Due to the complex and varied toxicological characteristics exhibited by different antibiotics, which present significant risks to both the environment and human health, there is an urgent requirement for highly efficient sensors capable of detecting antibiotics. The present study introduces a straightforward yet efficient colorimetric sensor array comprising surface-tailored nanoparticles, analyzed using different techniques including dynamic light scattering, zeta potential, Fourier transformation infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy, atomic force microscopy, field emission scanning electron microscopy, and high resolution transmission electron microscopy for identifying and discriminating antibiotics. Each antibiotic exhibits distinct binding affinities toward these sensing elements, leading to varied colorimetric and UV–visible absorption response patterns, which lead to unique “fingerprints” associated with each antibiotic. These patterns are quantitatively distinguishable through linear discriminant analysis, decision tree algorithm, random forest algorithm, support vector machine, and hierarchical clustering analysis. With 100% accuracy, the sensor array successfully discriminates between eight antibiotics (amoxicillin, azithromycin, neomycin, streptomycin, chloramphenicol, ofloxacin, fluconazole, and ciprofloxacin), with detection limits ranging from 1.7 to 8.3 μM. Additionally, binary and ternary mixture ratios of various antibiotics have also been successfully discriminated. Further, for the real-time applications, we have developed prototypes for colorimetric analysis and also modified the previously developed 96-well plate reader, which functions similarly to the UV–visible absorption spectrophotometer. These on-site sensing methods, with straightforward preparation, quick response, exceptional sensitivity, and consistently stable high-throughput signal output, show significant potential for practical use in food forensics and for environmental remediation.
{"title":"Tailoring Nanoparticle Surfaces Empowered by Multivariate Techniques for Detection of Multiple Antibiotic Fingerprints in Real Samples Using Hand-Held Colorimetric Signal Readout","authors":"Ranbir, Gagandeep Singh, Navneet Kaur, Narinder Singh","doi":"10.1021/acsami.5c21359","DOIUrl":"https://doi.org/10.1021/acsami.5c21359","url":null,"abstract":"Due to the complex and varied toxicological characteristics exhibited by different antibiotics, which present significant risks to both the environment and human health, there is an urgent requirement for highly efficient sensors capable of detecting antibiotics. The present study introduces a straightforward yet efficient colorimetric sensor array comprising surface-tailored nanoparticles, analyzed using different techniques including dynamic light scattering, zeta potential, Fourier transformation infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy, atomic force microscopy, field emission scanning electron microscopy, and high resolution transmission electron microscopy for identifying and discriminating antibiotics. Each antibiotic exhibits distinct binding affinities toward these sensing elements, leading to varied colorimetric and UV–visible absorption response patterns, which lead to unique “fingerprints” associated with each antibiotic. These patterns are quantitatively distinguishable through linear discriminant analysis, decision tree algorithm, random forest algorithm, support vector machine, and hierarchical clustering analysis. With 100% accuracy, the sensor array successfully discriminates between eight antibiotics (amoxicillin, azithromycin, neomycin, streptomycin, chloramphenicol, ofloxacin, fluconazole, and ciprofloxacin), with detection limits ranging from 1.7 to 8.3 μM. Additionally, binary and ternary mixture ratios of various antibiotics have also been successfully discriminated. Further, for the real-time applications, we have developed prototypes for colorimetric analysis and also modified the previously developed 96-well plate reader, which functions similarly to the UV–visible absorption spectrophotometer. These on-site sensing methods, with straightforward preparation, quick response, exceptional sensitivity, and consistently stable high-throughput signal output, show significant potential for practical use in food forensics and for environmental remediation.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"226 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729218","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}
Digital highly sensitive biodetection is increasingly crucial for early disease diagnosis and treatment, particularly for accurate quantification of low-abundance biomarkers. Current digital biodetection methods represented as single-molecule assay (Simoa), enzyme- or DNA-assisted signal amplification strategy, the fluorescence nanosphere labeling-based digital biodetection, etc. often rely on microcompartments or time-consuming signal amplification steps, facing challenges in terms of cumbersome workflow, insufficient signal strength, and limited clinical accessibility. To address these limitations, we propose a high-sensitivity chamber-free digital immunoassay strategy based on a standard flow cytometer, which utilizes dendritic mesoporous silica nanoparticles (DMSNs) doped with quantum dots (QDs) forming ultrabright fluorescence nanospheres (DMSN@QDs@Silica, DQS) as signal label. Structure–function relationship (SFR) of DQS was systematically investigated to obtain DQS with optimal labeling kinetics and fluorescence brightness. The synthesized DQS are significantly brighter than commercial label fluorescent nanospheres, enabling direct digital signal detection via flow cytometry, which eliminates the need for isolation chambers and multistep signal amplification processes, simplifying the assay and reducing associated costs. We demonstrate that the high-sensitive DQS-based digital assay provides approximately 24-fold improvement in sensitivity over traditional flow cytometry fluorescence immunoassay, achieving a detection limit of 0.37 pg/mL for interleukin-6 (IL-6). This chamber-free digital detection approach holds significant promise for low-abundance biomarker detection, offering enhanced sensitivity, simplicity, and clinical applicability.
