ACS Applied Materials & Interfaces最新文献

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Vertically Phase-Separated PEDOT:PSS Film via Solid–Liquid Interface Doping for Flexible Organic Electrochemical Transistors

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-11 DOI: 10.1021/acsami.5c01311

Jiahuan Qiu, Qiuyue Sheng, Xinyuan Qian, Junxian Yao, Yujie Zhao, Xinyue Zhang, Chengcan Han, Ziliang Wu, Hui Ye, Boyu Peng, Guorong Shan, Qiang Zheng, Hanying Li, Miao Du

Organic electrochemical transistors (OECTs) are seen as some of the most promising devices in organic bioelectronics. Recent interest in OECTs is sparked by the high performance of an organic semiconductor channel material, i.e., poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). The capability of ion penetration and charge transport of the channel determines the performance of the OECTs. However, the uniform structure of the PEDOT:PSS channel always makes it difficult to achieve a well-balanced between the two functions. Here, we report a novel PEDOT:PSS film with a vertical phase separation structure (VPSS-P), where PSS accumulates at the surface, and PEDOT enriches at the bottom of the film. Such a unique structure improves the electrochemical stability and reduces the contact resistance, significantly enhancing OECT performance with high transconductance (70.5 mS), product of mobility (μ) and volumetric capacitance (C*) (μC* ∼ 479 F cm^–1 V^–1 s^–1), and ultralow contact resistance (∼0.79 Ω cm). Flexible OECT devices with VPSS-P show robust performance against deformation. Our findings highlight a new class of high-performance transistors and provide guidelines for designing state-of-the-art channel materials.

{"title":"Vertically Phase-Separated PEDOT:PSS Film via Solid–Liquid Interface Doping for Flexible Organic Electrochemical Transistors","authors":"Jiahuan Qiu, Qiuyue Sheng, Xinyuan Qian, Junxian Yao, Yujie Zhao, Xinyue Zhang, Chengcan Han, Ziliang Wu, Hui Ye, Boyu Peng, Guorong Shan, Qiang Zheng, Hanying Li, Miao Du","doi":"10.1021/acsami.5c01311","DOIUrl":"https://doi.org/10.1021/acsami.5c01311","url":null,"abstract":"Organic electrochemical transistors (OECTs) are seen as some of the most promising devices in organic bioelectronics. Recent interest in OECTs is sparked by the high performance of an organic semiconductor channel material, i.e., poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). The capability of ion penetration and charge transport of the channel determines the performance of the OECTs. However, the uniform structure of the PEDOT:PSS channel always makes it difficult to achieve a well-balanced between the two functions. Here, we report a novel PEDOT:PSS film with a vertical phase separation structure (VPSS-P), where PSS accumulates at the surface, and PEDOT enriches at the bottom of the film. Such a unique structure improves the electrochemical stability and reduces the contact resistance, significantly enhancing OECT performance with high transconductance (70.5 mS), product of mobility (μ) and volumetric capacitance (C*) (μC* ∼ 479 F cm–1 V–1 s–1), and ultralow contact resistance (∼0.79 Ω cm). Flexible OECT devices with VPSS-P show robust performance against deformation. Our findings highlight a new class of high-performance transistors and provide guidelines for designing state-of-the-art channel materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"21 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590138","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}

引用次数: 0

Understanding the Structural Dynamics of 2D/3D Perovskite Interfaces

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-11 DOI: 10.1021/acsami.5c02680

Alan B. Kaplan, Quinn C. Burlingame, Marko R. Ivancevic, Yueh-Lin Loo

The use of 2D perovskite capping layers to passivate the surface defects of 3D perovskite active layers has become ubiquitous in high performance lead halide perovskite solar cells. However, these 2D/3D interfaces can be highly dynamic, with the structure evolving to form various mixed dimensional phases when exposed to thermal stress or illumination. Changes in the photoluminescence spectrum of formamidinium lead iodide (FAPbI₃) films capped with alkylammonium-based 2D perovskites as they age at 100 °C or under simulated 1 sun illumination indicate that the 2D perovskite transforms to progressively larger inorganic layer thicknesses (denoted by layer number n), eventually approaching a steady-state condition where only the 3D perovskite (n = ∞) is detectable. We find that this transformation slows by a factor of ∼2 when the length of the alkyl chain in the organic monoammonium ligand is increased from butylammonium to dodecylammonium. Furthermore, replacing dodecylammonium with its diammonium ligand counterpart, 1,12-dodecanediammonium, slows the structural transformation by 10-fold. These results point to the use of diammonium ligands as a possible pathway to form stable 2D/3D interfaces.

