta, Ding-Fu Shao, Evgeny Y. Tsymbal
A spin valve represents a well-established device concept in magnetic memory technologies, whose functionality is determined by electron transmission, controlled by the relative alignment of magnetic moments of the two ferromagnetic layers. Recently, the advent of valleytronics has conceptualized a valley spin valve (VSV)─a device that utilizes the valley degree of freedom and spin-valley locking to achieve a similar valve effect without relying on magnetism. In this study, we propose a nonvolatile VSV (n-VSV) based on a two-dimensional (2D) ferroelectric semiconductor where resistance of n-VSV is controlled by a ferroelectric domain wall between two uniformly polarized domains. Focusing on the 1T″ phase of MoS2, which is known to be ferroelectric down to a monolayer and using density functional theory combined with quantum transport calculations, we demonstrate that switching between the uniformly polarized state and the state with oppositely polarized domains separated by a domain wall results in a resistance change of as high as 107. This giant VSV effect occurs due to transmission being strongly dependent on matching (mismatching) the valley-dependent spin polarization in the two domains with the same (opposite) ferroelectric polarization orientations, when the chemical potential of 1T″-MoS2 lies within the spin-split valleys. The proposed n-VSV can be employed as a functional device for high-performance nonvolatile valleytronics.
{"title":"Two-Dimensional Nonvolatile Valley Spin Valve","authors":"Kai Huang, Kartik Samanta, Ding-Fu Shao, Evgeny Y. Tsymbal","doi":"10.1021/acsnano.4c12812","DOIUrl":"https://doi.org/10.1021/acsnano.4c12812","url":null,"abstract":"A spin valve represents a well-established device concept in magnetic memory technologies, whose functionality is determined by electron transmission, controlled by the relative alignment of magnetic moments of the two ferromagnetic layers. Recently, the advent of valleytronics has conceptualized a valley spin valve (VSV)─a device that utilizes the valley degree of freedom and spin-valley locking to achieve a similar valve effect without relying on magnetism. In this study, we propose a nonvolatile VSV (<i>n</i>-VSV) based on a two-dimensional (2D) ferroelectric semiconductor where resistance of <i>n</i>-VSV is controlled by a ferroelectric domain wall between two uniformly polarized domains. Focusing on the 1T″ phase of MoS<sub>2</sub>, which is known to be ferroelectric down to a monolayer and using density functional theory combined with quantum transport calculations, we demonstrate that switching between the uniformly polarized state and the state with oppositely polarized domains separated by a domain wall results in a resistance change of as high as 10<sup>7</sup>. This giant VSV effect occurs due to transmission being strongly dependent on matching (mismatching) the valley-dependent spin polarization in the two domains with the same (opposite) ferroelectric polarization orientations, when the chemical potential of 1T″-MoS<sub>2</sub> lies within the spin-split valleys. The proposed <i>n</i>-VSV can be employed as a functional device for high-performance nonvolatile valleytronics.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"7 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968599","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}
Bhaskar Sharma, Hagay Kohay, Sandeep Sharma, Marina Youngblood, Jarad P. Cochran, Jason M. Unrine, Olga V. Tsyusko, Gregory V. Lowry, Juan Pablo Giraldo
Nitrogen fertilizer delivery inefficiencies limit crop productivity and contribute to environmental pollution. Herein, we developed Zn- and Fe-doped hydroxyapatite nanomaterials (ZnHAU, FeHAU) loaded with urea (∼26% N) through hydrogen bonding and metal–ligand interactions. The nanomaterials attach to the leaf epidermal cuticle and localize in the apoplast of leaf epidermal cells, triggering a slow N release at acidic conditions (pH 5.8) that promote wheat (Triticum aestivum) growth and increased N uptake compared to conventional urea fertilizers. ZnHAU and FeHAU exhibited prolonged N release compared to urea in model plant apoplast fluid pH in vitro (up to 2 days) and in leaf membranes in plants (up to 10 days) with a high N retention (32% to 53%) under simulated high rainfall events (50 mm). Foliar N delivery doses of up to 4% as ZnHAU and FeHAU did not induce toxicity in plant cells. The foliar-applied ZnHAU and FeHAU enhanced fresh and dry biomass by ∼214% and ∼161%, and N uptake by ∼108% compared to foliar-applied urea under low soil N conditions in greenhouse experiments. Controlled N release by leaf-attached nanomaterials improves N delivery and use efficiency in crop plants, creating nanofertilizers with reduced environmental impact.