{"title":"Quantum Dot-Enriched Dendritic Mesoporous Silica Nanospheres for Chamber-Free Digital Detection: High Sensitivity, Easy Operation, and Clinical Accessibility","authors":"Feiyang Ou, Yida Huang, Yutong Zhang, Fang Gao, Hongchen Gu, Xinyu Zhao, Chang Lei, Chengzhong Yu, Hong Xu","doi":"10.1021/acsami.5c18654","DOIUrl":"https://doi.org/10.1021/acsami.5c18654","url":null,"abstract":"Digital highly sensitive biodetection is increasingly crucial for early disease diagnosis and treatment, particularly for accurate quantification of low-abundance biomarkers. Current digital biodetection methods represented as single-molecule assay (Simoa), enzyme- or DNA-assisted signal amplification strategy, the fluorescence nanosphere labeling-based digital biodetection, etc. often rely on microcompartments or time-consuming signal amplification steps, facing challenges in terms of cumbersome workflow, insufficient signal strength, and limited clinical accessibility. To address these limitations, we propose a high-sensitivity chamber-free digital immunoassay strategy based on a standard flow cytometer, which utilizes dendritic mesoporous silica nanoparticles (DMSNs) doped with quantum dots (QDs) forming ultrabright fluorescence nanospheres (DMSN@QDs@Silica, DQS) as signal label. Structure–function relationship (SFR) of DQS was systematically investigated to obtain DQS with optimal labeling kinetics and fluorescence brightness. The synthesized DQS are significantly brighter than commercial label fluorescent nanospheres, enabling direct digital signal detection via flow cytometry, which eliminates the need for isolation chambers and multistep signal amplification processes, simplifying the assay and reducing associated costs. We demonstrate that the high-sensitive DQS-based digital assay provides approximately 24-fold improvement in sensitivity over traditional flow cytometry fluorescence immunoassay, achieving a detection limit of 0.37 pg/mL for interleukin-6 (IL-6). This chamber-free digital detection approach holds significant promise for low-abundance biomarker detection, offering enhanced sensitivity, simplicity, and clinical applicability.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"372 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732093","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}
Xuan Zhou,Zhidan Huang,Huake Yang,Linbo Jin,Yiming Zhang
Diabetic wounds pose a growing healthcare challenge, characterized by heavy M1 macrophage infiltration, reactive oxygen species (ROS) overproduction, tissue hypoxia, and cytokine storms. The diabetic microenvironment fails to support the critical M1-to-M2 macrophage phenotypic switch, trapping tissues in persistent pathological inflammation that disrupts natural healing processes. In this study, we developed triphenylphosphonium (TPP)-modified mitochondria-targeting nanoparticles, where liposomes encapsulated two metabolomically guided agents: aminooxyacetic acid (AOAA) to suppress nitric oxide (NO) production and hollow mesoporous manganese dioxide (H-MnO2) to scavenge mitochondrial ROS and supply O2. In vitro, after successful mitochondrial internalization by macrophages, the nanoparticles reduced NO and ROS levels, enhanced mitochondrial respiration, and reprogrammed macrophage metabolism─shifting from aerobic glycolysis to oxidative phosphorylation (OXPHOS). This metabolic shift drove macrophage transition from pro-inflammatory M1 to anti-inflammatory M2 and thus resolved aberrant inflammation. In diabetic murine wound models, TPP-L@H-MnO2@AOAA further validated its efficacy. By modulating macrophage repolarization, it promoted re-epithelialization and collagen deposition. Overall, these anti-inflammatory nanoparticles with sustained-release capability provide a promising therapeutic tool for clinical management of diabetic wounds.
