The operation of all-solid-state lithium-metal batteries is primarily constrained by an inferior solid electrolyte. Here, we employ a porous dielectric fluorinated electrolyte to encapsulate a Li+ complex, achieving rapid and stable ion conduction throughout cycling. The electrolyte comprises a porous nanofiber (NF) skeleton made of dielectric fluorinated BaTiO3 (F-BaTiO3−δ) and all-trans block copolymer PVDF-b-PTFE, with an encapsulated poly(ethylene oxide) (PEO)-LiTFSI filler. The dielectric polarized NFs effectively dissociate LiTFSI to form a rapid conductive Li+ complex, while F-BaTiO3−δ bonds with PVDF-b-PTFE and PEO to create stable cross-phase Li+-conduction paths. This results in an electrolyte with a high room-temperature conductivity of 5.64 × 10–4 S cm–1 and a low activation energy of 0.21 eV. Additionally, the polarized electrolyte achieves dynamic interface stability by eliminating the space charge layer on the cathode and internal stress on the anode. The all-solid-state LiFePO4//Li batteries can cycle stably 1000 times at 0.5 C with a high capacity retention of 87.45%. Furthermore, the NCM811//Li and 30-Ah-pouch cells also demonstrate high cycling stability, showcasing potential commercial applications.
{"title":"Constructing a Dielectric Fluorinated Solid Electrolyte for Practically Operated All-Solid-State Lithium-Metal Batteries","authors":"Xianda Ma, Shuhui Ge, Shuo Chen, Liang Zhang, Rui Wang, Jianhua Yan, Shujie Liu, Bin Ding, Jianyong Yu","doi":"10.1021/acsnano.5c01171","DOIUrl":"https://doi.org/10.1021/acsnano.5c01171","url":null,"abstract":"The operation of all-solid-state lithium-metal batteries is primarily constrained by an inferior solid electrolyte. Here, we employ a porous dielectric fluorinated electrolyte to encapsulate a Li<sup>+</sup> complex, achieving rapid and stable ion conduction throughout cycling. The electrolyte comprises a porous nanofiber (NF) skeleton made of dielectric fluorinated BaTiO<sub>3</sub> (F-BaTiO<sub>3−δ</sub>) and all-trans block copolymer PVDF-<i>b</i>-PTFE, with an encapsulated poly(ethylene oxide) (PEO)-LiTFSI filler. The dielectric polarized NFs effectively dissociate LiTFSI to form a rapid conductive Li<sup>+</sup> complex, while F-BaTiO<sub>3−δ</sub> bonds with PVDF-<i>b</i>-PTFE and PEO to create stable cross-phase Li<sup>+</sup>-conduction paths. This results in an electrolyte with a high room-temperature conductivity of 5.64 × 10<sup>–4</sup> S cm<sup>–1</sup> and a low activation energy of 0.21 eV. Additionally, the polarized electrolyte achieves dynamic interface stability by eliminating the space charge layer on the cathode and internal stress on the anode. The all-solid-state LiFePO<sub>4</sub>//Li batteries can cycle stably 1000 times at 0.5 C with a high capacity retention of 87.45%. Furthermore, the NCM811//Li and 30-Ah-pouch cells also demonstrate high cycling stability, showcasing potential commercial applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"28 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518480","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}
Jia Chen, Zhuozhuo Tang, Da Zhu, Li Sheng, Kai Yang, Zhiguo Zhang, Jianlong Wang, Yaping Tang, Xiangming He, Hong Xu
Although Li-metal batteries have been widely used as high-capacity batteries, they are highly susceptible to electrolytes that lead to dendritic or dead Li growth, which significantly reduces the stability of Li-metal electrodes. Herein, we report an anionic covalent organic framework (sulfonate COF: Bd-COF) as a Li+-solvate dissociator that strips solvent molecules from encapsulated Li+ to stabilize Li-metal electrodes. The homogeneous and dense ionic COF separator was prepared using a template-assisted interface in-suit polymerization engineering. Notably, the well-developed anionic groups within the COF channels could as counter-charge ligands to Li+, that adsorb Li+-solvates and induce their partial desolvation. Meanwhile, the ordered anionic groups on the surface of COF pores provide continuous ion channels for Li+ migration, facilitating the removal of solvent molecules from Li+-solvated species. Combined with the dense nanoporous feature, the COF membrane was found to be effective in suppressing Li-dendrites and parasitic reactions. The Bd-COF/Celgard membrane realizes uniform Li deposition on Li-metal electrodes, exhibiting excellent cycling performance in Li-symmetric batteries and high-voltage Li-metal batteries with LiNi0.6Mn0.2Co0.2O2 cathodes, showcasing the application prospects of ion-conductive covalent organic frameworks in lithium battery separators.
