Natalie Marie Petryk, Nghia Le Ba Thai, Leo Vikram Saldanha, Shawn Tyrin Sutherland, Mary Beth B. Monroe
Polyurethane (PUr) shape memory polymer (SMP) foams have demonstrated excellent bleeding control in traumatic wounds. Unlike the current clinically available treatment options, PUr SMP foams can address noncompressible bleeds, are safe for prolonged use, and are highly tunable, offering broad functionalities like biodegradation and antimicrobial properties. Despite their hemostatic efficacy, PUrs are entirely synthetic, which limits their long-term healing capacity if left in a wound to degrade. This work employed methods for facile incorporation of bioactive collagen and gelatin into PUr foams postfabrication to enhance their clotting efficacy and drive cell interactions. The procoagulant nature of collagen and gelatin increased the clotting accomplished by the PUr SMP foams. Additionally, the bioactive PUr SMP foams promoted cell attachment, spreading, and proliferation on foam pores, which could facilitate tissue migration into the scaffold and promote wound repair. Overall, a bioactive PUr SMP foam dressing could significantly improve traumatic wound healing outcomes.
{"title":"Bioactive Polyurethane Shape Memory Polymer Foam Dressings with Enhanced Blood and Cell Interactions for Improved Wound Healing","authors":"Natalie Marie Petryk, Nghia Le Ba Thai, Leo Vikram Saldanha, Shawn Tyrin Sutherland, Mary Beth B. Monroe","doi":"10.1021/acsami.5c02532","DOIUrl":"https://doi.org/10.1021/acsami.5c02532","url":null,"abstract":"Polyurethane (PUr) shape memory polymer (SMP) foams have demonstrated excellent bleeding control in traumatic wounds. Unlike the current clinically available treatment options, PUr SMP foams can address noncompressible bleeds, are safe for prolonged use, and are highly tunable, offering broad functionalities like biodegradation and antimicrobial properties. Despite their hemostatic efficacy, PUrs are entirely synthetic, which limits their long-term healing capacity if left in a wound to degrade. This work employed methods for facile incorporation of bioactive collagen and gelatin into PUr foams postfabrication to enhance their clotting efficacy and drive cell interactions. The procoagulant nature of collagen and gelatin increased the clotting accomplished by the PUr SMP foams. Additionally, the bioactive PUr SMP foams promoted cell attachment, spreading, and proliferation on foam pores, which could facilitate tissue migration into the scaffold and promote wound repair. Overall, a bioactive PUr SMP foam dressing could significantly improve traumatic wound healing outcomes.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"17 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143862447","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kashif Saleem Saqib, Tom James Embleton, Jae Hong Choi, Sung-Jae Won, Jahanzaib Ali, Kyungmok Ko, Sumyeong Choi, Mina Jo, Sungwoo Park, Joohyuk Park, Watchareeya Kaveevivitchai, Yoonkook Son, Woo-Jae Lee, Pilgun Oh
The correction to our original article involves only the designation of equal authorship contribution for the three co-first authors: Kashif Saleem Saqib, Tom James Embleton, and Jae Hong Choi. This correction does not affect the findings and conclusions of the article. Kashif Saleem Saqib, Tom James Embleton, and Jae Hong Choi contributed equally to this work. This article has not yet been cited by other publications.
