Pub Date : 2024-11-05DOI: 10.1021/acsbiomaterials.4c00777
Payton J Martinez, Jane J Song, Jair I Castillo, John DeSisto, Kang-Ho Song, Adam L Green, Mark Borden
Blood-brain barrier opening (BBBO) using focused ultrasound (FUS) and microbubbles (MBs) has emerged as a promising technique for delivering therapeutics to the brain. However, the influence of various FUS and MB parameters on BBBO and subsequent sterile inflammatory response (SIR) remains unclear. In this study, we investigated the effects of MB size and composition, as well as the number of FUS sonication points, on BBBO and SIR in an immunocompetent mouse model. Using MRI-guided MB + FUS, we targeted the striatum and assessed extravasation of an MRI contrast agent to assess BBBO and RNaseq to assess SIR. Our results revealed distinct effects of these parameters on BBBO and SIR. Specifically, at a matched microbubble volume dose (MVD), MB size did not affect the extent of BBBO, but smaller (1 μm diameter) MBs exhibited a lower classification of SIR than larger (3 or 5 μm diameter) MBs. Lipid-shelled microbubbles exhibited greater BBBO and a more pronounced SIR compared to albumin-shelled microbubbles, likely owing to the latter's poor in vivo stability. As expected, increasing the number of sonication points resulted in greater BBBO and SIR. Furthermore, correlation analysis revealed strong associations between passive cavitation detection measurements of harmonic and inertial MB echoes, BBBO, and the expression of SIR gene sets. Our findings highlight the critical role of MB and FUS parameters in modulating BBBO and subsequent SIR in the brain. These insights inform the development of targeted drug delivery strategies and the mitigation of adverse inflammatory reactions in neurological disorders.
{"title":"Effect of Microbubble Size, Composition, and Multiple Sonication Points on Sterile Inflammatory Response in Focused Ultrasound-Mediated Blood-Brain Barrier Opening.","authors":"Payton J Martinez, Jane J Song, Jair I Castillo, John DeSisto, Kang-Ho Song, Adam L Green, Mark Borden","doi":"10.1021/acsbiomaterials.4c00777","DOIUrl":"10.1021/acsbiomaterials.4c00777","url":null,"abstract":"<p><p>Blood-brain barrier opening (BBBO) using focused ultrasound (FUS) and microbubbles (MBs) has emerged as a promising technique for delivering therapeutics to the brain. However, the influence of various FUS and MB parameters on BBBO and subsequent sterile inflammatory response (SIR) remains unclear. In this study, we investigated the effects of MB size and composition, as well as the number of FUS sonication points, on BBBO and SIR in an immunocompetent mouse model. Using MRI-guided MB + FUS, we targeted the striatum and assessed extravasation of an MRI contrast agent to assess BBBO and RNaseq to assess SIR. Our results revealed distinct effects of these parameters on BBBO and SIR. Specifically, at a matched microbubble volume dose (MVD), MB size did not affect the extent of BBBO, but smaller (1 μm diameter) MBs exhibited a lower classification of SIR than larger (3 or 5 μm diameter) MBs. Lipid-shelled microbubbles exhibited greater BBBO and a more pronounced SIR compared to albumin-shelled microbubbles, likely owing to the latter's poor <i>in vivo</i> stability. As expected, increasing the number of sonication points resulted in greater BBBO and SIR. Furthermore, correlation analysis revealed strong associations between passive cavitation detection measurements of harmonic and inertial MB echoes, BBBO, and the expression of SIR gene sets. Our findings highlight the critical role of MB and FUS parameters in modulating BBBO and subsequent SIR in the brain. These insights inform the development of targeted drug delivery strategies and the mitigation of adverse inflammatory reactions in neurological disorders.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":""},"PeriodicalIF":5.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142574779","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1021/acsami.4c0828710.1021/acsami.4c08287
Daniel Budáč, Vojtěch Miloš, Michal Carda, Martin Paidar*, Karel Bouzek and Jürgen Fuhrmann,
Porous ceramic composites play an important role in several applications. This is due to their unique properties resulting from a combination of various materials. Determination of the composite properties and structure is crucial for their further development and optimization. However, composite analysis often requires complex, expensive, and time-demanding experimental work. Mathematical modeling represents an effective tool to substitute experimental approach. The present study employs a Monte Carlo 3D equivalent electronic circuit network model developed to analyze a highly porous composite on the basis of minimum easily obtainable input parameters. Solid oxide cell electrodes were used as a model example, and this study focuses primarily on materials with a porosity of 55% and higher, characterized by deviation of behavior from those of lower void fraction share. This task is approached by adding to the original Monte Carlo model an additional parameter defining the void phase coalescence phenomenon. The enhanced model accurately simulates electrical conductivity for experimental samples of up to 75% porosity. Using sample composition, single-phase properties, and experimentally determined conductivity, this model allows us to estimate data of the internal structure of the material. This approach offers a rapid and cost-effective method to study material microstructure, providing insights into properties, such as electrical conductivity and heat conductivity. The present research thus contributes to advancing predictive capabilities in understanding and optimizing the performance of composite materials with potential in various technological applications.