{"title":"Stabilizing Li-Metal Electrode via Anion-Induced Desolvation in a Covalent Organic Framework Separator","authors":"Jia Chen, Zhuozhuo Tang, Da Zhu, Li Sheng, Kai Yang, Zhiguo Zhang, Jianlong Wang, Yaping Tang, Xiangming He, Hong Xu","doi":"10.1021/acsnano.5c00165","DOIUrl":"https://doi.org/10.1021/acsnano.5c00165","url":null,"abstract":"Although Li-metal batteries have been widely used as high-capacity batteries, they are highly susceptible to electrolytes that lead to dendritic or dead Li growth, which significantly reduces the stability of Li-metal electrodes. Herein, we report an anionic covalent organic framework (sulfonate COF: Bd-COF) as a Li<sup>+</sup>-solvate dissociator that strips solvent molecules from encapsulated Li<sup>+</sup> to stabilize Li-metal electrodes. The homogeneous and dense ionic COF separator was prepared using a template-assisted interface in-suit polymerization engineering. Notably, the well-developed anionic groups within the COF channels could as counter-charge ligands to Li<sup>+</sup>, that adsorb Li<sup>+</sup>-solvates and induce their partial desolvation. Meanwhile, the ordered anionic groups on the surface of COF pores provide continuous ion channels for Li<sup>+</sup> migration, facilitating the removal of solvent molecules from Li<sup>+</sup>-solvated species. Combined with the dense nanoporous feature, the COF membrane was found to be effective in suppressing Li-dendrites and parasitic reactions. The Bd-COF/Celgard membrane realizes uniform Li deposition on Li-metal electrodes, exhibiting excellent cycling performance in Li-symmetric batteries and high-voltage Li-metal batteries with LiNi<sub>0.6</sub>Mn<sub>0.2</sub>Co<sub>0.2</sub>O<sub>2</sub> cathodes, showcasing the application prospects of ion-conductive covalent organic frameworks in lithium battery separators.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"28 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143506828","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}
A first-principles approach for calculating ion separation in solution through two-dimensional (2D) membranes is proposed and applied. Ionic energy profiles across the membrane are obtained first, where solvation effects are simulated explicitly with machine-learning molecular dynamics, electrostatic corrections are applied to remove finite-size capacitive effects, and a mean-field treatment of the charging of the electrochemical double layer is used. Entropic contributions are assessed analytically and validated against thermodynamic integration. Ionic separations are then inferred through a microkinetic model of the filtration process, accounting for steady-state charge separation effects across the membrane. The approach is applied to Li+, Na+, K+ sieving through a crown-ether functionalized graphene membrane, with a case study of the mechanisms for a highly selective and efficient extraction of lithium from aqueous solutions.