{"title":"Controlled Nitrogen Release by Hydroxyapatite Nanomaterials in Leaves Enhances Plant Growth and Nitrogen Uptake","authors":"Bhaskar Sharma, Hagay Kohay, Sandeep Sharma, Marina Youngblood, Jarad P. Cochran, Jason M. Unrine, Olga V. Tsyusko, Gregory V. Lowry, Juan Pablo Giraldo","doi":"10.1021/acsnano.4c16362","DOIUrl":"https://doi.org/10.1021/acsnano.4c16362","url":null,"abstract":"Nitrogen fertilizer delivery inefficiencies limit crop productivity and contribute to environmental pollution. Herein, we developed Zn- and Fe-doped hydroxyapatite nanomaterials (ZnHAU, FeHAU) loaded with urea (∼26% N) through hydrogen bonding and metal–ligand interactions. The nanomaterials attach to the leaf epidermal cuticle and localize in the apoplast of leaf epidermal cells, triggering a slow N release at acidic conditions (pH 5.8) that promote wheat (<i>Triticum aestivum</i>) growth and increased N uptake compared to conventional urea fertilizers. ZnHAU and FeHAU exhibited prolonged N release compared to urea in model plant apoplast fluid pH in vitro (up to 2 days) and in leaf membranes in plants (up to 10 days) with a high N retention (32% to 53%) under simulated high rainfall events (50 mm). Foliar N delivery doses of up to 4% as ZnHAU and FeHAU did not induce toxicity in plant cells. The foliar-applied ZnHAU and FeHAU enhanced fresh and dry biomass by ∼214% and ∼161%, and N uptake by ∼108% compared to foliar-applied urea under low soil N conditions in greenhouse experiments. Controlled N release by leaf-attached nanomaterials improves N delivery and use efficiency in crop plants, creating nanofertilizers with reduced environmental impact.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"29 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968600","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}
Chunliang Zhang, Chunyuan Wang, Ruitao Cha, Qinghua Meng, Zhan Hu, Yang Sun, Zulan Li, Min Xiao, Yan Zhang, Xingyu Jiang
Extracellular matrix (ECM)-based small-diameter vascular grafts (SDVGs, inner diameter (ID) < 6 mm) hold great promise for clinical applications. However, existing ECM-based SDVGs suffer from limited donor availability, complex purification, high cost, and insufficient mechanical properties. SDVGs with ECM-like structure and function, and good mechanical properties were rapidly prepared by optimizing common materials and preparation, which can improve their clinical prospects. Here, we rapidly prepared an electrospinning film-collagen/red blood cell membrane-genipin hydrogel tube (ES-C/Rm-G-ht, ID = 2 mm) by the combination of the cross-linking of genipin, plastic compression, electrospinning, and rolling without a biological adhesive, which had a shorter preparation time of less than 17 h compared to the existing ECM-based SDVGs (preparation time of 4–18 weeks). ES-C/Rm-G-ht exhibited a layered honeycomb-like structure and demonstrated the ECM-like functions to promote the proliferation and migration of endothelial cells, and prevent thrombus and inflammation. Furthermore, ES-C/Rm-G-ht, possessing sufficient mechanical strength, showed high patency, rapid endothelialization (95%), good regeneration of smooth muscle cell layers and ECM, and effective antistenosis capability after implantation in the rabbit’s carotid artery for 31 days. This work provides a straightforward, cost-effective, and promising strategy to prepare SDVGs with ECM-like structure and function, which is an ideal alternative for vascular grafts and autologous vessels in the current clinic.
