Developing adsorbents that couple high uranium affinity with durability in complex environments remains a pivotal challenge for efficient uranium harvesting. Here, we report a hierarchically engineered magnetic composite, Fe3O4@PAO@MPN-Met, that integrates (i) a superparamagnetic Fe3O4 core for rapid separation, (ii) an amidoxime-rich polyamidoxime (PAO) shell for uranyl chelation, (iii) a bioinspired metal-polyphenol network (MPN) adhesive layer, and (iv) an in situ mineralized Cu2+/d-methionine (d-Met) metal-organic framework (MOF) that imparts long-lasting antibiofouling activity. Stepwise solvothermal synthesis, surface grafting, and self-assembly preserve nanoscale morphology while reducing the saturation magnetization only to 16.4 emu/g─still sufficient for 1 min magnetic separation. Under optimal conditions, the material achieves a maximum uranium uptake of 272 mg/g, fitting the Langmuir model and quasi-second-order kinetics, indicative mainly of monolayer chemisorption controlled. Thermodynamic analysis reveals a spontaneous, endothermic, and entropy-driven process. The composite shows outstanding selectivity, with uranyl distribution coefficients at least 2 orders of magnitude higher than those of competing ions. After five adsorption-desorption cycles using 0.1 M HNO3, 80% of the initial capacity is retained. Crucially, the Cu-Met nanochannels confer broad-spectrum antibacterial performance, suppressing Pseudomonas aeruginosa formation by 98.54%. In natural Bohai Sea water, after 7 days of adsorption, the uranium adsorption capacity is 0.322 mg/g, highlighting its salt tolerance and antifouling resilience. This multifunctional design, marrying strong amidoxime chelation, magnetic recoverability, and MOF-mediated antibacterial action, offers a viable route toward selective, reusable, and biofouling-resistant adsorbents for large-scale uranium harvesting from seawater.
{"title":"Rapid Magnetic Separation Absorbent Integrating Amidoxime Chelators and Antibiofouling MOF Coatings for Efficient Uranium Extraction.","authors":"Na Jiang, Tingting Zhang, Wei Li, Jingyi Sun, Jinlin Hu, Minghua Lei, Mengyi Yuan, Weihua Li, Rui Lu, Dadong Shao","doi":"10.1021/acsami.5c24112","DOIUrl":"https://doi.org/10.1021/acsami.5c24112","url":null,"abstract":"<p><p>Developing adsorbents that couple high uranium affinity with durability in complex environments remains a pivotal challenge for efficient uranium harvesting. Here, we report a hierarchically engineered magnetic composite, Fe<sub>3</sub>O<sub>4</sub>@PAO@MPN-Met, that integrates (i) a superparamagnetic Fe<sub>3</sub>O<sub>4</sub> core for rapid separation, (ii) an amidoxime-rich polyamidoxime (PAO) shell for uranyl chelation, (iii) a bioinspired metal-polyphenol network (MPN) adhesive layer, and (iv) an in situ mineralized Cu<sup>2+</sup>/d-methionine (d-Met) metal-organic framework (MOF) that imparts long-lasting antibiofouling activity. Stepwise solvothermal synthesis, surface grafting, and self-assembly preserve nanoscale morphology while reducing the saturation magnetization only to 16.4 emu/g─still sufficient for 1 min magnetic separation. Under optimal conditions, the material achieves a maximum uranium uptake of 272 mg/g, fitting the Langmuir model and quasi-second-order kinetics, indicative mainly of monolayer chemisorption controlled. Thermodynamic analysis reveals a spontaneous, endothermic, and entropy-driven process. The composite shows outstanding selectivity, with uranyl distribution coefficients at least 2 orders of magnitude higher than those of competing ions. After five adsorption-desorption cycles using 0.1 M HNO<sub>3</sub>, 80% of the initial capacity is retained. Crucially, the Cu-Met nanochannels confer broad-spectrum antibacterial performance, suppressing <i>Pseudomonas aeruginosa</i> formation by 98.54%. In natural Bohai Sea water, after 7 days of adsorption, the uranium adsorption capacity is 0.322 mg/g, highlighting its salt tolerance and antifouling resilience. This multifunctional design, marrying strong amidoxime chelation, magnetic recoverability, and MOF-mediated antibacterial action, offers a viable route toward selective, reusable, and biofouling-resistant adsorbents for large-scale uranium harvesting from seawater.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140309","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}
Suraj Loomba, Muhammad Waqas Khan, Muhammad Haris, Sharafadeen Gbadamasi, Vasundhara Nettem, Kevin Tran, Lars Thomsen, Anton Tadich, Robiul Alam, Ayesha Zafar, Michelle J S Spencer, Nasir Mahmood