{"title":"Mitochondrial-Targeting Drug-Loaded Nanoparticles Reprogram Macrophage Metabolism via ROS/NO Co-elimination for Diabetic Wound Healing.","authors":"Xuan Zhou,Zhidan Huang,Huake Yang,Linbo Jin,Yiming Zhang","doi":"10.1021/acsami.5c19664","DOIUrl":"https://doi.org/10.1021/acsami.5c19664","url":null,"abstract":"Diabetic wounds pose a growing healthcare challenge, characterized by heavy M1 macrophage infiltration, reactive oxygen species (ROS) overproduction, tissue hypoxia, and cytokine storms. The diabetic microenvironment fails to support the critical M1-to-M2 macrophage phenotypic switch, trapping tissues in persistent pathological inflammation that disrupts natural healing processes. In this study, we developed triphenylphosphonium (TPP)-modified mitochondria-targeting nanoparticles, where liposomes encapsulated two metabolomically guided agents: aminooxyacetic acid (AOAA) to suppress nitric oxide (NO) production and hollow mesoporous manganese dioxide (H-MnO2) to scavenge mitochondrial ROS and supply O2. In vitro, after successful mitochondrial internalization by macrophages, the nanoparticles reduced NO and ROS levels, enhanced mitochondrial respiration, and reprogrammed macrophage metabolism─shifting from aerobic glycolysis to oxidative phosphorylation (OXPHOS). This metabolic shift drove macrophage transition from pro-inflammatory M1 to anti-inflammatory M2 and thus resolved aberrant inflammation. In diabetic murine wound models, TPP-L@H-MnO2@AOAA further validated its efficacy. By modulating macrophage repolarization, it promoted re-epithelialization and collagen deposition. Overall, these anti-inflammatory nanoparticles with sustained-release capability provide a promising therapeutic tool for clinical management of diabetic wounds.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"15 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728623","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}
Fu Peng, Linwei He, Ruwei Chen, Yang Yang, Jinming Zheng, Ke He, Zhonglin Ma, Wenqi Zhang, Yunnan Tao, Lingyi Li, Qi Guo, Xintong Guo, Jie Li, Guohao Zhang, Junchang Chen, Songbai Tang, Xinghui Qi, Long Chen, Xiaoqin Nie, Chao Zhao, Zhifang Chai, Shuao Wang
Efficient capture of radioactive iodine is crucial for nuclear safety and environmental protection, yet it remains challenging under dynamic, high-temperature off-gas conditions. Herein, we systematically evaluated the in-depth iodine removal performance of two antimony sulfide frameworks, a 2D-layered and a 3D-channeled architecture (denoted as the 2D-Sb2S3 framework and 3D-Sb2S3 framework), featuring electron-rich sulfide sites and soft Lewis acid antimony ions. Both materials exhibit modest static iodine uptake capacities (3.32 and 3.12 g g–1, respectively), while the 3D framework achieves a superior dynamic capacity of 1.25 g g–1 at 373 K, outperforming benchmark materials such as SCU-SnS (0.88 g g–1) and Ag-loaded silica gel (0.54 g g–1). The application potential of the 3D framework was further confirmed by the continuous accumulation of 131I2 in a radioactive dynamic adsorption setup. Mechanism analysis combined with powder X-ray diffraction, X-ray photoelectron spectroscopy, and time-dependent Raman spectroscopy reveals that iodine uptake proceeds via multiple pathways, including charge-transfer interactions with incorporated macrocyclic polyamines and the redox-induced formation of SbI3. This work introduces a new design paradigm for redox-active metal sulfide adsorbents by leveraging soft acid/base interactions and framework reactivity, offering a viable approach for advanced iodine capture in nuclear waste management.
有效捕获放射性碘对核安全和环境保护至关重要，但在动态、高温的废气条件下仍然具有挑战性。在此，我们系统地评估了两种硫化锑框架的深度除碘性能，一种是2d层状结构，一种是3d通道结构（称为2D-Sb2S3框架和3D-Sb2S3框架），具有富电子硫化物位点和软刘易斯酸锑离子。两种材料都表现出适度的静态碘吸收能力（分别为3.32和3.12 g g- 1），而3D框架在373 K时达到了1.25 g g- 1的优异动态容量，优于SCU-SnS （0.88 g g- 1）和ag负载硅胶（0.54 g g- 1）等基准材料。在放射性动态吸附装置中，131I2的持续积累进一步证实了三维框架的应用潜力。结合粉末x射线衍射、x射线光电子能谱和时间相关拉曼光谱的机理分析表明，碘的吸收是通过多种途径进行的，包括与结合的大环多胺的电荷转移相互作用和氧化还原诱导的SbI3的形成。这项工作通过利用软酸/碱相互作用和框架反应性，介绍了一种新的氧化还原活性金属硫化物吸附剂的设计范式，为核废料管理中的高级碘捕获提供了一种可行的方法。