{"title":"Correction to “Understanding the Carbon Additive/Sulfide Solid Electrolyte Interface in Nickel-Rich Cathode Composites and Prioritizing the Corresponding Interplay between the Electrical and Ionic Conductive Networks to Enhance All-Solid-State-Battery Rate Capability”","authors":"Kashif Saleem Saqib, Tom James Embleton, Jae Hong Choi, Sung-Jae Won, Jahanzaib Ali, Kyungmok Ko, Sumyeong Choi, Mina Jo, Sungwoo Park, Joohyuk Park, Watchareeya Kaveevivitchai, Yoonkook Son, Woo-Jae Lee, Pilgun Oh","doi":"10.1021/acsami.5c04614","DOIUrl":"https://doi.org/10.1021/acsami.5c04614","url":null,"abstract":"The correction to our original article involves only the designation of equal authorship contribution for the three co-first authors: Kashif Saleem Saqib, Tom James Embleton, and Jae Hong Choi. This correction does not affect the findings and conclusions of the article. Kashif Saleem Saqib, Tom James Embleton, and Jae Hong Choi contributed equally to this work. This article has not yet been cited by other publications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"62 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858274","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Gyoung Gug Jang, Jong K. Keum, Swapnamoy Dutta, Joshua T. Damron, Alexander I. Wiechert, Candice E. Halbert, James F. Browning, Dale K. Hensley, David Jassby, Marta C. Hatzell, Costas Tsouris
An aluminum (Al)-based electrocoagulation (EC) system can effectively remove dissolved silica and hardness in groundwater. The effectiveness of Al-EC in terms of pollutant removal, Faradaic efficiency, and energy consumption depends on the interfacial electrolysis or passivation of the electrode in water. Thus, understanding the electrolysis reaction at the liquid/electrode interface during operation is important for sustainable EC deployment. A continuous flow-through Al-EC system was tested with various groundwater simulants, i.e., chloride (Cl–)-based, sulfate (SO42–)-based, and mixed solutions. High pollutant removal with low energy consumption was observed in Cl–-based groundwater treatment, while low pollutant removal with high energy consumption was observed in SO42–-based groundwater. For example, the required energy per unit mass of Al dosing in SO42–-based groundwater is three times higher than that in Cl–-based groundwater at 10 mA/cm2. However, increasing the Cl– concentration significantly reduces this energy demand. In SO42–-based groundwater, the silicate removal efficiency drops from 85.1% to 24.0% compared to that for Cl–-based groundwater, while Mg2+ and Ca2+ removal efficiencies decrease to 0.6% from 15.8% and 5.7% from 44.8%, respectively. To better understand this EC performance, we used in situ neutron reflectometry (NR) to examine the interfacial dynamics of Al dissolution and passivation at a 100 nm scale occurring on the surface of the sacrificial Al electrodes during EC. Ex situ X-ray reflectometry (XRR) was also used to support the in situ NR results. Both NR and XRR results revealed that Al dissolution is influenced by the presence of Cl– in the simulants, while a passivating layer forms on the electrode in a SO42–-based solution. In the Cl–-based solution, anodic Al dissolution occurred locally and inhomogeneously across the surface of the Al anode film, resulting in a localized thickness reduction over time. In the SO42–-based solution, no apparent dissolution of the Al anode was identified. Instead, Al underwent oxidation, forming an amorphous Al2O3 surface layer within the Al electrode film that increased in thickness over time. In the mixed solution, both anodic Al dissolution and surface Al2O3 layer formation occurred, indicating that Al dissolution and surface Al2O3 layer formation are attributable to the Cl– and SO42– ions, respectively.
{"title":"Understanding the Dissolution and Passivation of an Aluminum Electrode during Electrocoagulation of Groundwater Using Neutron and X-ray Reflectometry","authors":"Gyoung Gug Jang, Jong K. Keum, Swapnamoy Dutta, Joshua T. Damron, Alexander I. Wiechert, Candice E. Halbert, James F. Browning, Dale K. Hensley, David Jassby, Marta C. Hatzell, Costas Tsouris","doi":"10.1021/acsami.5c02215","DOIUrl":"https://doi.org/10.1021/acsami.5c02215","url":null,"abstract":"An aluminum (Al)-based electrocoagulation (EC) system can effectively remove dissolved silica and hardness in groundwater. The effectiveness of Al-EC in terms of pollutant removal, Faradaic efficiency, and energy consumption depends on the interfacial electrolysis or passivation of the electrode in water. Thus, understanding the electrolysis reaction at the liquid/electrode interface during operation is important for sustainable EC deployment. A continuous flow-through Al-EC system was tested with various groundwater simulants, i.e., chloride (Cl<sup>–</sup>)-based, sulfate (SO<sub>4</sub><sup>2–</sup>)-based, and mixed solutions. High pollutant removal with low energy consumption was observed in Cl<sup>–</sup>-based groundwater treatment, while low pollutant removal with high energy consumption was observed in SO<sub>4</sub><sup>2–</sup>-based groundwater. For example, the required energy per unit mass of Al dosing in SO<sub>4</sub><sup>2–</sup>-based groundwater is three times higher than that in Cl<sup>–</sup>-based groundwater at 10 mA/cm<sup>2</sup>. However, increasing the Cl<sup>–</sup> concentration significantly reduces this energy demand. In SO<sub>4</sub><sup>2–</sup>-based groundwater, the silicate removal efficiency drops from 85.1% to 24.0% compared to that for Cl<sup>–</sup>-based groundwater, while Mg<sup>2+</sup> and Ca<sup>2+</sup> removal efficiencies decrease to 0.6% from 15.8% and 5.7% from 44.8%, respectively. To better understand this EC performance, we used in situ neutron reflectometry (NR) to examine the interfacial dynamics of Al dissolution and passivation at a 100 nm scale occurring on the surface of the sacrificial Al electrodes during EC. Ex situ X-ray reflectometry (XRR) was also used to support the in situ NR results. Both NR and XRR results