{"title":"A Monte Carlo Approach for Simulating Electrical Conductivity in Highly Porous Ceramic Composites: Impact of Internal Structure","authors":"Daniel Budáč, Vojtěch Miloš, Michal Carda, Martin Paidar*, Karel Bouzek and Jürgen Fuhrmann, ","doi":"10.1021/acsami.4c0828710.1021/acsami.4c08287","DOIUrl":"https://doi.org/10.1021/acsami.4c08287https://doi.org/10.1021/acsami.4c08287","url":null,"abstract":"<p >Porous ceramic composites play an important role in several applications. This is due to their unique properties resulting from a combination of various materials. Determination of the composite properties and structure is crucial for their further development and optimization. However, composite analysis often requires complex, expensive, and time-demanding experimental work. Mathematical modeling represents an effective tool to substitute experimental approach. The present study employs a Monte Carlo 3D equivalent electronic circuit network model developed to analyze a highly porous composite on the basis of minimum easily obtainable input parameters. Solid oxide cell electrodes were used as a model example, and this study focuses primarily on materials with a porosity of 55% and higher, characterized by deviation of behavior from those of lower void fraction share. This task is approached by adding to the original Monte Carlo model an additional parameter defining the void phase coalescence phenomenon. The enhanced model accurately simulates electrical conductivity for experimental samples of up to 75% porosity. Using sample composition, single-phase properties, and experimentally determined conductivity, this model allows us to estimate data of the internal structure of the material. This approach offers a rapid and cost-effective method to study material microstructure, providing insights into properties, such as electrical conductivity and heat conductivity. The present research thus contributes to advancing predictive capabilities in understanding and optimizing the performance of composite materials with potential in various technological applications.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"62292–62300 62292–62300"},"PeriodicalIF":8.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsami.4c08287","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608388","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1021/acsami.4c1479310.1021/acsami.4c14793
Liangchao Guo, Junke Wang, Haoran Han, Peng Wang, Yunxiang Lu, Qilong Yuan, Chunyu Du, Shuo Yin, Ye Zhou* and Chao Zhang*,
Gas sensing is pivotal in critical areas such as industrial production and food safety. This study explores the gas classification capabilities of MXene-based gas sensors. Pure V2CTx MXene and an MXene/WO3 nanocomposite were synthesized, and MXene-based gas sensors were integrated into a 2 × 2 rudimentary electronic nose array. The tests on gas sensitivity revealed that the inclusion of WO3 nanoparticles (NPs) boosted the sensor’s response to 10 ppm of NO2 from 2.82 to 3.45 at room temperature. Moreover, the sensor showcased a rapid response/recovery duration of 74.5/149.0 s, excellent environmental stability, and long-term reliable sensing performance. Furthermore, we have improved the method of accurately identifying four toxic gases detected by an MXene-based sensor array using a spiking neural network (SNN) based on the memristive system. Also, the performance of this identification method revealed that the method achieved 95.83% accuracy in the identification of the four gases. Notably, the improved SNN demonstrated approximately 5% higher accuracy than the other gas recognition algorithm. These results highlight the potential of SNN as a powerful tool to accurately and reliably identify toxic gases based on the gas sensor array.