{"title":"Redox-Active Antimony Sulfide Frameworks for Dynamic Radioiodine Capture","authors":"Fu Peng, Linwei He, Ruwei Chen, Yang Yang, Jinming Zheng, Ke He, Zhonglin Ma, Wenqi Zhang, Yunnan Tao, Lingyi Li, Qi Guo, Xintong Guo, Jie Li, Guohao Zhang, Junchang Chen, Songbai Tang, Xinghui Qi, Long Chen, Xiaoqin Nie, Chao Zhao, Zhifang Chai, Shuao Wang","doi":"10.1021/acsami.5c19595","DOIUrl":"https://doi.org/10.1021/acsami.5c19595","url":null,"abstract":"Efficient capture of radioactive iodine is crucial for nuclear safety and environmental protection, yet it remains challenging under dynamic, high-temperature off-gas conditions. Herein, we systematically evaluated the in-depth iodine removal performance of two antimony sulfide frameworks, a 2D-layered and a 3D-channeled architecture (denoted as the 2D-Sb<sub>2</sub>S<sub>3</sub> framework and 3D-Sb<sub>2</sub>S<sub>3</sub> framework), featuring electron-rich sulfide sites and soft Lewis acid antimony ions. Both materials exhibit modest static iodine uptake capacities (3.32 and 3.12 g g<sup>–1</sup>, respectively), while the 3D framework achieves a superior dynamic capacity of 1.25 g g<sup>–1</sup> at 373 K, outperforming benchmark materials such as SCU-SnS (0.88 g g<sup>–1</sup>) and Ag-loaded silica gel (0.54 g g<sup>–1</sup>). The application potential of the 3D framework was further confirmed by the continuous accumulation of <sup>131</sup>I<sub>2</sub> in a radioactive dynamic adsorption setup. Mechanism analysis combined with powder X-ray diffraction, X-ray photoelectron spectroscopy, and time-dependent Raman spectroscopy reveals that iodine uptake proceeds via multiple pathways, including charge-transfer interactions with incorporated macrocyclic polyamines and the redox-induced formation of SbI<sub>3</sub>. This work introduces a new design paradigm for redox-active metal sulfide adsorbents by leveraging soft acid/base interactions and framework reactivity, offering a viable approach for advanced iodine capture in nuclear waste management.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"39 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732092","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}
Enzo Pichon,Alexander Fordham,Andrij Pich,Katrien V Bernaerts
Polyureas are a category of polymers widely used in the coating industry for their high performance and the variety of substrates they can efficiently protect. However, for decades, polyureas have been synthesized using toxic diisocyanates and petro-based building blocks, often formulated into solvent-based coatings that release volatile organic compounds (VOCs) upon drying. To address these issues, partially biobased nonisocyanate polyurea (NIPUrea) resins were developed for use in VOC-free hot-melt coating formulations. Since NIPUreas react slower with nucleophilic cross-linkers than isocyanates, NIPUrea-acrylate hybrids were introduced, leveraging rapid photopolymerization to achieve fast curing (30 s). However, the functionalization of polyureas with acrylate groups often requires hazardous reagents (e.g., acrylamide, 2-hydroxyethyl acrylate), emphasizing the need for safer and more sustainable methods. In this study, we developed partially biobased NIPUrea bearing controlled amounts of reactive primary amine end-groups via melt polycondensation. These end groups were functionalized via the aza-Michael reaction, at room temperature and using a nontoxic diacrylate compound. The developed NIPUrea-acrylate hybrids are semicrystalline and are mixed with potentially biobased isobornyl acrylate as a reactive diluent to obtain VOC-free hot-melt coating formulations. The formulations were cured for a maximum of 30 s via radiation curing, obtaining gel contents >96%, and yielded coatings with exceptional performance (>200 water and MEK double-rub resistance, 6H+ scratch hardness, 5B grade adhesion) on both glass and wooden substrates. This work offers a greener approach to the synthesis of fast-curing, high-throughput NIPUrea coating formulations by considerably reducing the toxicity (no acid chlorides, triethylamine, or dichloromethane for acrylate modification; no isocyanates; VOC-free coating application) of the products while maintaining interesting coating performance.