{"title":"Understanding the Structural Dynamics of 2D/3D Perovskite Interfaces","authors":"Alan B. Kaplan, Quinn C. Burlingame, Marko R. Ivancevic, Yueh-Lin Loo","doi":"10.1021/acsami.5c02680","DOIUrl":"https://doi.org/10.1021/acsami.5c02680","url":null,"abstract":"The use of 2D perovskite capping layers to passivate the surface defects of 3D perovskite active layers has become ubiquitous in high performance lead halide perovskite solar cells. However, these 2D/3D interfaces can be highly dynamic, with the structure evolving to form various mixed dimensional phases when exposed to thermal stress or illumination. Changes in the photoluminescence spectrum of formamidinium lead iodide (FAPbI3) films capped with alkylammonium-based 2D perovskites as they age at 100 °C or under simulated 1 sun illumination indicate that the 2D perovskite transforms to progressively larger inorganic layer thicknesses (denoted by layer number n), eventually approaching a steady-state condition where only the 3D perovskite (n = ∞) is detectable. We find that this transformation slows by a factor of ∼2 when the length of the alkyl chain in the organic monoammonium ligand is increased from butylammonium to dodecylammonium. Furthermore, replacing dodecylammonium with its diammonium ligand counterpart, 1,12-dodecanediammonium, slows the structural transformation by 10-fold. These results point to the use of diammonium ligands as a possible pathway to form stable 2D/3D interfaces.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"65 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590139","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}

引用次数: 0

Combination of Dynamic and Permanent Cross-Linking: A Pathway to Enhance Elasticity and Recyclability

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-11 DOI: 10.1021/acsami.5c02509

Xinyu Li, Jing Bai, Bing Yu, Fei Chen, Ming Tian

Thermosetting materials exhibit advantages such as dimensional stability and elasticity but lack reprocessability due to their permanently cross-linked internal structure. Introducing a reversible cross-linked network endows materials with reprocessability but often compromises resilience and mechanical properties. Hence, it is still a significant challenge to develop recyclable elastomers with high elasticity as traditional thermosetting materials and remolding ability as traditional thermoplastic materials. Based on this, this work incorporates both reversible and irreversible cross-linked networks into a polyurethane system, constructing synergistic networks with distinct properties to achieve high elasticity and reprocessability simultaneously. In addition, by adjusting the proportion of the synergistic networks, the relationship between elasticity and reprocessability in different materials was investigated, revealing the synergistic effect between the dynamic network and the chemical cross-linked network. This work provides theoretical support for the design of elastomer materials that combine the high resilience of thermoset materials with the remolding ability of thermoplastic materials.

{"title":"Combination of Dynamic and Permanent Cross-Linking: A Pathway to Enhance Elasticity and Recyclability","authors":"Xinyu Li, Jing Bai, Bing Yu, Fei Chen, Ming Tian","doi":"10.1021/acsami.5c02509","DOIUrl":"https://doi.org/10.1021/acsami.5c02509","url":null,"abstract":"Thermosetting materials exhibit advantages such as dimensional stability and elasticity but lack reprocessability due to their permanently cross-linked internal structure. Introducing a reversible cross-linked network endows materials with reprocessability but often compromises resilience and mechanical properties. Hence, it is still a significant challenge to develop recyclable elastomers with high elasticity as traditional thermosetting materials and remolding ability as traditional thermoplastic materials. Based on this, this work incorporates both reversible and irreversible cross-linked networks into a polyurethane system, constructing synergistic networks with distinct properties to achieve high elasticity and reprocessability simultaneously. In addition, by adjusting the proportion of the synergistic networks, the relationship between elasticity and reprocessability in different materials was investigated, revealing the synergistic effect between the dynamic network and the chemical cross-linked network. This work provides theoretical support for the design of elastomer materials that combine the high resilience of thermoset materials with the remolding ability of thermoplastic materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"68 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590259","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}

引用次数: 0

Quantum Wells in Magnesium-Manganese Bimetallic Antiperovskites for High Luminescence.