{"title":"MXene/WO3 Sensor Array with Improved SNN Algorithm for Accurate Identification of Toxic Gases","authors":"Liangchao Guo, Junke Wang, Haoran Han, Peng Wang, Yunxiang Lu, Qilong Yuan, Chunyu Du, Shuo Yin, Ye Zhou* and Chao Zhang*, ","doi":"10.1021/acsami.4c1479310.1021/acsami.4c14793","DOIUrl":"https://doi.org/10.1021/acsami.4c14793https://doi.org/10.1021/acsami.4c14793","url":null,"abstract":"<p >Gas sensing is pivotal in critical areas such as industrial production and food safety. This study explores the gas classification capabilities of MXene-based gas sensors. Pure V<sub>2</sub>CT<sub><i>x</i></sub> MXene and an MXene/WO<sub>3</sub> nanocomposite were synthesized, and MXene-based gas sensors were integrated into a 2 × 2 rudimentary electronic nose array. The tests on gas sensitivity revealed that the inclusion of WO<sub>3</sub> nanoparticles (NPs) boosted the sensor’s response to 10 ppm of NO<sub>2</sub> from 2.82 to 3.45 at room temperature. Moreover, the sensor showcased a rapid response/recovery duration of 74.5/149.0 s, excellent environmental stability, and long-term reliable sensing performance. Furthermore, we have improved the method of accurately identifying four toxic gases detected by an MXene-based sensor array using a spiking neural network (SNN) based on the memristive system. Also, the performance of this identification method revealed that the method achieved 95.83% accuracy in the identification of the four gases. Notably, the improved SNN demonstrated approximately 5% higher accuracy than the other gas recognition algorithm. These results highlight the potential of SNN as a powerful tool to accurately and reliably identify toxic gases based on the gas sensor array.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"62421–62428 62421–62428"},"PeriodicalIF":8.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608284","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1021/acsbiomaterials.4c01256
Khezina Rafiq, Iqra Sadia, Muhammad Zeeshan Abid, Muhammad Zaryab Waleed, Abdul Rauf, Ejaz Hussain
Size-dependent optical and electronic properties are unique characteristics of quantum dots (QDs). A significant advantage is the quantum confinement effect that allows their precise tuning to achieve required characteristics and behavior for the targeted applications. Regarding the aforementioned factors, QDs-based sensors have exhibited dramatic potential for the diverse and advanced applications. For example, QDs-based devices have been potentially utilized for bioimaging, drug delivery, cancer therapy, and environmental remediation. In recent years, use of QDs-based electrochemical sensors have been further extended in other areas like gas sensing, metal ion detection, monitoring of organic pollutants, and detection of radioactive isotopes. Objective of this study is to rationalize the QDs-based electrochemical sensors for state-of-the-art applications. This review article comprehensively illustrates the importance of aforementioned devices along with sources from which QDs devices have been formulated and fabricated. Other distinct features of QDs devices are associated with their extremely high active surfaces, inherent ability of reproducibility, sensitivity, and selectivity for the targeted analyte detection. In this review, major categories of QD materials along with justification of their key roles in electrochemical devices have been demonstrated and discussed. All categories have been evaluated with special emphasis on the advantages and drawbacks/challenges associated with QD materials. However, in the interests of readers and researchers, recent improvements also have been included and discussed. On the evaluation, it has been concluded that despite significant challenges, QDs-based electrochemical sensors exhibit excellent performances for state-of-the-art and targeted applications.
{"title":"Scientific Insights into the Quantum Dots (QDs)-Based Electrochemical Sensors for State-of-the-Art Applications.","authors":"Khezina Rafiq, Iqra Sadia, Muhammad Zeeshan Abid, Muhammad Zaryab Waleed, Abdul Rauf, Ejaz Hussain","doi":"10.1021/acsbiomaterials.4c01256","DOIUrl":"10.1021/acsbiomaterials.4c01256","url":null,"abstract":"<p><p>Size-dependent optical and electronic properties are unique characteristics of quantum dots (QDs). A significant advantage is the quantum confinement effect that allows their precise tuning to achieve required characteristics and behavior for the targeted applications. Regarding the aforementioned factors, QDs-based sensors have exhibited dramatic potential for the diverse and advanced applications. For example, QDs-based devices have been potentially utilized for bioimaging, drug delivery, cancer therapy, and environmental remediation. In recent years, use of QDs-based electrochemical sensors have been further extended in other areas like gas sensing, metal ion detection, monitoring of organic pollutants, and detection of radioactive isotopes. Objective of this study is to rationalize the QDs-based electrochemical sensors for state-of-the-art applications. This review article comprehensively illustrates the importance of aforementioned devices along with sources from which QDs devices have been formulated and fabricated. Other distinct features of QDs devices are associated with their extremely high active surfaces, inherent ability of reproducibility, sensitivity, and selectivity for the targeted analyte detection. In this review, major categories of QD materials along with justification of their key roles in electrochemical devices have been demonstrated and discussed. All categories have been evaluated with special emphasis on the advantages and drawbacks/challenges associated with QD materials. However, in the interests of readers and researchers, recent improvements also have been included and discussed. On the evaluation, it has been concluded that despite significant challenges, QDs-based electrochemical sensors exhibit excellent performances for state-of-the-art and targeted applications.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580905","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1021/acsami.4c1346010.1021/acsami.4c13460