Ionically bonded interfaces are crucial for achieving selective and stable direct seawater electrolysis, yet their vulnerability under corrosive and high-current conditions limits long-term performance. Here, we report a two-dimensional Fe-MOF@PW8O26.B2O3 heterostructured electrocatalyst, synthesized via a solid-liquid interfacial growth strategy, that integrates robust Fe-O-W and tunable Fe-P-W ionic bonds to strengthen interfacial electronic coupling, redox flexibility, and structural integrity. Subsurface B2O3 enhances surface hydroxylation via Lewis acid-base interactions, facilitating catalyst assembly and OH- affinity, while phosphate polyanions at the interface act as electrostatic shields that repel Cl- ions and modulate the redox environment of Fe active sites. This interfacial configuration enables chlorine-suppressive oxygen evolution with a Faradaic efficiency of 97.93%, achieving a current density of 1.75 A cm-2 at 2.0 V and stable operation above 1.5 A cm-2 for over 500 h in alkaline seawater, with an exceptionally low corrosion rate of 0.016 μm per year. NEXAFS and XPS analyses confirm the presence of dual ionic linkages, while DFT calculations reveal their cooperative role in stabilizing the electronic structure and interfacial charge distribution. Beyond hydrogen production, the spent electrolyte is repurposed for CO2 mineralization, achieving 88.76% conversion to stable carbonates, with cytotoxicity assays confirming reduced environmental toxicity. Together, this study establishes a multifunctional ionically engineered platform for durable, chlorine-free seawater electrolysis and integrated carbon capture, advancing the prospects of circular hydrogen systems.
{"title":"Phosphate-Mediated Cl<sup>-</sup> Repulsion and B<sub>2</sub>O<sub>3</sub>-Assisted Hydroxylation Synergize Ionic Interface Stability in Seawater Splitting.","authors":"Suraj Loomba, Muhammad Waqas Khan, Muhammad Haris, Sharafadeen Gbadamasi, Vasundhara Nettem, Kevin Tran, Lars Thomsen, Anton Tadich, Robiul Alam, Ayesha Zafar, Michelle J S Spencer, Nasir Mahmood","doi":"10.1021/acsami.5c20622","DOIUrl":"https://doi.org/10.1021/acsami.5c20622","url":null,"abstract":"<p><p>Ionically bonded interfaces are crucial for achieving selective and stable direct seawater electrolysis, yet their vulnerability under corrosive and high-current conditions limits long-term performance. Here, we report a two-dimensional Fe-MOF@PW<sub>8</sub>O<sub>26</sub>.B<sub>2</sub>O<sub>3</sub> heterostructured electrocatalyst, synthesized via a solid-liquid interfacial growth strategy, that integrates robust Fe-O-W and tunable Fe-P-W ionic bonds to strengthen interfacial electronic coupling, redox flexibility, and structural integrity. Subsurface B<sub>2</sub>O<sub>3</sub> enhances surface hydroxylation via Lewis acid-base interactions, facilitating catalyst assembly and OH<sup>-</sup> affinity, while phosphate polyanions at the interface act as electrostatic shields that repel Cl<sup>-</sup> ions and modulate the redox environment of Fe active sites. This interfacial configuration enables chlorine-suppressive oxygen evolution with a Faradaic efficiency of 97.93%, achieving a current density of 1.75 A cm<sup>-2</sup> at 2.0 V and stable operation above 1.5 A cm<sup>-2</sup> for over 500 h in alkaline seawater, with an exceptionally low corrosion rate of 0.016 μm per year. NEXAFS and XPS analyses confirm the presence of dual ionic linkages, while DFT calculations reveal their cooperative role in stabilizing the electronic structure and interfacial charge distribution. Beyond hydrogen production, the spent electrolyte is repurposed for CO<sub>2</sub> mineralization, achieving 88.76% conversion to stable carbonates, with cytotoxicity assays confirming reduced environmental toxicity. Together, this study establishes a multifunctional ionically engineered platform for durable, chlorine-free seawater electrolysis and integrated carbon capture, advancing the prospects of circular hydrogen systems.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140365","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}
Infrared (IR) photodetectors are crucial for a range of applications, including night vision, optical communication, and environmental monitoring. However, their effectiveness is often hindered by low charge transport and interfacial losses in colloidal quantum dot (CQD)-based designs. MXenes, known for their high metallic conductivity, adjustable surface terminations, and excellent optical transparency, present a unique opportunity to improve interfaces for better optoelectronic performance. In this work, Ti3C2Tx MXene via interface engineering for PbS CQD IR photodetectors, in which it functions as an electrode, transport layer, and interfacial modifier is systematically investigated. As a result, an ultrahigh responsivity of 1032.37 A/W with a specific detectivity of 1.12 × 1013 Jones and an external quantum efficiency of 1.311 × 105 % are obtained from photodetector ITO/ZnO/Ti3C2Tx/PbS/MoO3/Ti3C2Tx under 1 μW/cm2 980 nm illumination. Our finite difference time domain (FDTD) simulations further support and provide a physical basis for our experimental results, indicating that dual MXene incorporation significantly enhances optical field confinement and absorption within the PbS CQD layer. Thus, it illustrates that MXene-enabled interface engineering and optical coupling can establish an effective design paradigm for high-performance, solution-processed infrared photodetectors, effectively bridging the gap between quantum materials and practical optoelectronics.