IF 8.3 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.4c18047

Yangyang Cai, Siyu Yan, Yue-Jian Lin, Tingting Lin, Longzhen Qiu, Xiaoyong Pan, Weizhi Wang

Perovskite has attracted extensive attention in the realm of photovoltaic and light-emitting diodes (LEDs) on account of its outstanding photoelectric properties. Perovskite-type quantum wells (QW) have been developed for high-efficiency perovskite-type LEDs. However, there are few reports on the in situ quantum well structure formed by a bimetallic antiperovskite and its properties. In this work, we report a double/bimetallic antiperovskite composed of magnesium and manganese. It is an in situ homogeneous junction composed of a p-type manganese well layer and an n-type magnesium barrier layer, which promotes the recombination of carriers and increases the luminous efficiency. The in situ quantum wells enable the green antiperovskite LED to have a maximum external quantum efficiency reaching 20.2% and a maximum luminance as high as 19000 cd m^-2. These research results provide the chance to produce high-performance LEDs based on an in situ quantum well structure. Meanwhile, the strategy developed in this work is helpful for the design of other highly luminescent lead-free materials.

{"title":"Quantum Wells in Magnesium-Manganese Bimetallic Antiperovskites for High Luminescence.","authors":"Yangyang Cai, Siyu Yan, Yue-Jian Lin, Tingting Lin, Longzhen Qiu, Xiaoyong Pan, Weizhi Wang","doi":"10.1021/acsami.4c18047","DOIUrl":"https://doi.org/10.1021/acsami.4c18047","url":null,"abstract":"Perovskite has attracted extensive attention in the realm of photovoltaic and light-emitting diodes (LEDs) on account of its outstanding photoelectric properties. Perovskite-type quantum wells (QW) have been developed for high-efficiency perovskite-type LEDs. However, there are few reports on the in situ quantum well structure formed by a bimetallic antiperovskite and its properties. In this work, we report a double/bimetallic antiperovskite composed of magnesium and manganese. It is an in situ homogeneous junction composed of a p-type manganese well layer and an n-type magnesium barrier layer, which promotes the recombination of carriers and increases the luminous efficiency. The in situ quantum wells enable the green antiperovskite LED to have a maximum external quantum efficiency reaching 20.2% and a maximum luminance as high as 19000 cd m-2. These research results provide the chance to produce high-performance LEDs based on an in situ quantum well structure. Meanwhile, the strategy developed in this work is helpful for the design of other highly luminescent lead-free materials.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143583746","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}

引用次数: 0

Robust Tertiary Amine Suspended HCIPs for Catalytic Conversion of CO₂ into Cyclic Carbonates under Mild Conditions.

IF 8.3 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.5c01381

Yanbin Zeng, Rui Wang, Zijun Luo, Zhenzhu Tang, Jiaxiang Qiu, Chao Zou, Chunshan Li, Guanqun Xie, Xiaoxia Wang

A series of tertiary amine suspended hyper-cross-linked ionic polymers (HCIPs), characterized by a rich mesoporous structure, high ionic liquid (IL) density, and good CO₂ adsorption capability, were readily prepared via a postsynthetic method. The self-polymerization of 1,3,5-tris(bromomethyl) benzene (TBB) or its copolymerization with 4,4'-bis(bromomethyl) biphenyl (BBP) in varying ratios, followed by grafting with N,N,N',N'-tetramethyl-1,3-propanediamine (TMPDA), yielded the target TMPDA-HCIPs. These HCIPs constitute one of the limited categories of heterogeneous water-tolerant catalyst types ever developed for the cycloaddition reaction between CO₂ and epoxides. Specifically, chloropropylene carbonate (CPC) was produced in 99.9% yield with 99% selectivity at 80 °C and 1 bar of CO₂ pressure in the presence of 22 mol % water relative to the epoxide substrate. Furthermore, when simulated flue gas served as the CO₂ source, the same ratio of water enhanced the CPC yield from 81.9% to 91.5% under 1 MPa pressure, with the selectivity only slightly decreasing from 99% to 94.1%. Additionally, the catalyst could be easily recovered and maintained a high catalytic performance after six cycles. In conclusion, this study presents a robust water-tolerant heterogeneous catalyst for the efficient synthesis of cyclic carbonates from CO₂ under mild conditions, potentially reducing the high costs of purifying real flue gas that contains water vapor.