{"title":"Green Synthesis of Biobased NIPUrea-Acrylate Hybrids for Versatile, Fast-Curing Hot-Melt Coating Development.","authors":"Enzo Pichon,Alexander Fordham,Andrij Pich,Katrien V Bernaerts","doi":"10.1021/acsami.5c17304","DOIUrl":"https://doi.org/10.1021/acsami.5c17304","url":null,"abstract":"Polyureas are a category of polymers widely used in the coating industry for their high performance and the variety of substrates they can efficiently protect. However, for decades, polyureas have been synthesized using toxic diisocyanates and petro-based building blocks, often formulated into solvent-based coatings that release volatile organic compounds (VOCs) upon drying. To address these issues, partially biobased nonisocyanate polyurea (NIPUrea) resins were developed for use in VOC-free hot-melt coating formulations. Since NIPUreas react slower with nucleophilic cross-linkers than isocyanates, NIPUrea-acrylate hybrids were introduced, leveraging rapid photopolymerization to achieve fast curing (30 s). However, the functionalization of polyureas with acrylate groups often requires hazardous reagents (e.g., acrylamide, 2-hydroxyethyl acrylate), emphasizing the need for safer and more sustainable methods. In this study, we developed partially biobased NIPUrea bearing controlled amounts of reactive primary amine end-groups via melt polycondensation. These end groups were functionalized via the aza-Michael reaction, at room temperature and using a nontoxic diacrylate compound. The developed NIPUrea-acrylate hybrids are semicrystalline and are mixed with potentially biobased isobornyl acrylate as a reactive diluent to obtain VOC-free hot-melt coating formulations. The formulations were cured for a maximum of 30 s via radiation curing, obtaining gel contents >96%, and yielded coatings with exceptional performance (>200 water and MEK double-rub resistance, 6H+ scratch hardness, 5B grade adhesion) on both glass and wooden substrates. This work offers a greener approach to the synthesis of fast-curing, high-throughput NIPUrea coating formulations by considerably reducing the toxicity (no acid chlorides, triethylamine, or dichloromethane for acrylate modification; no isocyanates; VOC-free coating application) of the products while maintaining interesting coating performance.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"26 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145728633","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}
Wei Xiong, Haoran Tang, Xiaojian Zhang, Xi Luo, Jiashuai Wang, Fei Huang, Yong Cao
Conducting polymers, as a type of pseudocapacitive material, have garnered significant attention in the development of all-organic supercapacitors due to their superior electrochemical properties. While extensive research has been conducted on p-type conducting polymers, n-type analogues continue to face challenges such as poor stability and narrow electrochemical windows. This study presents a method to enhance n-type conducting polymer poly(benzodifurandione) (PBFDO)-based supercapacitors by introducing hydroquinone (HQ) as a redox-active electrolyte additive. With 20 mM HQ, an increase in specific capacitance from 33 to approximately 60 F g–1 is observed, and the device retains over 93% capacity after 50,000 cycles. Experimental results demonstrate that HQ facilitates reversible doping/dedoping processes, thereby improving ion diffusion and polymer stability. Remarkably, even under an ultrahigh power density of 50,000 W kg–1, the device still delivers 5.6 Wh kg–1 of energy density, demonstrating exceptional high-power endurance. Similarly, other hydroquinone derivatives also improve rate capability and long-term stability, thereby mechanistically confirming the universality of this strategy for improving the performance of all-organic energy storage devices.
导电聚合物作为一种赝电容材料，由于其优异的电化学性能，在全有机超级电容器的开发中受到了广泛的关注。虽然对p型导电聚合物进行了广泛的研究，但n型类似物仍然面临稳定性差和电化学窗口狭窄等挑战。本研究提出了一种通过引入对苯二酚作为氧化还原活性电解质添加剂来增强n型导电聚合物聚苯二呋喃二酮（pbdo）基超级电容器的方法。使用20 mM HQ时，观察到比电容从33增加到约60 gf - 1，并且该器件在50,000次循环后保持超过93%的容量。实验结果表明，HQ促进了可逆的掺杂/脱掺杂过程，从而改善了离子扩散和聚合物的稳定性。值得注意的是，即使在50,000 W kg-1的超高功率密度下，该设备仍能提供5.6 Wh kg-1的能量密度，表现出卓越的高功率续航能力。同样，其他对苯二酚衍生物也提高了速率能力和长期稳定性，从而在机械上证实了该策略在提高全有机储能装置性能方面的普遍性。
{"title":"High-Performance n-Type Conducting Polymer-Based Supercapacitors with Enhanced Capacitance and Stability via Redox Additives","authors":"Wei Xiong, Haoran Tang, Xiaojian Zhang, Xi Luo, Jiashuai Wang, Fei Huang, Yong Cao","doi":"10.1021/acsami.5c14387","DOIUrl":"https://doi.org/10.1021/acsami.5c14387","url":null,"abstract":"Conducting polymers, as a type of pseudocapacitive material, have garnered significant attention in the development of all-organic supercapacitors due to their superior electrochemical properties. While extensive research has been conducted on p-type conducting polymers, n-type analogues continue to face challenges such as poor stability and narrow electrochemical windows. This study presents a method to enhance n-type conducting polymer poly(benzodifurandione) (PBFDO)-based supercapacitors by introducing hydroquinone (HQ) as a redox-active electrolyte additive. With 20 mM HQ, an increase in specific capacitance from 33 to approximately 60 F g<sup>–1</sup> is observed, and the device retains over 93% capacity after 50,000 cycles. Experimental results demonstrate that HQ facilitates reversible doping/dedoping processes, thereby improving ion diffusion and polymer stability. Remarkably, even under an ultrahigh power density of 50,000 W kg<sup>–1</sup>, the device still delivers 5.6 Wh kg<sup>–1</sup> of energy density, demonstrating exceptional high-power endurance. Similarly, other hydroquinone derivatives also improve rate capability and long-term stability, thereby mechanistically confirming the universality of this strategy for improving the performance of all-organic energy storage devices.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"74 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718163","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}