Chenxi Liu, Mengze Li, Yifan Wang, Zijie Hou, Jian Chen, Kun Cao, Lihui Liu* and Shufen Chen*,
The development of flexible organic light-emitting didoes (FOLEDs) has spurred the research on flexible transparent electrodes (FTEs). Poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) is one of the most attractive FTEs due to its adjustable conductivity and compatibility with low-cost and large-scale solution processing techniques. Significantly, highly efficient FOLEDs have been achieved with modified PEDOT:PSS FTEs. However, the intrinsic mechanisms that contribute to device degradation of FOLEDs utilizing PEDOT:PSS FTEs have not yet been fully elucidated. In this work, three ionic liquids (ILs) are used to enhance the electrical conductivity and mechanical flexibility of PEDOT:PSS FTEs. Simultaneously, the influence of the electric field induced ion migration from PEDOT:PSS FTEs on the operational stability of FOLEDs is unraveled. We find that the ILs with larger ionic radii and higher steric hindrance are beneficial to suppressing the electrical field induced ion migration and improving the operational stability of FOLEDs. Finally, large-area and high-performance FOLEDs are achieved based on the IL of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide modified PEDOT:PSS FTEs, which demonstrate a high current efficiency of 98.1 cd/A and a longer lifetime of 66.7 min. This finding may promote the practical application of PEDOT:PSS FTEs in flexible optoelectronics.
{"title":"Unravelling the Electrical Field Induced Ion Migration in Flexible OLEDs with PEDOT:PSS Electrodes","authors":"Chenxi Liu, Mengze Li, Yifan Wang, Zijie Hou, Jian Chen, Kun Cao, Lihui Liu* and Shufen Chen*, ","doi":"10.1021/acsami.4c1346010.1021/acsami.4c13460","DOIUrl":"https://doi.org/10.1021/acsami.4c13460https://doi.org/10.1021/acsami.4c13460","url":null,"abstract":"<p >The development of flexible organic light-emitting didoes (FOLEDs) has spurred the research on flexible transparent electrodes (FTEs). Poly(3,4-ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS) is one of the most attractive FTEs due to its adjustable conductivity and compatibility with low-cost and large-scale solution processing techniques. Significantly, highly efficient FOLEDs have been achieved with modified PEDOT:PSS FTEs. However, the intrinsic mechanisms that contribute to device degradation of FOLEDs utilizing PEDOT:PSS FTEs have not yet been fully elucidated. In this work, three ionic liquids (ILs) are used to enhance the electrical conductivity and mechanical flexibility of PEDOT:PSS FTEs. Simultaneously, the influence of the electric field induced ion migration from PEDOT:PSS FTEs on the operational stability of FOLEDs is unraveled. We find that the ILs with larger ionic radii and higher steric hindrance are beneficial to suppressing the electrical field induced ion migration and improving the operational stability of FOLEDs. Finally, large-area and high-performance FOLEDs are achieved based on the IL of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide modified PEDOT:PSS FTEs, which demonstrate a high current efficiency of 98.1 cd/A and a longer lifetime of 66.7 min. This finding may promote the practical application of PEDOT:PSS FTEs in flexible optoelectronics.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"62469–62480 62469–62480"},"PeriodicalIF":8.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608283","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-05DOI: 10.1021/acsami.4c1659210.1021/acsami.4c16592
Haoyuan Tian, Jingpeng Lin, Jiurong Liu, Lei Li*, Bin Li, Sinan Zheng, Wei Liu, Chang Liu*, Zhihui Zeng* and Na Wu*,
The high-efficiency utilization of two-dimensional (2D) graphene layers for developing durable multifunctional electromagnetic wave (EMW) absorbing aerogels is highly demanded yet remains challenging. Here, renewable, low-density, high-strength, and large-aspect-ratio ceramic silicon dioxide (SiO2) nanofibers were efficiently prepared to assist in the preparation of ultralight yet robust, highly elastic, and hydrophobic graphene aerogels using facile, scalable freeze-drying followed by a carbonization approach. The ceramic nanofibers efficiently prevent the agglomeration of graphene and enhance interfacial interactions, significantly promoting mechanical strength. In addition to the high conduction loss capability derived from the interconnected graphene network, high interfacial polarization derived by abundant heterogeneous interfaces is accomplished for the three-dimensional (3D) hybrid aerogels. The hybrid aerogels thus showcase excellent EMW absorption performance, involving a minimum reflection loss of −74.5 dB at 1.8 mm and an effective absorption bandwidth of 5.7 GHz, comparable to those of the best EMW absorbers. Furthermore, the integration of one-dimensional SiO2 and 2D graphene into 3D hybrid aerogels enables remarkable photothermal antibacterial, photothermal oil absorption, and thermal insulation performances. This work thus provides a type of ultralight ceramic/graphene aerogel with a high-efficiency utilization of graphene for accomplishing high-performance multifunctional applications.