{"title":"Rapid Preparation of Collagen/Red Blood Cell Membrane Tubes for Stenosis-Free Vascular Regeneration","authors":"Chunliang Zhang, Chunyuan Wang, Ruitao Cha, Qinghua Meng, Zhan Hu, Yang Sun, Zulan Li, Min Xiao, Yan Zhang, Xingyu Jiang","doi":"10.1021/acsnano.4c11919","DOIUrl":"https://doi.org/10.1021/acsnano.4c11919","url":null,"abstract":"Extracellular matrix (ECM)-based small-diameter vascular grafts (SDVGs, inner diameter (ID) < 6 mm) hold great promise for clinical applications. However, existing ECM-based SDVGs suffer from limited donor availability, complex purification, high cost, and insufficient mechanical properties. SDVGs with ECM-like structure and function, and good mechanical properties were rapidly prepared by optimizing common materials and preparation, which can improve their clinical prospects. Here, we rapidly prepared an electrospinning film-collagen/red blood cell membrane-genipin hydrogel tube (ES-C/Rm-G-ht, ID = 2 mm) by the combination of the cross-linking of genipin, plastic compression, electrospinning, and rolling without a biological adhesive, which had a shorter preparation time of less than 17 h compared to the existing ECM-based SDVGs (preparation time of 4–18 weeks). ES-C/Rm-G-ht exhibited a layered honeycomb-like structure and demonstrated the ECM-like functions to promote the proliferation and migration of endothelial cells, and prevent thrombus and inflammation. Furthermore, ES-C/Rm-G-ht, possessing sufficient mechanical strength, showed high patency, rapid endothelialization (95%), good regeneration of smooth muscle cell layers and ECM, and effective antistenosis capability after implantation in the rabbit’s carotid artery for 31 days. This work provides a straightforward, cost-effective, and promising strategy to prepare SDVGs with ECM-like structure and function, which is an ideal alternative for vascular grafts and autologous vessels in the current clinic.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"6 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975426","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}
Yuna Song, Zhongtao Duan, Lei Peng, Juan Zhang, Xun Zhu, Qi Feng, Zhihao Ji, Yuqing Zou, Jingying Zhang, Ziyang Li, Zongzhi Zhang, Xiao-Lei Zhang, Fengxian Xie, Hao Zhang, Qingyuan Jin
The formation of large polarons resulting from the Fröhlich coupling of photogenerated carriers with the polarized crystal lattice is considered crucial in shaping the outstanding optoelectronic properties in hybrid organic–inorganic perovskite crystals. Until now, the initial polaron dynamics after photoexcitation have remained elusive in the hybrid perovskite system. Here, based on the terahertz time-domain spectroscopy and optical-pump terahertz probe, we access the nature of interplay between photoexcited unbound charge carriers and optical phonons in MAPbBr3 within the initial 5 ps after excitation and have demonstrated the simultaneous existence of both electron- and hole-polarons, together with the photogenerated carrier dynamic process. Two resonant peaks in the frequency-dependent photoconductivity are interpreted by the Drude–Smith–Lorentz model along with the ab initio excitation calculation, revealing that the electron-/hole-polaron is related to the vibration modes of the stretched/contracted Pb–Br bond. The red /blue shift of the corresponding peaks as the fingerprints of electron-/hole-polaron provides a channel for observing their dynamic behavior. Different from polarons with long lifetime (>300 ps) in single-crystalline grains, we observed in thin films the transient process from the formation to the dissociation of polarons occurring at timescales within ∼5 ps, resulting from the Mott phase transition for carriers at high concentrations. Moreover, the observation of the polaron dynamic process of the virtual state-assisted band gap transition (800 nm excitation) further reveals the competition of carriers cooling and polaron formation with photocarrier density. Our observations demonstrate a strategy for direct observation and manipulation of bipolar polaron transport in hybrid perovskites.