{"title":"High-Performance Solution-Processed Quantum Dot Infrared Photodetectors via Interface Engineering with MXenes","authors":"Shafaat Hussain,Shengyi Yang,Ayesha Zia,Muhammad Qasim,Bingsuo Zou,Yurong Jiang","doi":"10.1021/acsami.5c25535","DOIUrl":"https://doi.org/10.1021/acsami.5c25535","url":null,"abstract":"Infrared (IR) photodetectors are crucial for a range of applications, including night vision, optical communication, and environmental monitoring. However, their effectiveness is often hindered by low charge transport and interfacial losses in colloidal quantum dot (CQD)-based designs. MXenes, known for their high metallic conductivity, adjustable surface terminations, and excellent optical transparency, present a unique opportunity to improve interfaces for better optoelectronic performance. In this work, Ti3C2Tx MXene via interface engineering for PbS CQD IR photodetectors, in which it functions as an electrode, transport layer, and interfacial modifier is systematically investigated. As a result, an ultrahigh responsivity of 1032.37 A/W with a specific detectivity of 1.12 × 1013 Jones and an external quantum efficiency of 1.311 × 105 % are obtained from photodetector ITO/ZnO/Ti3C2Tx/PbS/MoO3/Ti3C2Tx under 1 μW/cm2 980 nm illumination. Our finite difference time domain (FDTD) simulations further support and provide a physical basis for our experimental results, indicating that dual MXene incorporation significantly enhances optical field confinement and absorption within the PbS CQD layer. Thus, it illustrates that MXene-enabled interface engineering and optical coupling can establish an effective design paradigm for high-performance, solution-processed infrared photodetectors, effectively bridging the gap between quantum materials and practical optoelectronics.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139016","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}
Morphology, which affects the dissociation of excitons and charge transport, determines the performance of organic solar cells (OSCs). Solid additives provide a powerful strategy for improving the molecular packing and fine-tuning the blend morphology. However, current research on additives has primarily focused on those with large dipole moments. Studies on quadrupolar solid additives remain limited, and the potential mechanisms by which the quadrupole moment influences the morphology of the active layer and device performance remain insufficiently understood. Herein, we designed and synthesized the quadrupole solid additive 2,5-di(thiophen-2-yl)pyrazine (M3) to explore its effect on the performance of the OSCs. The M3 molecule exhibits a planar configuration with a net dipole moment of zero while exhibiting a significant quadrupole moment along the π–π stacking direction (Qzz = −108.35 D), which enhances intermolecular interactions. M3 effectively modulates molecular aggregation and packing, influences crystallization behavior, and thereby optimizes the nanoscale morphology and facilitates efficient charge transfer. Consequently, M3-treated PM6:BTP-eC9 devices obtained a power conversion efficiency (PCE) of 19.16%. Impressively, the PM6:BTP-eC9:L8-BO devices processed with M3 achieve an outstanding PCE of 19.62%. This work provides valuable insights into the design of quadrupolar solid additives and elucidates the potential working mechanism for optimizing the morphology and device performance through quadrupolar solid additive engineering.