revealed that Al dissolution is influenced by the presence of Cl<sup>–</sup> in the simulants, while a passivating layer forms on the electrode in a SO<sub>4</sub><sup>2–</sup>-based solution. In the Cl<sup>–</sup>-based solution, anodic Al dissolution occurred locally and inhomogeneously across the surface of the Al anode film, resulting in a localized thickness reduction over time. In the SO<sub>4</sub><sup>2–</sup>-based solution, no apparent dissolution of the Al anode was identified. Instead, Al underwent oxidation, forming an amorphous Al<sub>2</sub>O<sub>3</sub> surface layer within the Al electrode film that increased in thickness over time. In the mixed solution, both anodic Al dissolution and surface Al<sub>2</sub>O<sub>3</sub> layer formation occurred, indicating that Al dissolution and surface Al<sub>2</sub>O<sub>3</sub> layer formation are attributable to the Cl<sup>–</sup> and SO<sub>4</sub><sup>2–</sup> ions, respectively.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"19 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858279","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wide-bandgap perovskite solar cells (WBG PSCs) have been receiving increasing focus due to the ideal application in tandem photovoltaics. Nonetheless, WBG perovskites tend to form high-density trap states, causing serious nonradiative recombination and phase segregation, which is detrimental to the efficiency and stability of WBG PSCs. In this work, a dual-field passivation strategy facilitated by isopropylamine hydroiodide (i-PAI) is introduced, in effect, showing both the molecular dipole field passivation and interface electric field passivation. This strategy reduces the charge trap density of WBG perovskite and suppresses the phase segregation, which is supported by the analysis of the experimental data and simulation results. Moreover, the dual functional passivation mitigates the open-circuit-voltage (VOC) deficit of the WBG (1.65 eV) PSCs to 0.39 V and increases the efficiency to a competitive value of 22.21%. The device also exhibits excellent photostability, maintaining 84.2% of the initial efficiency after 1080 h of illumination under 1-sun white LED. This work showcases a pivotal pathway to defect passivation that can markedly enhancing both the efficiency and stability of wide-bandgap perovskite solar cells.
{"title":"Dual Field Passivation Strategy for High-Performance Wide-Bandgap Perovskite Solar Cells","authors":"Xuzheng Feng, Xing Li, Zhuoxin Li, Yufei Xue, Xianggang Chen, Xiaoxu Sun, Jixiang Tang, Shuyi Liu, Zishuo Wang, Yuhang Xie, Rui Jia, Songyuan Dai, Guoping Gao, Molang Cai","doi":"10.1021/acsami.4c20406","DOIUrl":"https://doi.org/10.1021/acsami.4c20406","url":null,"abstract":"Wide-bandgap perovskite solar cells (WBG PSCs) have been receiving increasing focus due to the ideal application in tandem photovoltaics. Nonetheless, WBG perovskites tend to form high-density trap states, causing serious nonradiative recombination and phase segregation, which is detrimental to the efficiency and stability of WBG PSCs. In this work, a dual-field passivation strategy facilitated by isopropylamine hydroiodide (i-PAI) is introduced, in effect, showing both the molecular dipole field passivation and interface electric field passivation. This strategy reduces the charge trap density of WBG perovskite and suppresses the phase segregation, which is supported by the analysis of the experimental data and simulation results. Moreover, the dual functional passivation mitigates the open-circuit-voltage (<i>V</i><sub>OC</sub>) deficit of the WBG (1.65 eV) PSCs to 0.39 V and increases the efficiency to a competitive value of 22.21%. The device also exhibits excellent photostability, maintaining 84.2% of the initial efficiency after 1080 h of illumination under 1-sun white LED. This work showcases a pivotal pathway to defect passivation that can markedly enhancing both the efficiency and stability of wide-bandgap perovskite solar cells.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"46 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858264","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sukyung Choi, Jeong Won Park, Hyunsu Cho, Jin-Wook Shin, Kukjoo Kim, O. Eun Kwon, Jong-Heon Yang, Chan-mo Kang, Chun-Won Byun, Sang-Don Jung
Organic light-emitting diodes (OLEDs) have tremendous potential in biotechnology, but their vulnerability to oxygen and moisture presents a significant challenge in encapsulation. In this study, we developed a multilayer thin-film encapsulation consisting of dual inorganic layers and Parylene-C, offering excellent protection and biocompatibility. This encapsulation enhances the suitability of OLEDs for flexible substrates and biological applications. The multilayer structure, composed of Al2O3/SiOxNy/Parylene-C, was fabricated entirely below 100 °C to ensure compatibility with temperature-sensitive OLEDs. The encapsulation also exhibited high transparency in the visible spectrum, making it ideal for top-emission OLEDs. We confirmed the stability of the OLED by immersing it in a biologically relevant environment, specifically 37 °C PBS solution, and demonstrated its excellent durability. Through direct cell growth experiments and MTT assay tests, the multilayer encapsulated OLEDs demonstrated high biocompatibility. To advance this work toward optogenetic applications, we fabricated flexible OLED-sensing electrode integrated devices on a polyimide substrate, incorporating 13 sensing electrodes and 12 OLEDs. The Al2O3/SiOxNy/Parylene-C encapsulation provided sufficient stability during the selective etching of the sensing electrode region while maintaining OLED protection. The device demonstrated stable operation after immersion in PBS at 37 °C and supported direct cell growth on its surface. Additionally, the OLED arrays remained well functional even when the polyimide substrate was bent. These results highlight the potential of our flexible OLED-sensing electrode integrated device as a promising platform for future optogenetic applications.