{"title":"Robust Tertiary Amine Suspended HCIPs for Catalytic Conversion of CO2 into Cyclic Carbonates under Mild Conditions.","authors":"Yanbin Zeng, Rui Wang, Zijun Luo, Zhenzhu Tang, Jiaxiang Qiu, Chao Zou, Chunshan Li, Guanqun Xie, Xiaoxia Wang","doi":"10.1021/acsami.5c01381","DOIUrl":"https://doi.org/10.1021/acsami.5c01381","url":null,"abstract":"A series of tertiary amine suspended hyper-cross-linked ionic polymers (HCIPs), characterized by a rich mesoporous structure, high ionic liquid (IL) density, and good CO2 adsorption capability, were readily prepared via a postsynthetic method. The self-polymerization of 1,3,5-tris(bromomethyl) benzene (TBB) or its copolymerization with 4,4'-bis(bromomethyl) biphenyl (BBP) in varying ratios, followed by grafting with N,N,N',N'-tetramethyl-1,3-propanediamine (TMPDA), yielded the target TMPDA-HCIPs. These HCIPs constitute one of the limited categories of heterogeneous water-tolerant catalyst types ever developed for the cycloaddition reaction between CO2 and epoxides. Specifically, chloropropylene carbonate (CPC) was produced in 99.9% yield with 99% selectivity at 80 °C and 1 bar of CO2 pressure in the presence of 22 mol % water relative to the epoxide substrate. Furthermore, when simulated flue gas served as the CO2 source, the same ratio of water enhanced the CPC yield from 81.9% to 91.5% under 1 MPa pressure, with the selectivity only slightly decreasing from 99% to 94.1%. Additionally, the catalyst could be easily recovered and maintained a high catalytic performance after six cycles. In conclusion, this study presents a robust water-tolerant heterogeneous catalyst for the efficient synthesis of cyclic carbonates from CO2 under mild conditions, potentially reducing the high costs of purifying real flue gas that contains water vapor.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.3,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143583751","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}

引用次数: 0

Solution-Processed Metal-Oxide Nanoparticles to Prevent The Sputtering Damage in Perovskite/Silicon Tandem Solar Cells

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.5c00090

Erica Magliano, Francesco Di Giacomo, Harshavardhan Reddy Sathy, Shirin M. Pourmotlagh, Gemma Giliberti, David Becerril Rodriguez, Giuseppe Ammirati, Paolo Mariani, Francesca Zarotti, Fabio Matteocci, Marco Luce, Iurie Usatii, Eugenia Bobeico, Marco Della Noce, Antonio Cricenti, Federica Cappelluti, Lucia V. Mercaldo, Paola Delli Veneri, Aldo Di Carlo

Semitransparent perovskite solar cells (ST-PSCs) for tandem applications typically use a buffer layer deposited via atomic layer deposition (ALD) to protect the cell stack from the damage induced by the sputtering of the transparent electrode. Here, we present a simple yet effective solution-processed buffer layer based on metal-oxide nanoparticles to mitigate sputter-induced damage. We exploit this strategy in a monolithic tandem integrating the optimized ST-PSC on a polished front-side/unpolished rear-side p-type silicon heterojunction (SHJ) solar cell. The intrinsic roughness on the backside significantly boosts the absorption, thus suppressing the need for a dedicated texturization step and leading to a final maximum efficiency of 25.3%. Our findings highlight the potential of solution-processed buffer layers as a practical and scalable solution to mitigate the sputtering damage, as well as the potential of silicon wafers with an unpolished rear surface for enhanced photocurrent.