{"title":"Quadrupole Solid Additive Engineering-Induced Interactions with Both a Donor and an Acceptor Enable Organic Solar Cells Achieving 19.6% Efficiency","authors":"Yawei Miao,Qun Li,Tingting Xue,Shuai Zhang,Fei Zhao,Yunxiang Tang,Yaowei Zhu,Zhenyong Wang,Huajun Xu,Long Pang,Lingheng Kong,Aihuan Sun,Yinfeng Han,Chuantao Gu","doi":"10.1021/acsami.5c26188","DOIUrl":"https://doi.org/10.1021/acsami.5c26188","url":null,"abstract":"Morphology, which affects the dissociation of excitons and charge transport, determines the performance of organic solar cells (OSCs). Solid additives provide a powerful strategy for improving the molecular packing and fine-tuning the blend morphology. However, current research on additives has primarily focused on those with large dipole moments. Studies on quadrupolar solid additives remain limited, and the potential mechanisms by which the quadrupole moment influences the morphology of the active layer and device performance remain insufficiently understood. Herein, we designed and synthesized the quadrupole solid additive 2,5-di(thiophen-2-yl)pyrazine (M3) to explore its effect on the performance of the OSCs. The M3 molecule exhibits a planar configuration with a net dipole moment of zero while exhibiting a significant quadrupole moment along the π–π stacking direction (Qzz = −108.35 D), which enhances intermolecular interactions. M3 effectively modulates molecular aggregation and packing, influences crystallization behavior, and thereby optimizes the nanoscale morphology and facilitates efficient charge transfer. Consequently, M3-treated PM6:BTP-eC9 devices obtained a power conversion efficiency (PCE) of 19.16%. Impressively, the PM6:BTP-eC9:L8-BO devices processed with M3 achieve an outstanding PCE of 19.62%. This work provides valuable insights into the design of quadrupolar solid additives and elucidates the potential working mechanism for optimizing the morphology and device performance through quadrupolar solid additive engineering.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"1 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139012","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}
Xinyu Liu,Alexander F. Simafranca,Julia Chang,Diego Garcia Vidales,Kara Lo,Yutong Wu,Benjamin J. Schwartz,Yves Rubin,Sarah H. Tolbert
The chemical doping of water-soluble conjugated polyelectrolytes (CPEs) offers a promising pathway for the direct printing of semiconducting polymer films by using environmentally friendly solvents. In this study, we explored the chemical doping of the cationic cylindrical micelle-forming CPE poly(cyclopentadithiophene-alt-thiophene) (PCT-NBr) in aqueous solution using two Fe(III)-halide dopants, FeCl3 and FeBr3. Treatment with nonoxidizing salts (KCl and KBr) showed that polymer micelles preferentially interact with Br– ions over Cl– ions, resulting in a more rigid micelle and spectroscopic evidence of Br– ion accumulation around the polymer. Doping with both FeCl3 and FeBr3 was followed using UV-visible-near IR absorption spectroscopy, which indicated that the polymer micelles could be stably doped with both iron compounds. FeCl3 was shown to be a stronger dopant due to differences in the lability of Cl– and Br– ligands in water. Compared at similar concentrations, FeCl3 induces higher doping levels, while FeBr3 generates more delocalized charge carriers, as evidenced by spectral shifts in the polaronic bands, likely due to weaker counterion Coulombic trapping. Small-angle X-ray scattering was used to confirm that a micellar structure was preserved at all doping levels of PCT-NBr, but the data also indicate increased structural disorder in doped polymer micelles, likely due to partial loss of the polymer’s amphiphilic character and ion–polymer interactions. Films spin-cast directly from FeBr3-doped polymer solutions exhibited a stable conductivity of 1.0 S/cm, demonstrating the viability of using doped micellar CPE solutions as a route to single-step deposition of conductive polymer films.