{"title":"Biocompatible Multilayered Encapsulation for Organic Light-Emitting Diodes","authors":"Sukyung Choi, Jeong Won Park, Hyunsu Cho, Jin-Wook Shin, Kukjoo Kim, O. Eun Kwon, Jong-Heon Yang, Chan-mo Kang, Chun-Won Byun, Sang-Don Jung","doi":"10.1021/acsami.4c22567","DOIUrl":"https://doi.org/10.1021/acsami.4c22567","url":null,"abstract":"Organic light-emitting diodes (OLEDs) have tremendous potential in biotechnology, but their vulnerability to oxygen and moisture presents a significant challenge in encapsulation. In this study, we developed a multilayer thin-film encapsulation consisting of dual inorganic layers and Parylene-C, offering excellent protection and biocompatibility. This encapsulation enhances the suitability of OLEDs for flexible substrates and biological applications. The multilayer structure, composed of Al<sub>2</sub>O<sub>3</sub>/SiO<sub><i>x</i></sub>N<sub><i>y</i></sub>/Parylene-C, was fabricated entirely below 100 °C to ensure compatibility with temperature-sensitive OLEDs. The encapsulation also exhibited high transparency in the visible spectrum, making it ideal for top-emission OLEDs. We confirmed the stability of the OLED by immersing it in a biologically relevant environment, specifically 37 °C PBS solution, and demonstrated its excellent durability. Through direct cell growth experiments and MTT assay tests, the multilayer encapsulated OLEDs demonstrated high biocompatibility. To advance this work toward optogenetic applications, we fabricated flexible OLED-sensing electrode integrated devices on a polyimide substrate, incorporating 13 sensing electrodes and 12 OLEDs. The Al<sub>2</sub>O<sub>3</sub>/SiO<sub><i>x</i></sub>N<sub><i>y</i></sub>/Parylene-C encapsulation provided sufficient stability during the selective etching of the sensing electrode region while maintaining OLED protection. The device demonstrated stable operation after immersion in PBS at 37 °C and supported direct cell growth on its surface. Additionally, the OLED arrays remained well functional even when the polyimide substrate was bent. These results highlight the potential of our flexible OLED-sensing electrode integrated device as a promising platform for future optogenetic applications.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"37 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853144","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The solution to societal problems such as energy, environmental, and biomedical issues lies in the development of functional material systems with the capacity to address these problems. In the course of human development, we are entering a new era in which nanostructure control is considered in the major development of functional materials. The new concept of nanoarchitectonics is particularly significant in this regard, as it comprehensively promotes further development of nanotechnology and its fusion with materials chemistry. The integration of nanoscale phenomena and macroscopic actions is imperative for practical production of functional materials with nanoscale structural precision. This review focuses on dynamic flow-assisted nanoarchitectonics, wherein we explore the organization and control of functional structures by external mechanical stimuli, predominantly fluid flow. The review then proceeds to select some examples and divide them into categories for the purpose of discussion: structural organization by (i) natural flow, (ii) flow or stress created with artificial equipment or devices (forced flow), and (iii) flow at a specific field, namely interfaces, that is, layer-by-layer (LbL) assembly and the LB method. The final perspective section discusses the future research directions and requirements for dynamic flow-assisted nanoarchitectonics. The meaningful and effective use of nanotechnology and nanoarchitectonics in materials science is set to be a major area of focus in the future, and dynamic flow-assisted nanoarchitectonics is poised to play a significant role in achieving this objective.