{"title":"Photoinduced Fröhlich Interaction-Driven Distinct Electron- and Hole-Polaron Behaviors in Hybrid Organic–Inorganic Perovskites by Ultrafast Terahertz Probes","authors":"Yuna Song, Zhongtao Duan, Lei Peng, Juan Zhang, Xun Zhu, Qi Feng, Zhihao Ji, Yuqing Zou, Jingying Zhang, Ziyang Li, Zongzhi Zhang, Xiao-Lei Zhang, Fengxian Xie, Hao Zhang, Qingyuan Jin","doi":"10.1021/acsnano.4c12035","DOIUrl":"https://doi.org/10.1021/acsnano.4c12035","url":null,"abstract":"The formation of large polarons resulting from the Fröhlich coupling of photogenerated carriers with the polarized crystal lattice is considered crucial in shaping the outstanding optoelectronic properties in hybrid organic–inorganic perovskite crystals. Until now, the initial polaron dynamics after photoexcitation have remained elusive in the hybrid perovskite system. Here, based on the terahertz time-domain spectroscopy and optical-pump terahertz probe, we access the nature of interplay between photoexcited unbound charge carriers and optical phonons in MAPbBr<sub>3</sub> within the initial 5 ps after excitation and have demonstrated the simultaneous existence of both electron- and hole-polarons, together with the photogenerated carrier dynamic process. Two resonant peaks in the frequency-dependent photoconductivity are interpreted by the Drude–Smith–Lorentz model along with the ab initio excitation calculation, revealing that the electron-/hole-polaron is related to the vibration modes of the stretched/contracted Pb–Br bond. The red /blue shift of the corresponding peaks as the fingerprints of electron-/hole-polaron provides a channel for observing their dynamic behavior. Different from polarons with long lifetime (>300 ps) in single-crystalline grains, we observed in thin films the transient process from the formation to the dissociation of polarons occurring at timescales within ∼5 ps, resulting from the Mott phase transition for carriers at high concentrations. Moreover, the observation of the polaron dynamic process of the virtual state-assisted band gap transition (800 nm excitation) further reveals the competition of carriers cooling and polaron formation with photocarrier density. Our observations demonstrate a strategy for direct observation and manipulation of bipolar polaron transport in hybrid perovskites.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"223 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968604","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 non-ion conducting byproducts on zinc anode is notoriously detrimental to aqueous zinc-ion batteries (AZIBs). Herein, we successfully transform a representative detrimental byproduct, crystalline zinc hydroxide sulfate (ZHS) to fast-ion conducting solid-electrolyte interphase (SEI) via amorphization and fluorination induced by suspending CaF2 nanoparticles in dilute sulfate electrolytes. Distinct from widely reported nonhomogeneous organic–inorganic hybrid SEIs that exhibit structural and chemical instability, the designed single-phase SEI is homogeneous, mechanically robust, and chemically stable. These characteristics of the SEI facilitate the prevention of zinc dendrite growth and reduction of capacity loss during long-term cycling. Importantly, AZIB full cells based on this SEI-forming electrolyte exhibit exceptional stability over 20,000 cycles at 3 A/g with a charging voltage of 2.2 V without short circuits and electrolyte dry-out. This work suggests avenues for designing SEIs on a metal anode and provides insights into associated SEI chemistry.
{"title":"Transforming Detrimental Crystalline Zinc Hydroxide Sulfate to Homogeneous Fluorinated Amorphous Solid–Electrolyte Interphase on Zinc Anode","authors":"Siyu Tian, Taesoon Hwang, Zhuoxun Zhang, Shiwen Wu, Amirarsalan Mashhadian, Renzheng Zhang, Tye Milazzo, Tengfei Luo, Ruda Jian, Tianyi Li, Kyeongjae Cho, Guoping Xiong","doi":"10.1021/acsnano.4c04795","DOIUrl":"https://doi.org/10.1021/acsnano.4c04795","url":null,"abstract":"The formation of non-ion conducting byproducts on zinc anode is notoriously detrimental to aqueous zinc-ion batteries (AZIBs). Herein, we successfully transform a representative detrimental byproduct, crystalline zinc hydroxide sulfate (ZHS) to fast-ion conducting solid-electrolyte interphase (SEI) via amorphization and fluorination induced by suspending CaF<sub>2</sub> nanoparticles in dilute sulfate electrolytes. Distinct from widely reported nonhomogeneous organic–inorganic hybrid SEIs that exhibit structural and chemical instability, the designed single-phase SEI is homogeneous, mechanically robust, and chemically stable. These characteristics of the SEI facilitate the prevention of zinc dendrite growth and reduction of capacity loss during long-term cycling. Importantly, AZIB full cells based on this SEI-forming electrolyte exhibit exceptional stability over 20,000 cycles at 3 A/g with a charging voltage of 2.2 V without short circuits and electrolyte dry-out. This work suggests avenues for designing SEIs on a metal anode and provides insights into associated SEI chemistry.