{"title":"Ultralight SiO2 Nanofiber-Reinforced Graphene Aerogels for Multifunctional Electromagnetic Wave Absorber","authors":"Haoyuan Tian, Jingpeng Lin, Jiurong Liu, Lei Li*, Bin Li, Sinan Zheng, Wei Liu, Chang Liu*, Zhihui Zeng* and Na Wu*, ","doi":"10.1021/acsami.4c1659210.1021/acsami.4c16592","DOIUrl":"https://doi.org/10.1021/acsami.4c16592https://doi.org/10.1021/acsami.4c16592","url":null,"abstract":"<p >The high-efficiency utilization of two-dimensional (2D) graphene layers for developing durable multifunctional electromagnetic wave (EMW) absorbing aerogels is highly demanded yet remains challenging. Here, renewable, low-density, high-strength, and large-aspect-ratio ceramic silicon dioxide (SiO<sub>2</sub>) nanofibers were efficiently prepared to assist in the preparation of ultralight yet robust, highly elastic, and hydrophobic graphene aerogels using facile, scalable freeze-drying followed by a carbonization approach. The ceramic nanofibers efficiently prevent the agglomeration of graphene and enhance interfacial interactions, significantly promoting mechanical strength. In addition to the high conduction loss capability derived from the interconnected graphene network, high interfacial polarization derived by abundant heterogeneous interfaces is accomplished for the three-dimensional (3D) hybrid aerogels. The hybrid aerogels thus showcase excellent EMW absorption performance, involving a minimum reflection loss of −74.5 dB at 1.8 mm and an effective absorption bandwidth of 5.7 GHz, comparable to those of the best EMW absorbers. Furthermore, the integration of one-dimensional SiO<sub>2</sub> and 2D graphene into 3D hybrid aerogels enables remarkable photothermal antibacterial, photothermal oil absorption, and thermal insulation performances. This work thus provides a type of ultralight ceramic/graphene aerogel with a high-efficiency utilization of graphene for accomplishing high-performance multifunctional applications.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"61484–61494 61484–61494"},"PeriodicalIF":8.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The clinical efficacy of cancer vaccines is closely related to immunoadjuvants that play a crucial role in magnifying and prolonging the immune response. Muramyl dipeptide (MDP), a minimal and conserved peptidoglycan found in almost all bacteria, can trigger robust immune activation by uniquely antagonizing the nucleotide-binding oligomerization domain 2 (NOD2) pathway. However, its effectiveness has been hindered by limited solubility, poor membrane penetration, and rapid clearance from the body. Here, we introduce MDP-presenting polymersomes as artificial nanobacteria (NBA) to boost the antitumor immune response. The NBA, featuring abundant MDP molecules, induces superior stimulation of immune cells including macrophages and bone marrow-derived dendritic cells (BMDCs) compared to free MDP, likely via facilitating immune cell uptake and cooperatively stimulating systemic NOD2 signaling. Importantly, systemic administration of NBA significantly enhances the chemo-immunotherapy of B16-F10 melanoma-bearing mice pretreated with doxorubicin by reversing the immunosuppressive tumor microenvironment. Furthermore, NBA carrying ovalbumin and B16-F10 cell lysates induces robust OVA-IgG antibody production and effectively inhibit tumor growth, respectively. The artificial nanobacteria hold great promise as a potent systemic immunoadjuvant for cancer immunotherapy.