{"title":"Ion Sieving in Two-Dimensional Membranes from First Principles","authors":"Nicéphore Bonnet, Nicola Marzari","doi":"10.1021/acsnano.4c13575","DOIUrl":"https://doi.org/10.1021/acsnano.4c13575","url":null,"abstract":"A first-principles approach for calculating ion separation in solution through two-dimensional (2D) membranes is proposed and applied. Ionic energy profiles across the membrane are obtained first, where solvation effects are simulated explicitly with machine-learning molecular dynamics, electrostatic corrections are applied to remove finite-size capacitive effects, and a mean-field treatment of the charging of the electrochemical double layer is used. Entropic contributions are assessed analytically and validated against thermodynamic integration. Ionic separations are then inferred through a microkinetic model of the filtration process, accounting for steady-state charge separation effects across the membrane. The approach is applied to Li<sup>+</sup>, Na<sup>+</sup>, K<sup>+</sup> sieving through a crown-ether functionalized graphene membrane, with a case study of the mechanisms for a highly selective and efficient extraction of lithium from aqueous solutions.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"54 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518475","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}
Huicheng Hu, Jing Liu, Jing Liu, Mohan Yuan, Haifei Ma, Binbin Wang, Ya Wang, Hang Xia, Junrui Yang, Liang Gao, Jianbing Zhang, Jiang Tang, Xinzheng Lan
Photodetectors based on HgTe colloidal quantum dots (CQDs) are expected to enable the next generation of infrared detection technology due to their low-cost preparation, widely tunable absorption, and direct integration with Si-based electronics. However, the fabrication of HgTe CQD photodiode focal plane arrays (FPAs) has been hampered by the creation of rectifying homojunctions through delicate doping modulation and the time-consuming layer-by-layer assembly of the QD photoactive layer. Herein we address these challenges by exploring energetically favored ZnO/HgTe/ZnTe double heterojunctions (DH), and by forming colloidally stable HgTe ink that enables one-step direct film deposition. The DH HgTe CQD photodiode operates over a broad spectral range from 400 to 1800 nm, comparable to that of uncooled InGaAs detectors, with a record peak EQE of 56% at 1600 nm. A short-wave infrared (SWIR) imager has been finally demonstrated through monolithic integration with a CMOS readout integrated circuit (ROIC) comprising 640 × 512 pixels. The DH architecture is beneficial for the construction of high-performance HgTe CQD photodiodes compatible with silicon chip integration.
{"title":"Double-Heterojunction-Based HgTe Colloidal Quantum Dot Imagers","authors":"Huicheng Hu, Jing Liu, Jing Liu, Mohan Yuan, Haifei Ma, Binbin Wang, Ya Wang, Hang Xia, Junrui Yang, Liang Gao, Jianbing Zhang, Jiang Tang, Xinzheng Lan","doi":"10.1021/acsnano.4c17257","DOIUrl":"https://doi.org/10.1021/acsnano.4c17257","url":null,"abstract":"Photodetectors based on HgTe colloidal quantum dots (CQDs) are expected to enable the next generation of infrared detection technology due to their low-cost preparation, widely tunable absorption, and direct integration with Si-based electronics. However, the fabrication of HgTe CQD photodiode focal plane arrays (FPAs) has been hampered by the creation of rectifying homojunctions through delicate doping modulation and the time-consuming layer-by-layer assembly of the QD photoactive layer. Herein we address these challenges by exploring energetically favored ZnO/HgTe/ZnTe double heterojunctions (DH), and by forming colloidally stable HgTe ink that enables one-step direct film deposition. The DH HgTe CQD photodiode operates over a broad spectral range from 400 to 1800 nm, comparable to that of uncooled InGaAs detectors, with a record peak EQE of 56% at 1600 nm. A short-wave infrared (SWIR) imager has been finally demonstrated through monolithic integration with a CMOS readout integrated circuit (ROIC) comprising 640 × 512 pixels. The DH architecture is beneficial for the construction of high-performance HgTe CQD photodiodes compatible with silicon chip integration.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"7 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518479","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}
Chenxu Liu, Lin Yang, Yongxiang Sun, Pan Huang, Yuan Yao, Yu Tian, Hongbo Zeng
Functional soft materials that swell in water often exhibit surface wrinkling, similar to the ridges formed on human skin after prolonged immersion, typically leading to reduced optical transmittance. Surprisingly, there is a scarcity of materials that are transparent underwater yet opaque in air, despite their vast potential in applications such as smart windows, periscopes, and information encryption. Herein, we report a hydrogel-based system comprising a polyacrylamide layer on polydimethylsiloxane (PDMS), demonstrating a reversible transition between opacity in air and high transparency in water or wet conditions. Upon water-induced swelling, the transmittance of the hydrogel layer markedly increases from 7.8% in air to 77.1% with excellent repeatability. This behavior enables applications such as optical encryption and decryption and water writing. Micro- and nanostructural analysis reveals that the optical switching arises from the reduction in local surface roughness upon hydrogel swelling. Furthermore, when employed as a smart window, the hydrogel layer effectively reduces solar power transmission by 36%, achieving a temperature reduction of 5.09 °C under direct sunlight while retaining heat in the absence of sunlight. These findings highlight the hydrogel layer on PDMS as a versatile platform for water-responsive smart devices, offering exciting opportunities in optical encryption, interactive writing systems, and energy-efficient window technologies.