{"title":"Solution-Processed Metal-Oxide Nanoparticles to Prevent The Sputtering Damage in Perovskite/Silicon Tandem Solar Cells","authors":"Erica Magliano, Francesco Di Giacomo, Harshavardhan Reddy Sathy, Shirin M. Pourmotlagh, Gemma Giliberti, David Becerril Rodriguez, Giuseppe Ammirati, Paolo Mariani, Francesca Zarotti, Fabio Matteocci, Marco Luce, Iurie Usatii, Eugenia Bobeico, Marco Della Noce, Antonio Cricenti, Federica Cappelluti, Lucia V. Mercaldo, Paola Delli Veneri, Aldo Di Carlo","doi":"10.1021/acsami.5c00090","DOIUrl":"https://doi.org/10.1021/acsami.5c00090","url":null,"abstract":"Semitransparent perovskite solar cells (ST-PSCs) for tandem applications typically use a buffer layer deposited via atomic layer deposition (ALD) to protect the cell stack from the damage induced by the sputtering of the transparent electrode. Here, we present a simple yet effective solution-processed buffer layer based on metal-oxide nanoparticles to mitigate sputter-induced damage. We exploit this strategy in a monolithic tandem integrating the optimized ST-PSC on a polished front-side/unpolished rear-side p-type silicon heterojunction (SHJ) solar cell. The intrinsic roughness on the backside significantly boosts the absorption, thus suppressing the need for a dedicated texturization step and leading to a final maximum efficiency of 25.3%. Our findings highlight the potential of solution-processed buffer layers as a practical and scalable solution to mitigate the sputtering damage, as well as the potential of silicon wafers with an unpolished rear surface for enhanced photocurrent.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"31 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590248","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}

引用次数: 0

Quality by Design-Guided Development of Hydrogel-Forming Microneedles for Transdermal Delivery of Enfuvirtide

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.5c00499

Huanhuan Li, Lalitkumar K. Vora, Qonita Anjani, Abraham M. Abraham, Yilin Cong, Natalia Moreno-Castellanos, Ester Ballana, Eva Riveira Muñoz, Maria Nevot, Ryan F. Donnelly

Enfuvirtide, the inaugural biomimetic fusion inhibitor of HIV-1, has exhibited remarkable antiviral efficacy when administered in conjunction with an optimized antiretroviral regimen. Nonetheless, the high incidence (98%) of injection site reactions associated with twice-daily subcutaneous administration severely compromises patient adherence and long-term therapeutic outcomes. This study proposes hydrogel-forming microneedles (MNs) as a minimally invasive and painless modality for the transdermal delivery of this therapeutic peptide. Leveraging a rigorous Quality by Design (QbD) framework, this investigation systematically delineated the critical material attributes (CMAs) and critical process parameters (CPPs) of the hydrogel formulation, mapping their influence on the critical quality attributes (CQAs) of MNs to achieve a meticulously defined quality-target product profile (QTPP). The optimized MN formulation, achieving a desirability index of 0.871, was validated through comprehensive design space and feasibility analyses, demonstrating superior predictive accuracy and mechanical integrity. Ex vivo permeation studies elucidated the sustained and controlled release kinetics of enfuvirtide via MNs fabricated from the optimized formulation, attaining a maximum permeation of 36.26% using 11 × 11 molds, compared to 28.45% permeation observed with the control system over 24 h. Furthermore, the system’s favorable swelling kinetics and enhanced viscoelastic properties significantly augmented its delivery performance relative to conventional approaches. This study not only establishes hydrogel-forming MNs as an innovative and efficacious delivery platform for enfuvirtide but also presents a robust, systematic methodology for MN development, offering transformative potential for broader pharmaceutical applications and therapeutic paradigms.