{"title":"Exploring the Chemical Doping of a Water-Soluble Cylindrical Micelle-Forming Conjugated Polyelectrolyte","authors":"Xinyu Liu,Alexander F. Simafranca,Julia Chang,Diego Garcia Vidales,Kara Lo,Yutong Wu,Benjamin J. Schwartz,Yves Rubin,Sarah H. Tolbert","doi":"10.1021/acsami.5c24820","DOIUrl":"https://doi.org/10.1021/acsami.5c24820","url":null,"abstract":"The chemical doping of water-soluble conjugated polyelectrolytes (CPEs) offers a promising pathway for the direct printing of semiconducting polymer films by using environmentally friendly solvents. In this study, we explored the chemical doping of the cationic cylindrical micelle-forming CPE poly(cyclopentadithiophene-alt-thiophene) (PCT-NBr) in aqueous solution using two Fe(III)-halide dopants, FeCl3 and FeBr3. Treatment with nonoxidizing salts (KCl and KBr) showed that polymer micelles preferentially interact with Br– ions over Cl– ions, resulting in a more rigid micelle and spectroscopic evidence of Br– ion accumulation around the polymer. Doping with both FeCl3 and FeBr3 was followed using UV-visible-near IR absorption spectroscopy, which indicated that the polymer micelles could be stably doped with both iron compounds. FeCl3 was shown to be a stronger dopant due to differences in the lability of Cl– and Br– ligands in water. Compared at similar concentrations, FeCl3 induces higher doping levels, while FeBr3 generates more delocalized charge carriers, as evidenced by spectral shifts in the polaronic bands, likely due to weaker counterion Coulombic trapping. Small-angle X-ray scattering was used to confirm that a micellar structure was preserved at all doping levels of PCT-NBr, but the data also indicate increased structural disorder in doped polymer micelles, likely due to partial loss of the polymer’s amphiphilic character and ion–polymer interactions. Films spin-cast directly from FeBr3-doped polymer solutions exhibited a stable conductivity of 1.0 S/cm, demonstrating the viability of using doped micellar CPE solutions as a route to single-step deposition of conductive polymer films.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"90 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139017","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}
A promising method for directing cell behavior and tissue regeneration is the use of smart materials that can transform physical inputs into bioelectrical signals. In this study, the mechanoelectrical control of preosteoblast activity was investigated using a piezoelectric smart biointerface based on positively poled poly(vinylidene fluoride) (PVDF). Distinct mechanical regimes, including vibrational and cyclic stretching, were applied through customized bioreactors, enabling controlled mechanoelectrical inputs ranging from 63 to 227 μVpp mm-2. The biological response of MC3T3-E1 cells was evaluated in terms of metabolic activity, intracellular calcium signaling, alkaline phosphatase (ALP) activity, matrix mineralization, and gene expression (RUNX2, ALP, OPN, and OCN). The results demonstrated that stretching stimulation combined with higher mechano electric inputs (113-227 μVpp mm-2) enhanced calcium influx and enhanced osteogenic differentiation, while lower impulses (∼63 μVpp mm-2) under vibrational circumstances increased cell proliferation. These findings highlight the intensity- and mode-dependent nature of mechanoelectrical signaling in regulating osteogenic commitment. All things considered, this study shows how piezoelectric smart materials can be used as bioresponsive platforms to precisely control cell proliferation and differentiation, creating avenues for bone tissue engineering's next-generation regenerative techniques.
{"title":"Vibration or Stretch? Distinct Mechanoelectrical Signatures Govern Osteogenic Programming in PVDF.","authors":"Sylvie Ribeiro, Clarisse Ribeiro, Nélson Castro, Vitor Correia, Igor Irastorza, Unai Silván, Senentxu Lanceros-Mendez","doi":"10.1021/acsami.5c23327","DOIUrl":"https://doi.org/10.1021/acsami.5c23327","url":null,"abstract":"<p><p>A promising method for directing cell behavior and tissue regeneration is the use of smart materials that can transform physical inputs into bioelectrical signals. In this study, the mechanoelectrical control of preosteoblast activity was investigated using a piezoelectric smart biointerface based on positively poled poly(vinylidene fluoride) (PVDF). Distinct mechanical regimes, including vibrational and cyclic stretching, were applied through customized bioreactors, enabling controlled mechanoelectrical inputs ranging from 63 to 227 μVpp mm<sup>-2</sup>. The biological response of MC3T3-E1 cells was evaluated in terms of metabolic activity, intracellular calcium signaling, alkaline phosphatase (ALP) activity, matrix mineralization, and gene expression (RUNX2, ALP, OPN, and OCN). The results demonstrated that stretching stimulation combined with higher mechano electric inputs (113-227 μVpp mm<sup>-2</sup>) enhanced calcium influx and enhanced osteogenic differentiation, while lower impulses (∼63 μVpp mm<sup>-2</sup>) under vibrational circumstances increased cell proliferation. These findings highlight the intensity- and mode-dependent nature of mechanoelectrical signaling in regulating osteogenic commitment. All things considered, this study shows how piezoelectric smart materials can be used as bioresponsive platforms to precisely control cell proliferation and differentiation, creating avenues for bone tissue engineering's next-generation regenerative techniques.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140305","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}