{"title":"Hydrogel-Coated Polydimethylsiloxane with Reversible Transparency for Advanced Optical Switching","authors":"Chenxu Liu, Lin Yang, Yongxiang Sun, Pan Huang, Yuan Yao, Yu Tian, Hongbo Zeng","doi":"10.1021/acsnano.4c17403","DOIUrl":"https://doi.org/10.1021/acsnano.4c17403","url":null,"abstract":"Functional soft materials that swell in water often exhibit surface wrinkling, similar to the ridges formed on human skin after prolonged immersion, typically leading to reduced optical transmittance. Surprisingly, there is a scarcity of materials that are transparent underwater yet opaque in air, despite their vast potential in applications such as smart windows, periscopes, and information encryption. Herein, we report a hydrogel-based system comprising a polyacrylamide layer on polydimethylsiloxane (PDMS), demonstrating a reversible transition between opacity in air and high transparency in water or wet conditions. Upon water-induced swelling, the transmittance of the hydrogel layer markedly increases from 7.8% in air to 77.1% with excellent repeatability. This behavior enables applications such as optical encryption and decryption and water writing. Micro- and nanostructural analysis reveals that the optical switching arises from the reduction in local surface roughness upon hydrogel swelling. Furthermore, when employed as a smart window, the hydrogel layer effectively reduces solar power transmission by 36%, achieving a temperature reduction of 5.09 °C under direct sunlight while retaining heat in the absence of sunlight. These findings highlight the hydrogel layer on PDMS as a versatile platform for water-responsive smart devices, offering exciting opportunities in optical encryption, interactive writing systems, and energy-efficient window technologies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"57 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143506829","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}
Dianri Wang, Yun Wang, Sicheng Zhang, Xueting Yang, Yan Yang, Teng Han, Yi Luo, Chunyan Shui, Mu Yang, Yunfeng Lin, Chao Li
Oral squamous cell carcinoma (OSCC) represents a heterogeneous group of malignancies originating from the mucosal lining of the oral cavity. Current treatment modalities primarily involve surgery, chemotherapy, and radiotherapy. Despite the use of multimodal therapy, the 5 year overall survival rate for OSCC remains around 50%, underscoring the need for the development of nontoxic agents with potent antitumor activity. Extracellular vesicles (EVs) are nanoscale, membrane-bound structures that can selectively deliver small molecules, nucleic acids, and proteins to target cells, making them a promising platform for drug delivery in cancer therapy. Strategies to improve the uptake of EVs and enhance the delivery of therapeutic molecules to target cells are critical for advancing precision medicine. Tetrahedral DNA nanostructures (TDNs) have shown significant potential in facilitating drug endocytosis and delivery, as well as improving tissue penetration. In this study, TDN@EVs were conducted by modifying the membrane surface of M1-EVs with TDNs, which demonstrated improved biological stability and drug delivery efficiency compared to unmodified EVs. In vitro and in vivo experiments showed that TDN@EVs significantly inhibited OSCC cell proliferation and migration while promoting apoptosis. TDN@EVs exhibited superior drug penetration properties, further amplifying their antitumor effects. Proteomic analysis identified Hsc70 as the key protein responsible for the antitumor activity of the TDN@EVs. The efficient delivery of Hsc70 into tumor cells by TDN@EVs led to the degradation of GPX4, inducing ferroptosis, mitochondrial stress, and DNA damage in tumor cells. These findings highlight the potential of TDN@EVs as an effective and safe approach for cancer therapy. In conclusion, TDN@EVs present as a promising effective strategy for the targeted delivery of therapeutic agents in OSCC treatment, offering enhanced biological stability, efficient drug delivery, and significant antitumor effects.