{"title":"Dynamic Flow-Assisted Nanoarchitectonics","authors":"Katsuhiko Ariga, Shuta Fujioka, Yu Yamashita","doi":"10.1021/acsami.5c03820","DOIUrl":"https://doi.org/10.1021/acsami.5c03820","url":null,"abstract":"The solution to societal problems such as energy, environmental, and biomedical issues lies in the development of functional material systems with the capacity to address these problems. In the course of human development, we are entering a new era in which nanostructure control is considered in the major development of functional materials. The new concept of nanoarchitectonics is particularly significant in this regard, as it comprehensively promotes further development of nanotechnology and its fusion with materials chemistry. The integration of nanoscale phenomena and macroscopic actions is imperative for practical production of functional materials with nanoscale structural precision. This review focuses on dynamic flow-assisted nanoarchitectonics, wherein we explore the organization and control of functional structures by external mechanical stimuli, predominantly fluid flow. The review then proceeds to select some examples and divide them into categories for the purpose of discussion: structural organization by (i) natural flow, (ii) flow or stress created with artificial equipment or devices (forced flow), and (iii) flow at a specific field, namely interfaces, that is, layer-by-layer (LbL) assembly and the LB method. The final perspective section discusses the future research directions and requirements for dynamic flow-assisted nanoarchitectonics. The meaningful and effective use of nanotechnology and nanoarchitectonics in materials science is set to be a major area of focus in the future, and dynamic flow-assisted nanoarchitectonics is poised to play a significant role in achieving this objective.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"33 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853226","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Cancer immunotherapies, such as immune checkpoint inhibitors, have advanced rapidly and achieved notable success, yet they face significant challenges due to poor response rates and immune-related adverse effects, particularly in cases of triple-negative breast cancer (TNBC). Photodynamic therapy (PDT) can initiate immunogenic cell death (ICD) by inducing endoplasmic reticulum (ER) stress, thereby enhancing the effectiveness of tumor immunotherapy. Herein, we develop potent PDT biomimetic liposomes (PB Lipo) locating the ER to realize a synergistic immuno-photodynamic treatment. The PB Lipo is prepared using the optimal ratios of the phospholipids in the ER membrane. It is then loaded with indocyanine green (ICG), a photosensitizer approved for clinical use. PB Lipo has the unique ability to accumulate in the ER via membrane fusion, leading to severe ER stress when exposed to near-infrared (NIR) laser light, thus intensifying ICD. In combination with the antiprogrammed death-ligand 1 (PD-L1) antibody (αPD-L1), PB Lipo significantly improves efficiency against tumors in xenograft TNBC models. As a result, our combined treatment enhances mature dendritic cells, activates CD4+ T and CD8+ T cells, and promotes the secretion of cytotoxic cytokines. Collectively, our findings reveal that PB Lipo-mediated PDT presents a viable approach for effectively targeting the ER and enhancing ICD, thereby boosting antitumor efficacy in TNBC.
{"title":"Photodynamic Biomimetic Liposomes Targeted to the Endoplasmic Reticulum Enhance Combined Immunotherapy for Triple-Negative Breast Cancer","authors":"Tianyang Li, Haimei Meng, Xinfeng Huang, Qin Yu, Sizhe Sheng, Yufei Jiang, Fei Ren","doi":"10.1021/acsami.5c03687","DOIUrl":"https://doi.org/10.1021/acsami.5c03687","url":null,"abstract":"Cancer immunotherapies, such as immune checkpoint inhibitors, have advanced rapidly and achieved notable success, yet they face significant challenges due to poor response rates and immune-related adverse effects, particularly in cases of triple-negative breast cancer (TNBC). Photodynamic therapy (PDT) can initiate immunogenic cell death (ICD) by inducing endoplasmic reticulum (ER) stress, thereby enhancing the effectiveness of tumor immunotherapy. Herein, we develop potent PDT biomimetic liposomes (PB Lipo) locating the ER to realize a synergistic immuno-photodynamic treatment. The PB Lipo is prepared using the optimal ratios of the phospholipids in the ER membrane. It is then loaded with indocyanine green (ICG), a photosensitizer approved for clinical use. PB Lipo has the unique ability to accumulate in the ER via membrane fusion, leading to severe ER stress when exposed to near-infrared (NIR) laser light, thus intensifying ICD. In combination with the antiprogrammed death-ligand 1 (PD-L1) antibody (αPD-L1), PB Lipo significantly improves efficiency against tumors in xenograft TNBC models. As a result, our combined treatment enhances mature dendritic cells, activates CD4<sup>+</sup> T and CD8<sup>+</sup> T cells, and promotes the secretion of cytotoxic cytokines. Collectively, our findings reveal that PB Lipo-mediated PDT presents a viable approach for effectively targeting the ER and enhancing ICD, thereby boosting antitumor efficacy in TNBC.