Sanyukta A. Patil, Longtu Chen, Christopher Foster, Xinhao Lin, Yuhang Xiao, Xiuling Lu, Bin Feng, Courtney K. Rowe, Kelly A. Burke
Postsurgical pain management remains a persistent challenge for patients and healthcare providers. This work presents an implantable, degradable drug release platform based on silk biomaterials designed to be placed at a desired surgical site intraoperatively to release the local anesthetic bupivacaine in a sustained manner to prevent and treat postsurgical pain. Methacrylate monomers containing different pendant groups are used to generate brush-like polymers on silk fibroin films by surface-initiated reversible addition–fragmentation chain transfer polymerization. These brushes have side groups to control polymer hydrophilicity and facilitate drug attachment via a hydrolyzable tether. Spectroscopy and contact angle goniometry are used to characterize the chemical composition and hydrophobicity of the synthesized films at each synthetic step. In vitro culture and in vivo implant studies show no differences in biocompatibility compared with unmodified silk films. Bupivacaine can be continually released for at least 7 days. The amount of drug released in vitro is increased by increasing the hydrophilicity of the brush-like polymer, and the released anesthetic is effective at blocking the conduction of action potentials of C-fibers and Aδ-fibers ex vivo. These degradable films show promise as a platform to achieve controllable, continuous delivery of local anesthetics for pain control after surgery.
{"title":"Brush-like Polymer Surface on Silk Fibroin Films for Controlled Release of Local Anesthetics","authors":"Sanyukta A. Patil, Longtu Chen, Christopher Foster, Xinhao Lin, Yuhang Xiao, Xiuling Lu, Bin Feng, Courtney K. Rowe, Kelly A. Burke","doi":"10.1021/acsami.5c15685","DOIUrl":"https://doi.org/10.1021/acsami.5c15685","url":null,"abstract":"Postsurgical pain management remains a persistent challenge for patients and healthcare providers. This work presents an implantable, degradable drug release platform based on silk biomaterials designed to be placed at a desired surgical site intraoperatively to release the local anesthetic bupivacaine in a sustained manner to prevent and treat postsurgical pain. Methacrylate monomers containing different pendant groups are used to generate brush-like polymers on silk fibroin films by surface-initiated reversible addition–fragmentation chain transfer polymerization. These brushes have side groups to control polymer hydrophilicity and facilitate drug attachment via a hydrolyzable tether. Spectroscopy and contact angle goniometry are used to characterize the chemical composition and hydrophobicity of the synthesized films at each synthetic step. In vitro culture and in vivo implant studies show no differences in biocompatibility compared with unmodified silk films. Bupivacaine can be continually released for at least 7 days. The amount of drug released in vitro is increased by increasing the hydrophilicity of the brush-like polymer, and the released anesthetic is effective at blocking the conduction of action potentials of C-fibers and Aδ-fibers ex vivo. These degradable films show promise as a platform to achieve controllable, continuous delivery of local anesthetics for pain control after surgery.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"224 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718165","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}
Fei Wu, Le Yang, Qi Zhou, Junjie Wang, Haiping Yu, Mengxiao Li, Yu Li, Huijie Wang, Xinyu Wang, Jingru Liu, Mingjun Hu, Jun Yang
Aqueous batteries demonstrate promising application prospects in large-scale energy storage and portable electronics due to their high safety, environmental friendliness, and low cost. However, their practical application still faces challenges, such as low operating voltage and insufficient energy density. Herein, a pH-asymmetric biphase electrolyte, composed of an alkaline aqueous electrolyte (AE) and an ionic liquid-hydrofluoroether electrolyte (ILE), was designed to decouple the anode and cathode environments. This design caters to the distinct needs of each electrode and enables the successful construction of a high-voltage aqueous rocking-chair lithium-ion battery. This phase-separated electrolyte (PSE) design breaks through the performance limitations of traditional homogeneous electrolytes, achieving a wide electrochemical stability window of 4.1 V and enabling the application of high-potential LiMn2O4 cathode materials. Benefiting from the anode potential negative shift effect dominated by the high-pH value of the alkaline aqueous electrolyte, this dual-phase electrolyte system exhibits significant advantages over conventional single-phase electrolytes, delivering an average discharge voltage of 1.72 V (a 0.35 V enhancement) and an initial specific capacity as high as 220 mAh g–1 (based on the anode). By overcoming the potential limitations of both electrodes, this study provides an innovative technical pathway for developing high-voltage, high-energy-density aqueous batteries.