{"title":"Tetrahedral-DNA-Nanostructure-Modified Engineered Extracellular Vesicles Enhance Oral Squamous Cell Carcinomas Therapy by Targeting GPX4","authors":"Dianri Wang, Yun Wang, Sicheng Zhang, Xueting Yang, Yan Yang, Teng Han, Yi Luo, Chunyan Shui, Mu Yang, Yunfeng Lin, Chao Li","doi":"10.1021/acsnano.5c00674","DOIUrl":"https://doi.org/10.1021/acsnano.5c00674","url":null,"abstract":"Oral squamous cell carcinoma (OSCC) represents a heterogeneous group of malignancies originating from the mucosal lining of the oral cavity. Current treatment modalities primarily involve surgery, chemotherapy, and radiotherapy. Despite the use of multimodal therapy, the 5 year overall survival rate for OSCC remains around 50%, underscoring the need for the development of nontoxic agents with potent antitumor activity. Extracellular vesicles (EVs) are nanoscale, membrane-bound structures that can selectively deliver small molecules, nucleic acids, and proteins to target cells, making them a promising platform for drug delivery in cancer therapy. Strategies to improve the uptake of EVs and enhance the delivery of therapeutic molecules to target cells are critical for advancing precision medicine. Tetrahedral DNA nanostructures (TDNs) have shown significant potential in facilitating drug endocytosis and delivery, as well as improving tissue penetration. In this study, TDN@EVs were conducted by modifying the membrane surface of M1-EVs with TDNs, which demonstrated improved biological stability and drug delivery efficiency compared to unmodified EVs. In vitro and in vivo experiments showed that TDN@EVs significantly inhibited OSCC cell proliferation and migration while promoting apoptosis. TDN@EVs exhibited superior drug penetration properties, further amplifying their antitumor effects. Proteomic analysis identified Hsc70 as the key protein responsible for the antitumor activity of the TDN@EVs. The efficient delivery of Hsc70 into tumor cells by TDN@EVs led to the degradation of GPX4, inducing ferroptosis, mitochondrial stress, and DNA damage in tumor cells. These findings highlight the potential of TDN@EVs as an effective and safe approach for cancer therapy. In conclusion, TDN@EVs present as a promising effective strategy for the targeted delivery of therapeutic agents in OSCC treatment, offering enhanced biological stability, efficient drug delivery, and significant antitumor effects.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"49 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143518477","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}
Xudong Zhao, Xiang Liu, Tucan Chen, Han Xie, Shunji Li, Ying Zhang, Hongwei Zhang, Yulin Cao, Wei Du, Xiaojun Feng, Xin Liu, Yiwei Li, Peng Chen, Qiubai Li, Bi-Feng Liu
Exosomes present in the circulatory system demonstrate considerable promise for the diagnosis and treatment of diseases. Nevertheless, the complex nature of blood samples and the prevalence of highly abundant proteins pose a significant obstacle to prompt and effective isolation and functional evaluation of exosomes from blood. Here, we present a fully integrated lab-on-a-disc equipped with two nanofilters, also termed iExoDisc, which facilitates automated isolation of exosomes from 400 μL blood samples within 45 min. By integrating the plasma separation module, highly abundant protein removal module, and nanopore membrane-based total isolation module, the resulting exosomes exhibited significantly increased purity (∼3-6-fold) compared to conventional ultracentrifugation and polymer precipitation. Additionally, we then successfully performed nontargeted and targeted glycan profiling on exosomes derived from clinical triple-negative breast cancer (TNBC) patients using MALDI-TOF-MS and lectin microarray containing 56 kinds of lectins. The findings from both methodologies indicated that galactosylation and sialylation exhibit potential as diagnostic indicators for TNBC. Finally, by utilizing the exosome-specific glycosylated protein CD63 as a proof-of-concept, we successfully realized the integration of point-of-care on-chip exosome separation and in situ detection with 2 h. Thus, the iExoDisc provides a potential approach to early cancer detection, liquid biopsy, and point-of-care diagnosis.