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"43 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858266","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Circulating tumor cells (CTCs) are crucial for understanding cancer metastasis. Poly(dimethylsiloxane) (PDMS) microfluidic chips utilizing aptamers (APTs) effectively separate CTCs, but the hydrophobicity of PDMS causes issues with nonspecific adsorption and reduces cell viability. Therefore, it is imperative to develop innovative surface modification techniques for PDMS to enhance its biocompatibility and optimize its performance in microfluidic applications. In this study, oligo(ethylene glycol) methacrylate (OEGMA) and adamantane-modified OEGMA were copolymerized onto an initiator-containing PDMS surface. Poly(OEGMA) prevents nonspecific adsorption, and biotin-modified β-cyclodextrin (β-CD) was introduced through host–guest interaction between β-CD and adamantane. By using the biotin–streptavidin interaction, streptavidin and biotin-modified aptamers (TD05 APT and Sgc8 APT) were sequentially immobilized on the copolymer-grafted PDMS substrate. The data indicate that the PDMS substrate functionalized with TD05 APT achieved a capture efficiency of 91% and a selectivity of 30.2 for Ramos cells, while the substrate functionalized with Sgc8 APT achieved a capture efficiency of 93% and a selectivity of 33.3 for CEM cells. Furthermore, treating the APT-functionalized surfaces with sodium dodecyl sulfate released the β-CD component, allowing for the regeneration and switching of the surface biofunctionality by reimmobilizing TD05 APT or Sgc8 APT. Finally, the PDMS microfluidic chips modified using this strategy achieved high capture efficiency (96% for Ramos cells, 93% for CEM cells) and high selectivity (11.4 for Ramos cells, 9.2 for CEM cells). The host–guest chemistry endows the modified PDMS substrate with renewable and switchable biofunctionality, offering insights into the potential applications in the isolation and enrichment of CTCs.
{"title":"Renewable and Switchable Biofunctional Modification of Poly(dimethylsiloxane) Surfaces via Host–Guest Interactions for Enhanced Capture of Circulating Tumor Cells in Microfluidics","authors":"Shengen Gu, Jiao Lei, Shuaihang Guo, Jun Sun, Yu Duan, Aiqing Li, Mengying Zhan, Lisha Pan, Feng Zhou, Xiaoli Liu, Hong Chen","doi":"10.1021/acsami.5c00707","DOIUrl":"https://doi.org/10.1021/acsami.5c00707","url":null,"abstract":"Circulating tumor cells (CTCs) are crucial for understanding cancer metastasis. Poly(dimethylsiloxane) (PDMS) microfluidic chips utilizing aptamers (APTs) effectively separate CTCs, but the hydrophobicity of PDMS causes issues with nonspecific adsorption and reduces cell viability. Therefore, it is imperative to develop innovative surface modification techniques for PDMS to enhance its biocompatibility and optimize its performance in microfluidic applications. In this study, oligo(ethylene glycol) methacrylate (OEGMA) and adamantane-modified OEGMA were copolymerized onto an initiator-containing PDMS surface. Poly(OEGMA) prevents nonspecific adsorption, and biotin-modified β-cyclodextrin (β-CD) was introduced through host–guest interaction between β-CD and adamantane. By using the biotin–streptavidin interaction, streptavidin and biotin-modified aptamers (TD05 APT and Sgc8 APT) were sequentially immobilized on the copolymer-grafted PDMS substrate. The data indicate that the PDMS substrate functionalized with TD05 APT achieved a capture efficiency of 91% and a selectivity of 30.2 for Ramos cells, while the substrate functionalized with Sgc8 APT achieved a capture efficiency of 93% and a selectivity of 33.3 for CEM cells. Furthermore, treating the APT-functionalized surfaces with sodium dodecyl sulfate released the β-CD component, allowing for the regeneration and switching of the surface biofunctionality by reimmobilizing TD05 APT or Sgc8 APT. Finally, the PDMS microfluidic chips modified using this strategy achieved high capture efficiency (96% for Ramos cells, 93% for CEM cells) and high selectivity (11.4 for Ramos cells, 9.2 for CEM cells). The host–guest chemistry endows the modified PDMS substrate with renewable and switchable biofunctionality, offering insights into the potential applications in the isolation and enrichment of CTCs.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"37 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Manuela Cedrún-Morales, Martina Migliavacca, Manuel Ceballos, Marta Perez-Maseda, Giulia Zampini, María Teresa Alameda Felgueiras, Jon Ostolaza-Paraiso, Marisa Juanes, Irene Rincón, David Fairen-Jimenez, Javier Montenegro, Patricia Horcajada, Ester Polo, Beatriz Pelaz, Pablo del Pino