癌症疫苗的临床疗效与免疫佐剂密切相关,免疫佐剂在放大和延长免疫反应方面起着至关重要的作用。氨甲酰基二肽(MDP)是一种几乎存在于所有细菌中的最小且保守的肽聚糖,它能通过独特的方式拮抗核苷酸结合寡聚化结构域 2(NOD2)途径,从而引发强有力的免疫激活。然而,由于其溶解度有限、膜穿透性差以及在体内清除速度快,其有效性一直受到阻碍。在这里,我们引入了以 MDP 为载体的聚合体作为人工纳米细菌(NBA),以增强抗肿瘤免疫反应。与游离 MDP 相比,具有丰富 MDP 分子的 NBA 能诱导巨噬细胞和骨髓树突状细胞(BMDCs)等免疫细胞产生更强的刺激作用,这可能是通过促进免疫细胞摄取和协同刺激全身 NOD2 信号传导实现的。重要的是,通过逆转免疫抑制性肿瘤微环境,全身给药 NBA 能显著增强用多柔比星预处理的 B16-F10 黑色素瘤小鼠的化疗免疫疗法。此外,携带卵清蛋白和 B16-F10 细胞裂解物的 NBA 可分别诱导产生强效的 OVA-IgG 抗体,并有效抑制肿瘤生长。人工纳米细菌有望成为癌症免疫疗法的一种强效全身免疫佐剂。
{"title":"Muramyl Dipeptide-Presenting Polymersomes as Artificial Nanobacteria to Boost Systemic Antitumor Immunity","authors":"Guanhong Cui, Yinping Sun, Shenqiang Wang, Fenghua Meng and Zhiyuan Zhong*, ","doi":"10.1021/acsami.4c1304110.1021/acsami.4c13041","DOIUrl":"https://doi.org/10.1021/acsami.4c13041https://doi.org/10.1021/acsami.4c13041","url":null,"abstract":"<p >The clinical efficacy of cancer vaccines is closely related to immunoadjuvants that play a crucial role in magnifying and prolonging the immune response. Muramyl dipeptide (MDP), a minimal and conserved peptidoglycan found in almost all bacteria, can trigger robust immune activation by uniquely antagonizing the nucleotide-binding oligomerization domain 2 (NOD2) pathway. However, its effectiveness has been hindered by limited solubility, poor membrane penetration, and rapid clearance from the body. Here, we introduce MDP-presenting polymersomes as artificial nanobacteria (NBA) to boost the antitumor immune response. The NBA, featuring abundant MDP molecules, induces superior stimulation of immune cells including macrophages and bone marrow-derived dendritic cells (BMDCs) compared to free MDP, likely via facilitating immune cell uptake and cooperatively stimulating systemic NOD2 signaling. Importantly, systemic administration of NBA significantly enhances the chemo-immunotherapy of B16-F10 melanoma-bearing mice pretreated with doxorubicin by reversing the immunosuppressive tumor microenvironment. Furthermore, NBA carrying ovalbumin and B16-F10 cell lysates induces robust OVA-IgG antibody production and effectively inhibit tumor growth, respectively. The artificial nanobacteria hold great promise as a potent systemic immunoadjuvant for cancer immunotherapy.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"61655–61663 61655–61663"},"PeriodicalIF":8.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608398","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The major ampullate silk of orb-weaving spiders is renowned for its exceptional mechanical properties, including high tensile strength and extensibility. The development of artificial spider silk presents a promising alternative to traditional fibers with significant environmental impacts. This study aims to elucidate the relationship between sequence motifs of natural spider silk and the mechanical properties of artificial spider silk. Using the Spider Silkome Database, we identified motifs correlated with specific physical properties and substituted them into MaSp2-based mini-spidroin BP1. We then measured the mechanical properties of the resulting recombinant artificial spider silk through tensile tests, observed structural properties via birefringence measurement and wide-angle X-ray scattering, and evaluated the water response through boiled water shrinkage tests. Introducing a positively correlated motif increased the tensile strength by 9.3%, while a negatively correlated motif decreased it by 5.1%, confirming the sequence-property relationship. These findings demonstrate that targeted motif substitution can effectively control the physical properties of artificial spider silk, facilitating the development of sustainable biomaterials with tailored mechanical properties for diverse industrial applications.