{"title":"Fully Integrated Centrifugal Microfluidics for Rapid Exosome Isolation, Glycan Analysis, and Point-of-Care Diagnosis.","authors":"Xudong Zhao, Xiang Liu, Tucan Chen, Han Xie, Shunji Li, Ying Zhang, Hongwei Zhang, Yulin Cao, Wei Du, Xiaojun Feng, Xin Liu, Yiwei Li, Peng Chen, Qiubai Li, Bi-Feng Liu","doi":"10.1021/acsnano.4c16988","DOIUrl":"https://doi.org/10.1021/acsnano.4c16988","url":null,"abstract":"<p><p>Exosomes present in the circulatory system demonstrate considerable promise for the diagnosis and treatment of diseases. Nevertheless, the complex nature of blood samples and the prevalence of highly abundant proteins pose a significant obstacle to prompt and effective isolation and functional evaluation of exosomes from blood. Here, we present a fully integrated lab-on-a-disc equipped with two nanofilters, also termed iExoDisc, which facilitates automated isolation of exosomes from 400 μL blood samples within 45 min. By integrating the plasma separation module, highly abundant protein removal module, and nanopore membrane-based total isolation module, the resulting exosomes exhibited significantly increased purity (∼3-6-fold) compared to conventional ultracentrifugation and polymer precipitation. Additionally, we then successfully performed nontargeted and targeted glycan profiling on exosomes derived from clinical triple-negative breast cancer (TNBC) patients using MALDI-TOF-MS and lectin microarray containing 56 kinds of lectins. The findings from both methodologies indicated that galactosylation and sialylation exhibit potential as diagnostic indicators for TNBC. Finally, by utilizing the exosome-specific glycosylated protein CD63 as a proof-of-concept, we successfully realized the integration of point-of-care on-chip exosome separation and in situ detection with 2 h. Thus, the iExoDisc provides a potential approach to early cancer detection, liquid biopsy, and point-of-care diagnosis.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":""},"PeriodicalIF":15.8,"publicationDate":"2025-02-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143522191","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 interfacial wettability between electrodes and electrolytes could ensure sufficient physical contact and fast mass transfer at the gas–solid–liquid, solid–liquid, and solid–solid interfaces, which could improve the reaction kinetics and cycle stability of rechargeable metal-based batteries (RMBs). Herein, interfacial wettability engineering at multiphase interfaces is summarized from the electrolyte and electrode aspects to promote the interface reaction rate and durability of RMBs, which illustrates the revolution that is taking place in this field and thus provides inspiration for future developments in RMBs. Specifically, this review presents the principle of interfacial wettability at macro- and microscale and summarizes emerging applications concerning the interfacial wettability effect on mass transfer in RMBs. Moreover, deep insight into the future development of interfacial wettability is provided in the outlook. Therefore, this review not only provides insights into interfacial wettability engineering but also offers strategic guidance for wettability modification and optimization toward stable electrode–electrolyte interfaces for fast mass transfer in RMBs.