水电池具有安全、环保、成本低等优点，在大规模储能和便携式电子领域具有广阔的应用前景。然而，它们的实际应用仍然面临着工作电压低、能量密度不足等挑战。本文设计了一种ph不对称双相电解质，由碱性水溶液电解质（AE）和离子液体-氢氟醚电解质（ILE）组成，以实现阳极和阴极环境的去耦。这种设计迎合了每个电极的不同需求，并使高压水性摇椅锂离子电池的成功构建成为可能。这种相分离电解质（PSE）设计突破了传统均质电解质的性能限制，实现了4.1 V的宽电化学稳定窗口，使高电位LiMn2O4正极材料得以应用。得益于高ph值碱性水溶液电解质主导的阳极电位负移效应，该双相电解质体系比传统单相电解质具有显著优势，平均放电电压为1.72 V（提高0.35 V），初始比容量高达220 mAh g-1（基于阳极）。通过克服两种电极的潜在局限性，本研究为开发高压、高能量密度水性电池提供了一条创新的技术途径。
{"title":"Decoupling Electrode Environments with a pH-Asymmetric Biphase Electrolyte for High-Voltage Aqueous Rocking-Chair Batteries","authors":"Fei Wu, Le Yang, Qi Zhou, Junjie Wang, Haiping Yu, Mengxiao Li, Yu Li, Huijie Wang, Xinyu Wang, Jingru Liu, Mingjun Hu, Jun Yang","doi":"10.1021/acsami.5c19509","DOIUrl":"https://doi.org/10.1021/acsami.5c19509","url":null,"abstract":"Aqueous batteries demonstrate promising application prospects in large-scale energy storage and portable electronics due to their high safety, environmental friendliness, and low cost. However, their practical application still faces challenges, such as low operating voltage and insufficient energy density. Herein, a pH-asymmetric biphase electrolyte, composed of an alkaline aqueous electrolyte (AE) and an ionic liquid-hydrofluoroether electrolyte (ILE), was designed to decouple the anode and cathode environments. This design caters to the distinct needs of each electrode and enables the successful construction of a high-voltage aqueous rocking-chair lithium-ion battery. This phase-separated electrolyte (PSE) design breaks through the performance limitations of traditional homogeneous electrolytes, achieving a wide electrochemical stability window of 4.1 V and enabling the application of high-potential LiMn<sub>2</sub>O<sub>4</sub> cathode materials. Benefiting from the anode potential negative shift effect dominated by the high-pH value of the alkaline aqueous electrolyte, this dual-phase electrolyte system exhibits significant advantages over conventional single-phase electrolytes, delivering an average discharge voltage of 1.72 V (a 0.35 V enhancement) and an initial specific capacity as high as 220 mAh g<sup>–1</sup> (based on the anode). By overcoming the potential limitations of both electrodes, this study provides an innovative technical pathway for developing high-voltage, high-energy-density aqueous batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"8 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718212","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}
Efficient and durable catalysts are essential for enhancing the rate of CO2 hydration in aqueous capture systems and addressing the environmental challenges posed by rising atmospheric CO2 levels. Traditional capture methods that rely on strongly alkaline solvents face substantial drawbacks, including high regeneration energy costs and safety concerns owing to harmful byproducts. Carbonic anhydrase (CA), a zinc-containing metalloenzyme, catalyzes CO2 hydration at near-diffusion-limited rates but rapidly degrades in real-world environments. Although various CA-mimetic catalysts have been investigated, they frequently exhibit poor durability and structural stability. In this study, we introduce ZnNC900, a robust Zn single-atom nanozyme derived from a zeolitic imidazolate framework (ZIF-8) through controlled carbonization. ZnNC900 exhibited remarkable catalytic activity for the p-nitrophenyl acetate esterase reaction, which was attributed to its CA-resembling single-atomic Zn sites. Furthermore, surface functionalization with amine-terminalized polyethylene glycol improves the colloidal stability and catalytic performance of ZnNC900 by enhancing its hydrophilicity and CO2 affinity. These enhancements highlight the potential of ZnNC900 as a durable and efficient catalyst for aqueous CO2 capture.