Nanosized microporous metal–organic-frameworks (NMOFs) serve as versatile drug delivery systems capable of navigating complex microenvironments and interacting with cells in specific tissues. The physicochemical properties of NMOFs, such as size, composition, porosity, colloidal stability, and external surface functionalization are essential for their success as efficient carriers. This study introduces a flexible, clickable coating using an amphiphilic polymer derivatized with dibenzo cyclooctyne groups as a universal, postsynthetic functionalization tool. To prove its universality, nanosized MOFs with different structure and composition (UiO-67, NU-1000, PCN-222, and ZIF-8) were produced with high monodispersity and were coated with a clickable, amphiphilic polymer. The resulting polymer-coated NMOFs display exceptional colloidal and structural stability in different biologically relevant media. For comparative purposes, we selected two size-equivalent NMOFs, ZIF-8 and UiO-67, which were functionalized with a library of biologically relevant azide-derivatized (macro)molecules, including poly(ethylene glycol), mannose, and a dynein-binding cell-penetrating peptide, using a bioorthogonal reaction. The choice of ZIF-8 and UiO-67, both 150 nm in size but with distinct coordination and surface chemistries, is pivotal due to their differing acid and base stability characteristics, which may potentially influence their performance in cellular environments. To track their performance in vitro, the NMOFs were loaded with cresyl violet, a common histological stain and lysosomal marker. Cellular internalization of the surface-functionalized NMOFs was markedly governed by their distinct (macro)molecule characteristics. This demonstrates that surface properties critically influence uptake efficiency, while also highlighting the versatility and effectiveness of the proposed coating strategy. In particular, the one functionalized with the dynein-binding peptide demonstrated a markedly higher rate of cellular internalization compared to other NMOFs. In contrast, derivatizations with mannose and poly(ethylene glycol) are associated with a substantial reduction in cellular uptake, suggesting stealth behavior. These results provide a bioorthogonal and versatile alternative for the external surface engineering of NMOFs, aiming to improve targeted drug delivery effectiveness.
{"title":"Clickable Polymer-Based Coatings for Modulating the Interaction of Metal–Organic Framework Nanocrystals with Living Cells","authors":"Manuela Cedrún-Morales, Martina Migliavacca, Manuel Ceballos, Marta Perez-Maseda, Giulia Zampini, María Teresa Alameda Felgueiras, Jon Ostolaza-Paraiso, Marisa Juanes, Irene Rincón, David Fairen-Jimenez, Javier Montenegro, Patricia Horcajada, Ester Polo, Beatriz Pelaz, Pablo del Pino","doi":"10.1021/acsami.5c01695","DOIUrl":"https://doi.org/10.1021/acsami.5c01695","url":null,"abstract":"Nanosized microporous metal–organic-frameworks (NMOFs) serve as versatile drug delivery systems capable of navigating complex microenvironments and interacting with cells in specific tissues. The physicochemical properties of NMOFs, such as size, composition, porosity, colloidal stability, and external surface functionalization are essential for their success as efficient carriers. This study introduces a flexible, clickable coating using an amphiphilic polymer derivatized with dibenzo cyclooctyne groups as a universal, postsynthetic functionalization tool. To prove its universality, nanosized MOFs with different structure and composition (UiO-67, NU-1000, PCN-222, and ZIF-8) were produced with high monodispersity and were coated with a clickable, amphiphilic polymer. The resulting polymer-coated NMOFs display exceptional colloidal and structural stability in different biologically relevant media. For comparative purposes, we selected two size-equivalent NMOFs, ZIF-8 and UiO-67, which were functionalized with a library of biologically relevant azide-derivatized (macro)molecules, including poly(ethylene glycol), mannose, and a dynein-binding cell-penetrating peptide, using a bioorthogonal reaction. The choice of ZIF-8 and UiO-67, both 150 nm in size but with distinct coordination and surface chemistries, is pivotal due to their differing acid and base stability characteristics, which may potentially influence their performance in cellular environments. To track their performance <i>in vitro</i>, the NMOFs were loaded with cresyl violet, a common histological stain and lysosomal marker. Cellular internalization of the surface-functionalized NMOFs was markedly governed by their distinct (macro)molecule characteristics. This demonstrates that surface properties critically influence uptake efficiency, while also highlighting the versatility and effectiveness of the proposed coating strategy. In particular, the one functionalized with the dynein-binding peptide demonstrated a markedly higher rate of cellular internalization compared to other NMOFs. In contrast, derivatizations with mannose and poly(ethylene glycol) are associated with a substantial reduction in cellular uptake, suggesting stealth behavior. These results provide a bioorthogonal and versatile alternative for the external surface engineering of NMOFs, aiming to improve targeted drug delivery effectiveness.