{"title":"Regulating Interfacial Wettability for Fast Mass Transfer in Rechargeable Metal-Based Batteries","authors":"Ruijuan Shi, Shilong Jiao, Zirui Yang, Zhihui Bo, Junrong Jiao, Yong Zhao","doi":"10.1021/acsnano.4c17836","DOIUrl":"https://doi.org/10.1021/acsnano.4c17836","url":null,"abstract":"The interfacial wettability between electrodes and electrolytes could ensure sufficient physical contact and fast mass transfer at the gas–solid–liquid, solid–liquid, and solid–solid interfaces, which could improve the reaction kinetics and cycle stability of rechargeable metal-based batteries (RMBs). Herein, interfacial wettability engineering at multiphase interfaces is summarized from the electrolyte and electrode aspects to promote the interface reaction rate and durability of RMBs, which illustrates the revolution that is taking place in this field and thus provides inspiration for future developments in RMBs. Specifically, this review presents the principle of interfacial wettability at macro- and microscale and summarizes emerging applications concerning the interfacial wettability effect on mass transfer in RMBs. Moreover, deep insight into the future development of interfacial wettability is provided in the outlook. Therefore, this review not only provides insights into interfacial wettability engineering but also offers strategic guidance for wettability modification and optimization toward stable electrode–electrolyte interfaces for fast mass transfer in RMBs.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"14 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496097","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}
Jingjing Cao, Wenji Zhan, Meng Ren, Yao Wang, Haifei Wang, Ni Zhang, Yuetian Chen, Tianfu Wang, Yanfeng Miao, Yixin Zhao
The application of promising perovskite light-emitting diodes (PeLEDs) faces a significant challenge known as efficiency roll-off, which refers to the decline in external quantum efficiency (EQE) at high current densities. This issue arises mainly from high trap densities in perovskite films and imbalanced carrier injection, which limit improvements in brightness and stability of PeLEDs. Here, we develop a green solvent strategy using γ-valerolactone (GVL) to suppress efficiency roll-off in PeLEDs. This strategy effectively slows down the crystallization kinetics, yielding cubic-phase formamidinium lead triiodide (α-FAPbI3) films with reduced trap states, enhanced charge carrier injection, and suppressed Auger recombination. As a result, we achieve a record radiance of 1411 W sr–1 m–2 for GVL-based PeLEDs. These PeLEDs exhibit a substantially reduced efficiency roll-off, maintaining an EQE above 20% even at a high current density of 900 mA cm–2. Our findings highlight the potential of the green solvent approach for developing high-brightness, high-efficiency PeLEDs for practical applications.
{"title":"High-Brightness Perovskite Light-Emitting Diodes with Suppressed Efficiency Roll-off Using the Green Solvent γ-Valerolactone","authors":"Jingjing Cao, Wenji Zhan, Meng Ren, Yao Wang, Haifei Wang, Ni Zhang, Yuetian Chen, Tianfu Wang, Yanfeng Miao, Yixin Zhao","doi":"10.1021/acsnano.4c17765","DOIUrl":"https://doi.org/10.1021/acsnano.4c17765","url":null,"abstract":"The application of promising perovskite light-emitting diodes (PeLEDs) faces a significant challenge known as efficiency roll-off, which refers to the decline in external quantum efficiency (EQE) at high current densities. This issue arises mainly from high trap densities in perovskite films and imbalanced carrier injection, which limit improvements in brightness and stability of PeLEDs. Here, we develop a green solvent strategy using γ-valerolactone (GVL) to suppress efficiency roll-off in PeLEDs. This strategy effectively slows down the crystallization kinetics, yielding cubic-phase formamidinium lead triiodide (α-FAPbI<sub>3</sub>) films with reduced trap states, enhanced charge carrier injection, and suppressed Auger recombination. As a result, we achieve a record radiance of 1411 W sr<sup>–1</sup> m<sup>–2</sup> for GVL-based PeLEDs. These PeLEDs exhibit a substantially reduced efficiency roll-off, maintaining an EQE above 20% even at a high current density of 900 mA cm<sup>–2</sup>. Our findings highlight the potential of the green solvent approach for developing high-brightness, high-efficiency PeLEDs for practical applications.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"18 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143506874","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}