Vu Thi Tuyet Thuy,Lam Tan Hao,Hyo Jeong Kim,Dominik Voll,Patrick Theato
Water presents a fundamental challenge for tissue adhesives, requiring both the removal of bulk water and the interfacial hydration layer to achieve robust adhesion. Most marine-organism-inspired phenolic adhesives fail to meet key requirements for clinical use, including rapid, strong adhesion under physiological conditions, long-term stability, and scalable fabrication. Herein, we report a scalable guanidinium-functionalized double-sided tape (Gd+-DST) incorporating tannic acid that acts as a cross-linker and a phenolic adhesive component. This DST adheres within 5 s and achieves a record-high wet adhesion on porcine skin with interfacial toughness up to 1200 J m–2 and shear strength up to 210 kPa after being underwater for 24 h. This performance arises from a synergistic mechanism: the Gd+-DST matrix rapidly absorbs and removes bulk water while suppressing swelling via chain rearrangement, and guanidinium-mediated multifaceted interactions and chaotropic properties promote interfacial dehydration and hydrophobic reorganization. These processes enable spontaneous, time-dependent adhesion reinforcement without external stimuli. Our Gd+-DST is flexible and biocompatible and gradually disintegrates under physiological conditions while also serving as a platform for drug loading and delivery. This study establishes a practical, multifunctional underwater adhesive with clinical relevance and offers molecular-level insights into water removal adhesion mechanisms.
{"title":"Guanidinium-Functionalized Double-Sided Tape as a Robust Tissue Adhesive Combining Bulk Water Clearance and Interfacial Dehydration","authors":"Vu Thi Tuyet Thuy,Lam Tan Hao,Hyo Jeong Kim,Dominik Voll,Patrick Theato","doi":"10.1021/acsami.5c24574","DOIUrl":"https://doi.org/10.1021/acsami.5c24574","url":null,"abstract":"Water presents a fundamental challenge for tissue adhesives, requiring both the removal of bulk water and the interfacial hydration layer to achieve robust adhesion. Most marine-organism-inspired phenolic adhesives fail to meet key requirements for clinical use, including rapid, strong adhesion under physiological conditions, long-term stability, and scalable fabrication. Herein, we report a scalable guanidinium-functionalized double-sided tape (Gd+-DST) incorporating tannic acid that acts as a cross-linker and a phenolic adhesive component. This DST adheres within 5 s and achieves a record-high wet adhesion on porcine skin with interfacial toughness up to 1200 J m–2 and shear strength up to 210 kPa after being underwater for 24 h. This performance arises from a synergistic mechanism: the Gd+-DST matrix rapidly absorbs and removes bulk water while suppressing swelling via chain rearrangement, and guanidinium-mediated multifaceted interactions and chaotropic properties promote interfacial dehydration and hydrophobic reorganization. These processes enable spontaneous, time-dependent adhesion reinforcement without external stimuli. Our Gd+-DST is flexible and biocompatible and gradually disintegrates under physiological conditions while also serving as a platform for drug loading and delivery. This study establishes a practical, multifunctional underwater adhesive with clinical relevance and offers molecular-level insights into water removal adhesion mechanisms.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"45 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146138986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The pursuit of durable and eco-friendly antifouling surfaces has become a critical challenge across engineered systems, ranging from architectural coatings to marine infrastructure. Herein, we propose an innovative stepwise physicochemical antifouling mechanism through the rational integration of hierarchical superamphiphobic architectures with bactericidal copper oxide nanoparticles. The designed coating operates via a sequential defense protocol: physical antiadhesion enabled by a superamphiphobic surface exhibiting ultralow surface energy, coupled with a chemical antibacterial effect through controlled Cu2+ ion release from embedded CuO nanoparticles. When the action time reaches 24 h, the coating shows excellent antibacterial effects against Gram-negative Escherichia coli (E. coli), Pseudomonas aeruginosa (P. aeruginosa), and Gram-positive Staphylococcus aureus (S. aureus). A scalable spray-coating technique was developed using 3-aminopropyltriethoxysilane (APTES)-functionalized CuO/SiO2 nanocomposites with 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PFDTES) modification for the coating fabrication. Systematic characterization combining Cassie-Baxter modeling, X-ray Photoelectron Spectroscopy (XPS) analysis, and bacterial viability assays confirms the mechanistic coupling between topographical liquid repellency and chemical bactericidal activity. The contact angle (CA) value of CuO-SiO2/APTES@PFDTES calculated by dynamic density functional theory (DDFT) is 165.5°. This work provides a promising strategy for the rational design of advanced superamphiphobic antifouling coatings through physicochemical antibacterial strategies.