织眶蛛的主要安培蛛丝以其卓越的机械性能而闻名,包括高拉伸强度和延展性。人工蜘蛛丝的开发有望替代对环境有重大影响的传统纤维。本研究旨在阐明天然蜘蛛丝序列图案与人造蜘蛛丝机械性能之间的关系。利用蜘蛛丝组数据库,我们确定了与特定物理特性相关的基序,并将其替换到基于 MaSp2 的微型蜘蛛丝 BP1 中。然后,我们通过拉伸试验测量了重组人工蜘蛛丝的机械性能,通过双折射测量和广角 X 射线散射观察了结构性能,并通过沸水收缩试验评估了水响应。结果表明,引入一个正相关的基因片段可使拉伸强度提高 9.3%,而引入一个负相关的基因片段可使拉伸强度降低 5.1%,从而证实了序列与性能之间的关系。这些研究结果表明,有针对性的基序置换可以有效控制人工蜘蛛丝的物理性质,从而促进具有定制机械性能的可持续生物材料的开发,并将其应用于不同的工业领域。
{"title":"Correlating Mechanical Properties and Sequence Motifs in Artificial Spider Silk by Targeted Motif Substitution.","authors":"Hiroyuki Nakamura, Yusuke Ito, Ryota Sato, Hongfang Chi, Chikako Sato, Yasuha Watanabe, Kazuharu Arakawa","doi":"10.1021/acsbiomaterials.4c01389","DOIUrl":"https://doi.org/10.1021/acsbiomaterials.4c01389","url":null,"abstract":"<p><p>The major ampullate silk of orb-weaving spiders is renowned for its exceptional mechanical properties, including high tensile strength and extensibility. The development of artificial spider silk presents a promising alternative to traditional fibers with significant environmental impacts. This study aims to elucidate the relationship between sequence motifs of natural spider silk and the mechanical properties of artificial spider silk. Using the Spider Silkome Database, we identified motifs correlated with specific physical properties and substituted them into MaSp2-based mini-spidroin BP1. We then measured the mechanical properties of the resulting recombinant artificial spider silk through tensile tests, observed structural properties via birefringence measurement and wide-angle X-ray scattering, and evaluated the water response through boiled water shrinkage tests. Introducing a positively correlated motif increased the tensile strength by 9.3%, while a negatively correlated motif decreased it by 5.1%, confirming the sequence-property relationship. These findings demonstrate that targeted motif substitution can effectively control the physical properties of artificial spider silk, facilitating the development of sustainable biomaterials with tailored mechanical properties for diverse industrial applications.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":" ","pages":""},"PeriodicalIF":5.4,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142580903","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-04DOI: 10.1021/acsami.4c1197410.1021/acsami.4c11974
Li Xu, Haowei Liu, Jianmei Xu, Wei Zhou, Zhihong Yang, Wei Xu and Jian Sun*,
The exploitation of simply processed p-type semiconductors and photodetectors with promising optoelectrical properties remains challenging yet essential for current and future advanced optoelectronic applications. Transparent p-type CuI and Sn-doped CuI (Cu–Sn–I) films and their self-powered photodetectors have been successfully fabricated by the spraying method. It is found that the incorporation of Sn dopants enhances the optical, electrical, and photoelectric properties of CuI thin films as well as their corresponding self-powered heterojunction photodetectors. This improvement of the optoelectrical properties of the Cu–Sn–I film and its photodetector can be attributed to the adjustment of the acceptor defect level and increased hole concentration resulting from Sn doping. The Cu–Sn–I/n-Si photodetector exhibits a responsivity of 10.7 mA/W, a detectivity of 6.79 × 1011 Jones, and a response time of 77 μs/30 μs (0 V bias). The response time exhibits the fastest rise and decay times compared with the other CuI-based self-powered UV photodetectors in recent years, showcasing promising applications in the realm of transparent electronics moving forward. This study also presents an effective strategy for enhancing the electrical properties of p-type semiconductors and devices through effective doping.
开发具有良好光电特性的简单加工 p 型半导体和光电探测器仍然具有挑战性,但对于当前和未来的先进光电应用至关重要。通过喷涂方法,我们成功地制造出了透明的 p 型 CuI 和 Sn 掺杂 CuI(Cu-Sn-I)薄膜及其自供电光电探测器。研究发现,锡掺杂物的加入增强了 CuI 薄膜及其相应的自供电异质结光电探测器的光学、电学和光电特性。Cu-Sn-I 薄膜及其光电探测器光电特性的改善可归因于掺杂锡后受体缺陷水平的调整和空穴浓度的增加。Cu-Sn-I/n-Si 光电探测器的响应率为 10.7 mA/W,探测率为 6.79 × 1011 Jones,响应时间为 77 μs/30μs(0 V 偏置)。与近年来其他基于 CuI 的自供电紫外光检测器相比,其响应时间具有最快的上升和衰减时间,在透明电子学领域的应用前景十分广阔。这项研究还提出了一种通过有效掺杂来增强 p 型半导体和器件电气性能的有效策略。