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"19 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975417","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 emergence of multidrug-resistant (MDR) pathogens, coupled with the limited effectiveness of existing antibiotics in eradicating biofilms, presents a significant threat to global health care. This critical situation underscores the urgent need for the discovery and development of antimicrobial agents. Recently, peptide-derived antimicrobial nanomaterials have shown promise in combating such infections. Amino acid noncovalent forces, notably π–π stacking and electrostatic interactions, remain underutilized for guiding the coassembly of peptides into bacteriostatic nanomaterials. Thus, we constructed a dimeric nanopeptide system using the disulfide bonds of cysteine. The self-assembly of dimeric peptides into nanofibers was realized by the interaction of π–π aromatic amino acids (Trp, Phe, and Pyr) and the electrostatic attraction between oppositely charged amino acids (Asp and Arg). The optimal dimeric peptide 2D2W exhibits potent antibacterial activity against resistant bacteria and is nontoxic. Mechanistically, 2D2W penetrated the outer membrane after electrostatic adsorption, resulting in plasma membrane depolarization, homeostatic disruption, and ultimately bacterial death. In a mouse model of peritonitis, 2D2W demonstrated efficacy in the in vivo treatment of bacterial infections. In conclusion, the design of dimeric nanopeptides co-driven by intermolecular forces provides a promising avenue for the development of high-performance antimicrobial nanomaterials. These advances may also facilitate the application and advancement of peptide-based bacteriostatic agents in clinical practice.
{"title":"Combating Antibiotic-Resistant Bacterial Infection Using Coassembled Dimeric Antimicrobial Peptide-Based Nanofibers","authors":"Guoyu Li, Haoran Deng, Wanying Xu, Wenwen Chen, Zhenheng Lai, Yongjie Zhu, Licong Zhang, Changxuan Shao, Anshan Shan","doi":"10.1021/acsnano.4c09347","DOIUrl":"https://doi.org/10.1021/acsnano.4c09347","url":null,"abstract":"The emergence of multidrug-resistant (MDR) pathogens, coupled with the limited effectiveness of existing antibiotics in eradicating biofilms, presents a significant threat to global health care. This critical situation underscores the urgent need for the discovery and development of antimicrobial agents. Recently, peptide-derived antimicrobial nanomaterials have shown promise in combating such infections. Amino acid noncovalent forces, notably π–π stacking and electrostatic interactions, remain underutilized for guiding the coassembly of peptides into bacteriostatic nanomaterials. Thus, we constructed a dimeric nanopeptide system using the disulfide bonds of cysteine. The self-assembly of dimeric peptides into nanofibers was realized by the interaction of π–π aromatic amino acids (Trp, Phe, and Pyr) and the electrostatic attraction between oppositely charged amino acids (Asp and Arg). The optimal dimeric peptide 2D2W exhibits potent antibacterial activity against resistant bacteria and is nontoxic. Mechanistically, 2D2W penetrated the outer membrane after electrostatic adsorption, resulting in plasma membrane depolarization, homeostatic disruption, and ultimately bacterial death. In a mouse model of peritonitis, 2D2W demonstrated efficacy in the in vivo treatment of bacterial infections. In conclusion, the design of dimeric nanopeptides co-driven by intermolecular forces provides a promising avenue for the development of high-performance antimicrobial nanomaterials. These advances may also facilitate the application and advancement of peptide-based bacteriostatic agents in clinical practice.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"36 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968326","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}
Thermally driven membrane desalination processes have garnered significant interest for their potential in the treatment of hypersaline wastewater. However, achieving high rejection rates for volatiles while maintaining a high water flux remains a considerable challenge. Herein, we propose a thermo-osmosis-evaporation (TOE) system that utilizes molecular intercalation-regulated graphene oxide (GO) as the thermo-osmotic selective permeation layer, positioned on a hydrophobic poly(vinylidene fluoride) fibrous membrane serving as the thermo-evaporation layer. By carefully constructing architectural interlaminar nanochannels of GO membranes via simultaneously confining small molecules to enlarge the interlayer spacing and incorporating polymers within the GO interlayers to create a dense network, the resultant demonstrates a rejection rate of 100% for NaCl and 97.41% for volatile phenylamine, with a water permeance of 63.80 L m–2 h–1 at a temperature difference of 40 °C, outperforming previously reported GO-based membranes. Simulation and calculation results reveal that the polymer network between the GO interlayers facilitates the high-efficiency separation of nonvolatile ions and volatile molecules, while the enlarged channels reduce vapor diffusion resistance. This study provides valuable insights for the design of advanced membranes and serves as inspiration for the continued development of the TOE system for complex hypersaline wastewater treatment.