{"title":"Quality by Design-Guided Development of Hydrogel-Forming Microneedles for Transdermal Delivery of Enfuvirtide","authors":"Huanhuan Li, Lalitkumar K. Vora, Qonita Anjani, Abraham M. Abraham, Yilin Cong, Natalia Moreno-Castellanos, Ester Ballana, Eva Riveira Muñoz, Maria Nevot, Ryan F. Donnelly","doi":"10.1021/acsami.5c00499","DOIUrl":"https://doi.org/10.1021/acsami.5c00499","url":null,"abstract":"Enfuvirtide, the inaugural biomimetic fusion inhibitor of HIV-1, has exhibited remarkable antiviral efficacy when administered in conjunction with an optimized antiretroviral regimen. Nonetheless, the high incidence (98%) of injection site reactions associated with twice-daily subcutaneous administration severely compromises patient adherence and long-term therapeutic outcomes. This study proposes hydrogel-forming microneedles (MNs) as a minimally invasive and painless modality for the transdermal delivery of this therapeutic peptide. Leveraging a rigorous Quality by Design (QbD) framework, this investigation systematically delineated the critical material attributes (CMAs) and critical process parameters (CPPs) of the hydrogel formulation, mapping their influence on the critical quality attributes (CQAs) of MNs to achieve a meticulously defined quality-target product profile (QTPP). The optimized MN formulation, achieving a desirability index of 0.871, was validated through comprehensive design space and feasibility analyses, demonstrating superior predictive accuracy and mechanical integrity. Ex vivo permeation studies elucidated the sustained and controlled release kinetics of enfuvirtide via MNs fabricated from the optimized formulation, attaining a maximum permeation of 36.26% using 11 × 11 molds, compared to 28.45% permeation observed with the control system over 24 h. Furthermore, the system’s favorable swelling kinetics and enhanced viscoelastic properties significantly augmented its delivery performance relative to conventional approaches. This study not only establishes hydrogel-forming MNs as an innovative and efficacious delivery platform for enfuvirtide but also presents a robust, systematic methodology for MN development, offering transformative potential for broader pharmaceutical applications and therapeutic paradigms.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"192 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590270","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}

引用次数: 0

An Antibacterial, Antioxidant Adherent Sponge Constructed for Control of Arterial Bleeding Via Gallic Acid-Mediated Robust Assembly of Fibrous Clay in Collagen

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.4c19209

Xin Guo, Xingling Zeng, Yeqing He, Xiaoxia Zhang, Wenli Shi, Ruimin Ran, Guoying Li

Acute hemorrhage death on battlefields, during clinical surgeries, and in major accidents is a widespread worldwide problem. Clay-based hemostatic materials have received considerable attention for their low cost and reliable clotting activity, especially in cases of severe bleeding, such as QuikClot, which is a kaolin-based hemostatic gauze that is preferred for battlefield resuscitation. However, the easy detachment of clay particles and the associated risk of thrombosis have seriously hindered the development of clay-based hemostatic materials. Here, inexpensive palygorskite (Pal) nanoclay was integrated into the collagen (COL) matrix by loading Ca²⁺ in the clay and further using gallic acid (GA) to mediate the robust assembly of clay on the COL matrix. This targeted interfacial design is a simple and gentle method that effectively improves the dispersion of the Pal particles and reduces the risk of shedding. Unlike QuikClot where the aqueous solution was significantly turbid after 2 min of ultrasonic washing, the aqueous solution of the composite sponge (Ca-Pal-GA-COL) remained clear and was accompanied by 82.71% of the mass residue after 10 min of ultrasonic washing. The composite sponge also exhibited excellent antibacterial (87.93% inhibition rate of Escherichia coli), antioxidant, and tissue adhesion properties. Importantly, the Ca-Pal-GA-COL sponge exhibited less blood loss (632 mg) and a shorter hemostasis time (151 s) in a rat femoral artery hemorrhage model than the medical gauze (3850 mg and 299 s), pure COL sponge (1627 mg and 201 s), and Pal-COL sponge (1494 mg and 193 s) in a co-mingled mode, which are comparable to those of QuikClot (559 mg and 142 s). Furthermore, certain tissue adhesion properties render the Ca-Pal-GA-COL sponge more suitable than QuikClot for severe femoral artery active bleeding scenarios. Cellular experiments confirmed that the composite dressing has a certain biosafety.