{"title":"Spraying-Deposited Transparent p-Type Sn-Doped CuI Film and Its Ultrahigh-Speed Self-Powered Photodetector","authors":"Li Xu, Haowei Liu, Jianmei Xu, Wei Zhou, Zhihong Yang, Wei Xu and Jian Sun*, ","doi":"10.1021/acsami.4c1197410.1021/acsami.4c11974","DOIUrl":"https://doi.org/10.1021/acsami.4c11974https://doi.org/10.1021/acsami.4c11974","url":null,"abstract":"<p >The exploitation of simply processed p-type semiconductors and photodetectors with promising optoelectrical properties remains challenging yet essential for current and future advanced optoelectronic applications. Transparent p-type CuI and Sn-doped CuI (Cu–Sn–I) films and their self-powered photodetectors have been successfully fabricated by the spraying method. It is found that the incorporation of Sn dopants enhances the optical, electrical, and photoelectric properties of CuI thin films as well as their corresponding self-powered heterojunction photodetectors. This improvement of the optoelectrical properties of the Cu–Sn–I film and its photodetector can be attributed to the adjustment of the acceptor defect level and increased hole concentration resulting from Sn doping. The Cu–Sn–I/n-Si photodetector exhibits a responsivity of 10.7 mA/W, a detectivity of 6.79 × 10<sup>11</sup> Jones, and a response time of 77 μs/30 μs (0 V bias). The response time exhibits the fastest rise and decay times compared with the other CuI-based self-powered UV photodetectors in recent years, showcasing promising applications in the realm of transparent electronics moving forward. This study also presents an effective strategy for enhancing the electrical properties of p-type semiconductors and devices through effective doping.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"62326–62334 62326–62334"},"PeriodicalIF":8.3,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-04DOI: 10.1021/acsami.4c1428010.1021/acsami.4c14280
Rocío Sayago-Carro, Irene Barba-Nieto, Natividad Gómez-Cerezo, José A. Rodriguez*, Marcos Fernández-García* and Anna Kubacka*,
The valorization of CO2 is an important challenge within the current panorama, since this molecule is probably the main contributor to climate change. In this study, the synthesis of materials based on a nanostructured batonnet-type indium oxide is carried out. In them, different amounts of Co are introduced, varying between 2 and 8% mol. It is verified that the most active sample in the transformation of carbon dioxide to carbon monoxide contains 6 mol %. of Co. This sample’s activity under dual excitation exceeds the thermal counterpart by more than 30%. After carrying out a complete physical and chemical characterization with the help of X-ray absorption spectroscopy and other techniques, it is shown that catalysts with amounts of cobalt equal to or below 4 mol % contain isolated single-atom species, while those with higher amounts of metal display a Co–Co interaction which triggers the evolution of the samples under reaction conditions. The optimum control of this Co–Co interaction and the nature of the final cobalt-containing species determine dual photothermal catalytic properties. This work establishes a structure–activity relationship to interpret the catalytic behavior of highly dispersed subnanometric cobalt species, and thus an avenue to optimize the photothermal valorization of carbon dioxide.
{"title":"Optimizing Materials to Boost the Valorization of CO2: Tuning Cobalt–Cobalt Interactions on In2O3-Based Photothermal Catalysts","authors":"Rocío Sayago-Carro, Irene Barba-Nieto, Natividad Gómez-Cerezo, José A. Rodriguez*, Marcos Fernández-García* and Anna Kubacka*, ","doi":"10.1021/acsami.4c1428010.1021/acsami.4c14280","DOIUrl":"https://doi.org/10.1021/acsami.4c14280https://doi.org/10.1021/acsami.4c14280","url":null,"abstract":"<p >The valorization of CO<sub>2</sub> is an important challenge within the current panorama, since this molecule is probably the main contributor to climate change. In this study, the synthesis of materials based on a nanostructured batonnet-type indium oxide is carried out. In them, different amounts of Co are introduced, varying between 2 and 8% mol. It is verified that the most active sample in the transformation of carbon dioxide to carbon monoxide contains 6 mol %. of Co. This sample’s activity under dual excitation exceeds the thermal counterpart by more than 30%. After carrying out a complete physical and chemical characterization with the help of X-ray absorption spectroscopy and other techniques, it is shown that catalysts with amounts of cobalt equal to or below 4 mol % contain isolated single-atom species, while those with higher amounts of metal display a Co–Co interaction which triggers the evolution of the samples under reaction conditions. The optimum control of this Co–Co interaction and the nature of the final cobalt-containing species determine dual photothermal catalytic properties. This work establishes a structure–activity relationship to interpret the catalytic behavior of highly dispersed subnanometric cobalt species, and thus an avenue to optimize the photothermal valorization of carbon dioxide.</p>","PeriodicalId":8,"journal":{"name":"ACS Biomaterials Science & Engineering","volume":"16 45","pages":"62131–62141 62131–62141"},"PeriodicalIF":8.3,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608383","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"医学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}