{"title":"Volatile Sieving Using Architecturally Designed Nanochannel Lamellar Membranes in Membrane Desalination","authors":"Zhigao Zhu, Xiaohui Wang, Yujun Zhou, Junwen Qi, Yue Yang, Wei Wang, Jiansheng Li","doi":"10.1021/acsnano.4c15010","DOIUrl":"https://doi.org/10.1021/acsnano.4c15010","url":null,"abstract":"Thermally driven membrane desalination processes have garnered significant interest for their potential in the treatment of hypersaline wastewater. However, achieving high rejection rates for volatiles while maintaining a high water flux remains a considerable challenge. Herein, we propose a thermo-osmosis-evaporation (TOE) system that utilizes molecular intercalation-regulated graphene oxide (GO) as the thermo-osmotic selective permeation layer, positioned on a hydrophobic poly(vinylidene fluoride) fibrous membrane serving as the thermo-evaporation layer. By carefully constructing architectural interlaminar nanochannels of GO membranes via simultaneously confining small molecules to enlarge the interlayer spacing and incorporating polymers within the GO interlayers to create a dense network, the resultant demonstrates a rejection rate of 100% for NaCl and 97.41% for volatile phenylamine, with a water permeance of 63.80 L m<sup>–2</sup> h<sup>–1</sup> at a temperature difference of 40 °C, outperforming previously reported GO-based membranes. Simulation and calculation results reveal that the polymer network between the GO interlayers facilitates the high-efficiency separation of nonvolatile ions and volatile molecules, while the enlarged channels reduce vapor diffusion resistance. This study provides valuable insights for the design of advanced membranes and serves as inspiration for the continued development of the TOE system for complex hypersaline wastewater treatment.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"22 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975220","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}
Yashi Wang, Sheng Yin, Dan He, Yujia Zhang, Ziyan Dong, Zhipeng Tian, Jiayu Li, Fang Chen, Yang Wang, Man Li, Qin He
Endolysosomal degradation of small interfering RNA (siRNA) significantly reduces the efficacy of RNA interference (RNAi) delivered by nonviral systems. Leveraging Golgi apparatus/endoplasmic reticulum (Golgi/ER) transport can help siRNA bypass the endolysosomal degradation pathway, but this approach may also result in insufficient siRNA release and an increased risk of Golgi/ER-mediated exocytosis. To address these challenges, we developed two distinct strategies using a nanocomplex of cell-penetrating poly(disulfide)s and chondroitin sulfate, which enhances targeted internalization, Golgi transport, and rapid cytoplasmic release of loaded siRNA. In the first strategy, monensin synergy was found to enhance RNAi by inhibiting both exocytosis and autophagic degradation. In the second strategy, a “directed sorting” approach based on KDEL peptide-mediated retrograde transport was introduced. By conjugation of the KDEL peptide to chondroitin sulfate, Golgi-to-ER transport was promoted, reducing “random” Golgi/ER-related exocytosis. These two strategies operate alternatively to achieve high-efficiency RNAi with a significant therapeutic potential. Notably, in a mouse melanoma model using anti-Bcl-2 siRNA, the strategies achieved tumor inhibition rates of 87.1 and 90.1%, respectively. These two strategies, based on “targeting” and “anchoring” Golgi/ER, provide potent solutions to overcome the challenges of cellular internalization, intracellular release, and exocytosis in efficient siRNA delivery.