{"title":"An Antibacterial, Antioxidant Adherent Sponge Constructed for Control of Arterial Bleeding Via Gallic Acid-Mediated Robust Assembly of Fibrous Clay in Collagen","authors":"Xin Guo, Xingling Zeng, Yeqing He, Xiaoxia Zhang, Wenli Shi, Ruimin Ran, Guoying Li","doi":"10.1021/acsami.4c19209","DOIUrl":"https://doi.org/10.1021/acsami.4c19209","url":null,"abstract":"Acute hemorrhage death on battlefields, during clinical surgeries, and in major accidents is a widespread worldwide problem. Clay-based hemostatic materials have received considerable attention for their low cost and reliable clotting activity, especially in cases of severe bleeding, such as QuikClot, which is a kaolin-based hemostatic gauze that is preferred for battlefield resuscitation. However, the easy detachment of clay particles and the associated risk of thrombosis have seriously hindered the development of clay-based hemostatic materials. Here, inexpensive palygorskite (Pal) nanoclay was integrated into the collagen (COL) matrix by loading Ca2+ in the clay and further using gallic acid (GA) to mediate the robust assembly of clay on the COL matrix. This targeted interfacial design is a simple and gentle method that effectively improves the dispersion of the Pal particles and reduces the risk of shedding. Unlike QuikClot where the aqueous solution was significantly turbid after 2 min of ultrasonic washing, the aqueous solution of the composite sponge (Ca-Pal-GA-COL) remained clear and was accompanied by 82.71% of the mass residue after 10 min of ultrasonic washing. The composite sponge also exhibited excellent antibacterial (87.93% inhibition rate of Escherichia coli), antioxidant, and tissue adhesion properties. Importantly, the Ca-Pal-GA-COL sponge exhibited less blood loss (632 mg) and a shorter hemostasis time (151 s) in a rat femoral artery hemorrhage model than the medical gauze (3850 mg and 299 s), pure COL sponge (1627 mg and 201 s), and Pal-COL sponge (1494 mg and 193 s) in a co-mingled mode, which are comparable to those of QuikClot (559 mg and 142 s). Furthermore, certain tissue adhesion properties render the Ca-Pal-GA-COL sponge more suitable than QuikClot for severe femoral artery active bleeding scenarios. Cellular experiments confirmed that the composite dressing has a certain biosafety.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"39 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590260","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}

引用次数: 0

Intranasal Delivery of Hydrophobic AC5216 Loaded Nanoemulsion into Brain To Alleviate Chronic Unpredictable Stress-Induced Depressive-like Behaviors

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.4c19377

Yuan Zhang, Yuqi Wang, Huijuan Wang, Liang Bian, Feng Gao, Honghong Yao, Jinbing Xie

Major depressive disorder (MDD) represents a widespread mental health condition. Efficiently moving therapeutic substances across the blood–brain barrier (BBB) remains a critical obstacle in addressing depressive disorders. AC5216, identified as a translocator protein (TSPO) ligand and considered a potential treatment for major depressive disorder (MDD), faces limitations due to its subpar druggability and oral bioavailability. In this context, an amphiphilic polymer composed of polyethylene glycol, poly-l-lysine, and poly(lactic-co-glycolic acid) (PEG-PLL-PLGA) has been utilized to encapsulate the hydrophobic compound AC5216. This results in the formation of cell-penetrating peptide-modified nanoemulsions (termed CPP-PPP-AC5216), designed to deliver AC5216 directly into the central nervous system via intranasal administration for MDD therapy. Research on animal models has shown that CPP-PPP-AC5216 effectively transports AC5216 to the brain, significantly mitigating chronic unpredictable stress (CUS)-induced depressive behaviors with a dosage as low as 0.03 mg/kg when administered intranasally. Furthermore, it was observed that CPP-PPP-AC5216 substantially reduces microglial activation, prevents BBB leakage, and ameliorates astrocyte dysfunction caused by CUS. The findings suggest a promising potential for using this nanoemulsion approach to deliver hydrophobic compounds through the nasal route for the treatment of MDD.