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"13 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853149","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The development of post-lithium-ion batteries has sparked significant interest in alkali-metal anodes, particularly sodium (Na), potassium (K), and sodium–potassium (Na–K) alloys. Na–K alloys are promising for partially liquid anodes due to their unique low melting points. A critical factor influencing Na–K-based anode performance is wetting behavior, which governs electrical conductivity, mechanical contact, and long-term stability. At the heart of wetting lies surface tension, a fundamental property of solid–liquid–gas interactions. However, the surface tension of alkali metals and their alloys, particularly Na–K systems, remains poorly understood due to experimental and theoretical challenges. This study bridged these gaps by employing Du Noüy ring tensiometry for the first time in alkali-metal systems to measure the surface tension of Na, K, and Na–K alloys across temperatures from ambient to 180 °C. A key innovation in this work is the development of the push-in Du Noüy method, which provided significantly higher precision and reliability compared to the traditional pull-out technique, without requiring a correction factor. The measured surface tension decreased with increasing temperature for the studied Na–K alloys. For instance, for a eutectic Na–K mixture, the surface tension decreases from 121.7 mN m–1 to 112.2 mN m–1 when increasing the temperature from ambient to 180 °C. Additionally, this study presented the first use of Gibbs free energy minimization to model the surface tension of the Na–K system. The robust method significantly enhanced the predictive accuracy compared to the previous simplified model, reducing deviations from 25% to 2%. Our findings reveal that surface tension increases with sodium mole fraction in the bulk phase, yet the surface monolayer remains potassium-rich, indicating non-ideal surface behavior. This study deepens the understanding of alkali-metal wetting behavior, providing valuable insights for designing optimized interfaces in next-generation semi-solid alkali-metal batteries.
{"title":"High-Precision Surface Tension Measurements of Sodium, Potassium, and Their Alloys via Du Noüy Ring Tensiometry","authors":"Naiyu Qi, Rachana Somaskandan, Gustav Graeber","doi":"10.1021/acsami.5c02183","DOIUrl":"https://doi.org/10.1021/acsami.5c02183","url":null,"abstract":"The development of post-lithium-ion batteries has sparked significant interest in alkali-metal anodes, particularly sodium (Na), potassium (K), and sodium–potassium (Na–K) alloys. Na–K alloys are promising for partially liquid anodes due to their unique low melting points. A critical factor influencing Na–K-based anode performance is wetting behavior, which governs electrical conductivity, mechanical contact, and long-term stability. At the heart of wetting lies surface tension, a fundamental property of solid–liquid–gas interactions. However, the surface tension of alkali metals and their alloys, particularly Na–K systems, remains poorly understood due to experimental and theoretical challenges. This study bridged these gaps by employing Du Noüy ring tensiometry for the first time in alkali-metal systems to measure the surface tension of Na, K, and Na–K alloys across temperatures from ambient to 180 °C. A key innovation in this work is the development of the push-in Du Noüy method, which provided significantly higher precision and reliability compared to the traditional pull-out technique, without requiring a correction factor. The measured surface tension decreased with increasing temperature for the studied Na–K alloys. For instance, for a eutectic Na–K mixture, the surface tension decreases from 121.7 mN m<sup>–1</sup> to 112.2 mN m<sup>–1</sup> when increasing the temperature from ambient to 180 °C. Additionally, this study presented the first use of Gibbs free energy minimization to model the surface tension of the Na–K system. The robust method significantly enhanced the predictive accuracy compared to the previous simplified model, reducing deviations from 25% to 2%. Our findings reveal that surface tension increases with sodium mole fraction in the bulk phase, yet the surface monolayer remains potassium-rich, indicating non-ideal surface behavior. This study deepens the understanding of alkali-metal wetting behavior, providing valuable insights for designing optimized interfaces in next-generation semi-solid alkali-metal batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"4 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143853145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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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