{"title":"Dual Strategies Based on Golgi Apparatus/Endoplasmic Reticulum Targeting and Anchoring for High-Efficiency siRNA Delivery and Tumor RNAi Therapy","authors":"Yashi Wang, Sheng Yin, Dan He, Yujia Zhang, Ziyan Dong, Zhipeng Tian, Jiayu Li, Fang Chen, Yang Wang, Man Li, Qin He","doi":"10.1021/acsnano.4c14778","DOIUrl":"https://doi.org/10.1021/acsnano.4c14778","url":null,"abstract":"Endolysosomal degradation of small interfering RNA (siRNA) significantly reduces the efficacy of RNA interference (RNAi) delivered by nonviral systems. Leveraging Golgi apparatus/endoplasmic reticulum (Golgi/ER) transport can help siRNA bypass the endolysosomal degradation pathway, but this approach may also result in insufficient siRNA release and an increased risk of Golgi/ER-mediated exocytosis. To address these challenges, we developed two distinct strategies using a nanocomplex of cell-penetrating poly(disulfide)s and chondroitin sulfate, which enhances targeted internalization, Golgi transport, and rapid cytoplasmic release of loaded siRNA. In the first strategy, monensin synergy was found to enhance RNAi by inhibiting both exocytosis and autophagic degradation. In the second strategy, a “directed sorting” approach based on KDEL peptide-mediated retrograde transport was introduced. By conjugation of the KDEL peptide to chondroitin sulfate, Golgi-to-ER transport was promoted, reducing “random” Golgi/ER-related exocytosis. These two strategies operate alternatively to achieve high-efficiency RNAi with a significant therapeutic potential. Notably, in a mouse melanoma model using anti-Bcl-2 siRNA, the strategies achieved tumor inhibition rates of 87.1 and 90.1%, respectively. These two strategies, based on “targeting” and “anchoring” Golgi/ER, provide potent solutions to overcome the challenges of cellular internalization, intracellular release, and exocytosis in efficient siRNA delivery.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"197 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968602","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 exponential growth of the Internet of Things (IoTs) has led to the widespread deployment of millions of sensors, crucial for the sensing layer’s perception capabilities. In particular, there is a strong interest in intelligent photonic sensing. However, the current photonic sensing device and chip typically offer limited functionality, and the devices providing their power take up excessive amounts of space. There is a pressing need for smart, multifunctional sensing chips with the capability of intelligent recognition. Here, we propose and demonstrate the functionalities of a two-dimensional van der Waals photonic bipolar junction transistor (2D-vdW photonic BJT) in simultaneous sensing and discerning different wavelength bands of light. Also, a dual-function chip application is given. The optoelectronic detection characteristics in the vision-near-infrared (vis-NIR) band and photovoltaic characteristics are systematically studied. It exhibits negative photoconductivity (NPC) for the 1064 nm laser while maintaining positive photoconductivity (PPC) for the 638 and 1550 nm lasers. Also, the electrical tunable response is realized. Moreover, the function of this chip under real-application conditions has shown its efficacy in applications such as detecting dim light with ∼10 lx illuminance, identifying wavelength bands, and generating power photovoltaically. This work provides a solution for the interconnection of everything.
{"title":"van der Waals Photonic Bipolar Junction Transistors Capable of Simultaneously Discerning Wavelength Bands and Dual-Function Chip Application","authors":"Zhengrui Zhu, Liwei Liu, Shaozhi Deng, Ningsheng Xu","doi":"10.1021/acsnano.4c14065","DOIUrl":"https://doi.org/10.1021/acsnano.4c14065","url":null,"abstract":"The exponential growth of the Internet of Things (IoTs) has led to the widespread deployment of millions of sensors, crucial for the sensing layer’s perception capabilities. In particular, there is a strong interest in intelligent photonic sensing. However, the current photonic sensing device and chip typically offer limited functionality, and the devices providing their power take up excessive amounts of space. There is a pressing need for smart, multifunctional sensing chips with the capability of intelligent recognition. Here, we propose and demonstrate the functionalities of a two-dimensional van der Waals photonic bipolar junction transistor (2D-vdW photonic BJT) in simultaneous sensing and discerning different wavelength bands of light. Also, a dual-function chip application is given. The optoelectronic detection characteristics in the vision-near-infrared (vis-NIR) band and photovoltaic characteristics are systematically studied. It exhibits negative photoconductivity (NPC) for the 1064 nm laser while maintaining positive photoconductivity (PPC) for the 638 and 1550 nm lasers. Also, the electrical tunable response is realized. Moreover, the function of this chip under real-application conditions has shown its efficacy in applications such as detecting dim light with ∼10 lx illuminance, identifying wavelength bands, and generating power photovoltaically. This work provides a solution for the interconnection of everything.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"68 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968537","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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