{"title":"Intranasal Delivery of Hydrophobic AC5216 Loaded Nanoemulsion into Brain To Alleviate Chronic Unpredictable Stress-Induced Depressive-like Behaviors","authors":"Yuan Zhang, Yuqi Wang, Huijuan Wang, Liang Bian, Feng Gao, Honghong Yao, Jinbing Xie","doi":"10.1021/acsami.4c19377","DOIUrl":"https://doi.org/10.1021/acsami.4c19377","url":null,"abstract":"Major depressive disorder (MDD) represents a widespread mental health condition. Efficiently moving therapeutic substances across the blood–brain barrier (BBB) remains a critical obstacle in addressing depressive disorders. AC5216, identified as a translocator protein (TSPO) ligand and considered a potential treatment for major depressive disorder (MDD), faces limitations due to its subpar druggability and oral bioavailability. In this context, an amphiphilic polymer composed of polyethylene glycol, poly-l-lysine, and poly(lactic-co-glycolic acid) (PEG-PLL-PLGA) has been utilized to encapsulate the hydrophobic compound AC5216. This results in the formation of cell-penetrating peptide-modified nanoemulsions (termed CPP-PPP-AC5216), designed to deliver AC5216 directly into the central nervous system via intranasal administration for MDD therapy. Research on animal models has shown that CPP-PPP-AC5216 effectively transports AC5216 to the brain, significantly mitigating chronic unpredictable stress (CUS)-induced depressive behaviors with a dosage as low as 0.03 mg/kg when administered intranasally. Furthermore, it was observed that CPP-PPP-AC5216 substantially reduces microglial activation, prevents BBB leakage, and ameliorates astrocyte dysfunction caused by CUS. The findings suggest a promising potential for using this nanoemulsion approach to deliver hydrophobic compounds through the nasal route for the treatment of MDD.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"91 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590262","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}

引用次数: 0

Earth-Abundant W18O49 Coupled with Minimal Pt for Enhanced Hydrogen Evolution under Dark and Visible Light Conditions

IF 9.5 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces

Pub Date : 2025-03-10 DOI: 10.1021/acsami.4c22952

Hugo L. S. Santos, Md Mofakkharulhashan, Shiqi Wang, Eric V. Formo, Mykhailo Chundak, Mikko Ritala, Wenyi Huo, Pedro H. C. Camargo

The development of cost-effective and efficient electrocatalysts for the hydrogen evolution reaction (HER) is critical to advancing green hydrogen production technologies. Here, we present a plasmonic tungsten oxide (W₁₈O₄₉) material integrated with ultralow platinum (Pt) loadings (0.4, 0.8, and 1.6 wt %) that delivers high HER performances under both dark and visible light conditions. The 0.4 wt % Pt–W₁₈O₄₉ catalyst exhibits remarkable mass activity, outperforming commercial Pt/C by factors of 15 and 30 under dark and 740 nm LED illumination, respectively. Density functional theory (DFT) calculations reveal that the synergy between Pt and plasmonically active W₁₈O₄₉ optimizes charge transfer and hydrogen adsorption, resulting in lowered energy barriers for HER kinetics. Furthermore, plasmonic excitation of W₁₈O₄₉ enhances catalytic activity by facilitating electron transfer. This work introduces a scalable, cost-effective strategy for combining earth-abundant plasmonic materials with minimal Pt usage, providing a pathway toward high-efficiency HER catalysts. These findings highlight the potential of plasmonic-catalyst integration in green hydrogen technologies.

{"title":"Earth-Abundant W18O49 Coupled with Minimal Pt for Enhanced Hydrogen Evolution under Dark and Visible Light Conditions","authors":"Hugo L. S. Santos, Md Mofakkharulhashan, Shiqi Wang, Eric V. Formo, Mykhailo Chundak, Mikko Ritala, Wenyi Huo, Pedro H. C. Camargo","doi":"10.1021/acsami.4c22952","DOIUrl":"https://doi.org/10.1021/acsami.4c22952","url":null,"abstract":"The development of cost-effective and efficient electrocatalysts for the hydrogen evolution reaction (HER) is critical to advancing green hydrogen production technologies. Here, we present a plasmonic tungsten oxide (W18O49) material integrated with ultralow platinum (Pt) loadings (0.4, 0.8, and 1.6 wt %) that delivers high HER performances under both dark and visible light conditions. The 0.4 wt % Pt–W18O49 catalyst exhibits remarkable mass activity, outperforming commercial Pt/C by factors of 15 and 30 under dark and 740 nm LED illumination, respectively. Density functional theory (DFT) calculations reveal that the synergy between Pt and plasmonically active W18O49 optimizes charge transfer and hydrogen adsorption, resulting in lowered energy barriers for HER kinetics. Furthermore, plasmonic excitation of W18O49 enhances catalytic activity by facilitating electron transfer. This work introduces a scalable, cost-effective strategy for combining earth-abundant plasmonic materials with minimal Pt usage, providing a pathway toward high-efficiency HER catalysts. These findings highlight the potential of plasmonic-catalyst integration in green hydrogen technologies.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"31 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143590267","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}

引用次数: 0

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