{"title":"Stepwise Physicochemical Design of Antifouling Materials: Integrating Superamphiphobic Surfaces with Antibacterial Nanoparticles for Dual-Action Defense.","authors":"Yuxuan Chen, Zhipeng Liu, Jiadong Yang, Fanfeng Ding, Zhen Jia, Zhe Hu, Yanan Li, Yu Liu, Zebao Rui","doi":"10.1021/acsami.5c13854","DOIUrl":"https://doi.org/10.1021/acsami.5c13854","url":null,"abstract":"<p><p>The pursuit of durable and eco-friendly antifouling surfaces has become a critical challenge across engineered systems, ranging from architectural coatings to marine infrastructure. Herein, we propose an innovative stepwise physicochemical antifouling mechanism through the rational integration of hierarchical superamphiphobic architectures with bactericidal copper oxide nanoparticles. The designed coating operates via a sequential defense protocol: physical antiadhesion enabled by a superamphiphobic surface exhibiting ultralow surface energy, coupled with a chemical antibacterial effect through controlled Cu<sup>2+</sup> ion release from embedded CuO nanoparticles. When the action time reaches 24 h, the coating shows excellent antibacterial effects against Gram-negative <i>Escherichia coli</i> (<i>E. coli</i>), <i>Pseudomonas aeruginosa</i> (<i>P. aeruginosa</i>), and Gram-positive <i>Staphylococcus aureus</i> (<i>S. aureus</i>). A scalable spray-coating technique was developed using 3-aminopropyltriethoxysilane (APTES)-functionalized CuO/SiO<sub>2</sub> nanocomposites with 1H,1H,2H,2H-perfluorodecyltriethoxysilane (PFDTES) modification for the coating fabrication. Systematic characterization combining Cassie-Baxter modeling, X-ray Photoelectron Spectroscopy (XPS) analysis, and bacterial viability assays confirms the mechanistic coupling between topographical liquid repellency and chemical bactericidal activity. The contact angle (CA) value of CuO-SiO<sub>2</sub>/APTES@PFDTES calculated by dynamic density functional theory (DDFT) is 165.5°. This work provides a promising strategy for the rational design of advanced superamphiphobic antifouling coatings through physicochemical antibacterial strategies.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140284","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}
Kyoung Ryeol Park, Phuong Minh Nguyen, Seyoung Park, Jihoon Son, Daehyeon Ko, Kyu-Bong Jang, Hyeyoung Shin, Sungwook Mhin
Rational design of efficient and robust electrocatalysts for the oxygen evolution reaction (OER) is essential for advancing electrochemical water splitting systems. In this work, we report an Fe-incorporated NiCo layered double hydroxide (NiCoFe-LDH) nanosheet array grown directly on three-dimensional (3D) nickel foam via a facile hydrothermal route. Among the various compositions investigated, optimized NiCoFe-LDH exhibits significantly enhanced OER activity, delivering a low overpotential of 215 mV at 100 mA cm-2 and maintaining long-term catalytic stability. Structural and compositional analyses reveal that Fe incorporation induces a distinct electronic modulation: Fe doping downshifts the d-band center, which weakens the adsorption of key OER intermediates such as *O and lowers the reaction energy barrier for the rate-determining step, thereby accelerating OER kinetics. Bader charge analysis and the crystal orbital Hamilton population further support weakened metal-oxygen bonding upon Fe substitution. The combined modulation of the local electronic structure and active site configuration provides clear mechanistic insight into the origin of the enhanced OER activity, presenting an effective design strategy for developing transition metal-based electrocatalysts with high OER performance.