Dasol Kim, Sungwon Kim, Jisu Jung, Jaeseung Kim, Sungwook Choi, Carl-Friedrich Schön, Changwoo Lee, Hyeonwook Lim, Jaehun Jeong, Sanghyuck Yu, Yeonsu Jeong, Hanjoo Lee, Sangsoo Kim, Daewoong Nam, Intae Eom, Dogeun Jang, Kyung Sook Kim, Seongil Im, Seungwu Han, Hyunjung Kim, Mann-Ho Cho
Disordering atomic structures offers a functionality hardly expected in ordered states, including phase-change memory and photonic computing, offering the potential to renovate von Neumann architecture for neuromorphic engineering with low latency. However, significant energy consumption during the disordering compromises the data reliability and integration efficiency, which is traditionally regarded to take place after melting. Here, we investigate time for disordering in isochronal and isochoric manners, challenging the conventional melt-quenching theory. The disordering times of pure Sb, Ag–In–Sb–Te, and In surpass that of InSb by over 50 times, despite a higher melting point and a lower laser absorption rate of Sb compared to InSb. This nontrivial contrast is elucidated by theoretical calculation that delocalized electrons enable flexible modification of bond lengths even below the melting points where undermined bond directionality provides room for atoms to depart from their original positions. Facilitated by delocalized electrons, specifically through metavalent and metallic bonding rather than covalent bonding, atoms can be disordered without undergoing melting, which aligns with the rapid disordering of Sb compared to that of InSb. The results bridge the unaddressed gap between chemical interaction and kinetic behaviors during the disordering and suggest design rules highlighting electron-delocalization rather than solely relying on melting points to improve energy efficiency.
{"title":"Nonmelting Disordering Facilitated by Electron Delocalization","authors":"Dasol Kim, Sungwon Kim, Jisu Jung, Jaeseung Kim, Sungwook Choi, Carl-Friedrich Schön, Changwoo Lee, Hyeonwook Lim, Jaehun Jeong, Sanghyuck Yu, Yeonsu Jeong, Hanjoo Lee, Sangsoo Kim, Daewoong Nam, Intae Eom, Dogeun Jang, Kyung Sook Kim, Seongil Im, Seungwu Han, Hyunjung Kim, Mann-Ho Cho","doi":"10.1021/acsnano.5c00755","DOIUrl":"https://doi.org/10.1021/acsnano.5c00755","url":null,"abstract":"Disordering atomic structures offers a functionality hardly expected in ordered states, including phase-change memory and photonic computing, offering the potential to renovate von Neumann architecture for neuromorphic engineering with low latency. However, significant energy consumption during the disordering compromises the data reliability and integration efficiency, which is traditionally regarded to take place after melting. Here, we investigate time for disordering in isochronal and isochoric manners, challenging the conventional melt-quenching theory. The disordering times of pure Sb, Ag–In–Sb–Te, and In surpass that of InSb by over 50 times, despite a higher melting point and a lower laser absorption rate of Sb compared to InSb. This nontrivial contrast is elucidated by theoretical calculation that delocalized electrons enable flexible modification of bond lengths even below the melting points where undermined bond directionality provides room for atoms to depart from their original positions. Facilitated by delocalized electrons, specifically through metavalent and metallic bonding rather than covalent bonding, atoms can be disordered without undergoing melting, which aligns with the rapid disordering of Sb compared to that of InSb. The results bridge the unaddressed gap between chemical interaction and kinetic behaviors during the disordering and suggest design rules highlighting electron-delocalization rather than solely relying on melting points to improve energy efficiency.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496103","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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：