{"title":"Carbonic Anhydrase-Inspired Zn-Single-Atom Nanozyme with High Stability for Enhanced CO2 Hydration Performance","authors":"Daeeun Choi, Seonhye Park, Jinwoo Lee","doi":"10.1021/acsami.5c20250","DOIUrl":"https://doi.org/10.1021/acsami.5c20250","url":null,"abstract":"Efficient and durable catalysts are essential for enhancing the rate of CO<sub>2</sub> hydration in aqueous capture systems and addressing the environmental challenges posed by rising atmospheric CO<sub>2</sub> levels. Traditional capture methods that rely on strongly alkaline solvents face substantial drawbacks, including high regeneration energy costs and safety concerns owing to harmful byproducts. Carbonic anhydrase (CA), a zinc-containing metalloenzyme, catalyzes CO<sub>2</sub> hydration at near-diffusion-limited rates but rapidly degrades in real-world environments. Although various CA-mimetic catalysts have been investigated, they frequently exhibit poor durability and structural stability. In this study, we introduce ZnNC900, a robust Zn single-atom nanozyme derived from a zeolitic imidazolate framework (ZIF-8) through controlled carbonization. ZnNC900 exhibited remarkable catalytic activity for the <i>p</i>-nitrophenyl acetate esterase reaction, which was attributed to its CA-resembling single-atomic Zn sites. Furthermore, surface functionalization with amine-terminalized polyethylene glycol improves the colloidal stability and catalytic performance of ZnNC900 by enhancing its hydrophilicity and CO<sub>2</sub> affinity. These enhancements highlight the potential of ZnNC900 as a durable and efficient catalyst for aqueous CO<sub>2</sub> capture.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"36 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145718214","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}
Tianyi Ji, Yongsheng Liu, Chenhong Zhang, Wei Gong, Yuqing Tian, Jie Gu, Wenjie Zhao, Kerui Li, Qinghong Zhang, Yaogang Li, Chengyi Hou, Hongzhi Wang
As a vital component of humanoid robots and a key module in smart wearable devices, electronic skin plays a significant role in enabling biomimetic perception and interactive feedback. However, achieving the synergistic integration of multimodal perception–response and low-power signal processing remains a significant challenge. In this work, we present a bioinspired electronic skin system with logic-level decoupling of multimodal inputs as its core innovation, which integrates a triboelectric/pyroelectric dual-mode self-powered sensor, an organic electrochemical transistor (OECT) array, and a feedback unit to construct a closed-loop perception–response pathway. By designing OECTs with low threshold voltage and fast response, and optimizing the impedance matching between the electrolyte and the sensor, the system is capable of recognizing and responding to transient and weak signals. More importantly, employing OECTs with different threshold voltages enables clear separation and reliable processing of multimodal signals at the logic level, ensuring accurate information interpretation. The system is ultimately integrated into both a robotic hand and a flexible wearable platform, demonstrating its application potential in human–machine interaction and intelligent feedback.
{"title":"Bioinspired Electronic Skin with Low-Threshold OECTs for Direct Processing of Multimodal Sensing Signals","authors":"Tianyi Ji, Yongsheng Liu, Chenhong Zhang, Wei Gong, Yuqing Tian, Jie Gu, Wenjie Zhao, Kerui Li, Qinghong Zhang, Yaogang Li, Chengyi Hou, Hongzhi Wang","doi":"10.1021/acsami.5c15135","DOIUrl":"https://doi.org/10.1021/acsami.5c15135","url":null,"abstract":"As a vital component of humanoid robots and a key module in smart wearable devices, electronic skin plays a significant role in enabling biomimetic perception and interactive feedback. However, achieving the synergistic integration of multimodal perception–response and low-power signal processing remains a significant challenge. In this work, we present a bioinspired electronic skin system with logic-level decoupling of multimodal inputs as its core innovation, which integrates a triboelectric/pyroelectric dual-mode self-powered sensor, an organic electrochemical transistor (OECT) array, and a feedback unit to construct a closed-loop perception–response pathway. By designing OECTs with low threshold voltage and fast response, and optimizing the impedance matching between the electrolyte and the sensor, the system is capable of recognizing and responding to transient and weak signals. More importantly, employing OECTs with different threshold voltages enables clear separation and reliable processing of multimodal signals at the logic level, ensuring accurate information interpretation. The system is ultimately integrated into both a robotic hand and a flexible wearable platform, demonstrating its application potential in human–machine interaction and intelligent feedback.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"56 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145729220","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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