{"title":"Fe-Mediated Destabilization of Oxygen Intermediates Boosts Oxygen Evolution in Multimetallic Layered Double Hydroxides.","authors":"Kyoung Ryeol Park, Phuong Minh Nguyen, Seyoung Park, Jihoon Son, Daehyeon Ko, Kyu-Bong Jang, Hyeyoung Shin, Sungwook Mhin","doi":"10.1021/acsami.5c23304","DOIUrl":"https://doi.org/10.1021/acsami.5c23304","url":null,"abstract":"<p><p>Rational design of efficient and robust electrocatalysts for the oxygen evolution reaction (OER) is essential for advancing electrochemical water splitting systems. In this work, we report an Fe-incorporated NiCo layered double hydroxide (NiCoFe-LDH) nanosheet array grown directly on three-dimensional (3D) nickel foam via a facile hydrothermal route. Among the various compositions investigated, optimized NiCoFe-LDH exhibits significantly enhanced OER activity, delivering a low overpotential of 215 mV at 100 mA cm<sup>-2</sup> and maintaining long-term catalytic stability. Structural and compositional analyses reveal that Fe incorporation induces a distinct electronic modulation: Fe doping downshifts the d-band center, which weakens the adsorption of key OER intermediates such as *O and lowers the reaction energy barrier for the rate-determining step, thereby accelerating OER kinetics. Bader charge analysis and the crystal orbital Hamilton population further support weakened metal-oxygen bonding upon Fe substitution. The combined modulation of the local electronic structure and active site configuration provides clear mechanistic insight into the origin of the enhanced OER activity, presenting an effective design strategy for developing transition metal-based electrocatalysts with high OER performance.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140344","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}
Radiative cooling is a passive cooling technology that could potentially address critical sustainability challenges by improving energy efficiency across different applications, including building materials, coatings, electronics, and outdoor devices. Photonic radiative coolers are a discrete category that utilizes photonic structures to optimize the emission properties of the material in the atmospheric transparency window (ATW) regime (8-13 μm). Due to their efficiency and adaptive nature, photonic radiative coolers offer a promising avenue as an adaptable cooling technology. However, a major challenge in transitioning this technology from laboratory to practical use remains. To address this barrier, large area, scalable and low-cost methods and materials need to be implemented. In this study, we demonstrate the fabrication of a transparent microstructured polymer-based radiative cooling (MPRC) film using nanoimprint lithography with a hybrid organic-inorganic UV-curable resist, namely, Ormocomp. We report the optical properties of Ormocomp within the atmospheric transparency window, which had not been previously characterized and utilize them to reveal the underlying mechanisms leading to emissivity enhancement. The MPRC film has over 90% transmission in the visible-NIR wavelengths and provides an─above ambient─cooling effect of -3 °C compared to bare Si reference sample under direct sunlight even though the solar absorptivity of silicon is lower. Our suggested design and fabrication approach is suitable for applications that need optical transparency or can be paired with reflective substrates to further enhance cooling performance, offering a practical and scalable radiative cooling solution.
{"title":"Radiative Cooling with Transparent Microstructured Hybrid Organic-Inorganic Polymer Film Fabricated by Nanoimprint Lithography.","authors":"Nefeli Dimogerontaki, Nikolaos Matthaiakakis, Nikolaos Kehagias","doi":"10.1021/acsami.5c19843","DOIUrl":"https://doi.org/10.1021/acsami.5c19843","url":null,"abstract":"<p><p>Radiative cooling is a passive cooling technology that could potentially address critical sustainability challenges by improving energy efficiency across different applications, including building materials, coatings, electronics, and outdoor devices. Photonic radiative coolers are a discrete category that utilizes photonic structures to optimize the emission properties of the material in the atmospheric transparency window (ATW) regime (8-13 μm). Due to their efficiency and adaptive nature, photonic radiative coolers offer a promising avenue as an adaptable cooling technology. However, a major challenge in transitioning this technology from laboratory to practical use remains. To address this barrier, large area, scalable and low-cost methods and materials need to be implemented. In this study, we demonstrate the fabrication of a transparent microstructured polymer-based radiative cooling (MPRC) film using nanoimprint lithography with a hybrid organic-inorganic UV-curable resist, namely, Ormocomp. We report the optical properties of Ormocomp within the atmospheric transparency window, which had not been previously characterized and utilize them to reveal the underlying mechanisms leading to emissivity enhancement. The MPRC film has over 90% transmission in the visible-NIR wavelengths and provides an─above ambient─cooling effect of -3 °C compared to bare Si reference sample under direct sunlight even though the solar absorptivity of silicon is lower. Our suggested design and fabrication approach is suitable for applications that need optical transparency or can be paired with reflective substrates to further enhance cooling performance, offering a practical and scalable radiative cooling solution.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":" ","pages":""},"PeriodicalIF":8.2,"publicationDate":"2026-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146140350","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}