ACS Applied Materials & Interfaces最新文献

{"title":"Corrections to “Synergistic Amelioration of Osseointegration and Osteoimmunomodulation with a Microarc Oxidation-Treated Three-Dimensionally Printed Ti-24Nb-4Zr-8Sn Scaffold via Surface Activity and Low Elastic Modulus”","authors":"Xinyue Yang, Lijun Wu, Cheng Li, Shujun Li, Wentao Hou, Yulin Hao, Yiping Lu, Lei Li","doi":"10.1021/acsami.6c12212","DOIUrl":"10.1021/acsami.6c12212","url":null,"abstract":"","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"56918–56919"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092218","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}

{"title":"Rapid Joule-Heating Preparation of GO/GNs Graphene-Based Composite Films for Thermal Management","authors":"Ning Li,&nbsp;Jianyin Miao,&nbsp;Junhao Liu,&nbsp;Jing Li","doi":"10.1021/acsami.6c12867","DOIUrl":"10.1021/acsami.6c12867","url":null,"abstract":"<p>Traditional metal heat sinks are limited by moderate thermal conductivity, high density, and poor flexibility, which restrict their use in compact and lightweight electronics. Graphene films offer high in-plane thermal conductivity, but rapid reduction of graphene oxide (GO) releases gases from oxygen-containing groups and can generate pores, interlayer damage, and poor film densification. Here, we report a precursor-design strategy that combines reduced graphene oxide nanosheets (GNs) with carboxylated cellulose nanofibers (CNFs). The composite films (GO/GNs-X) were prepared by blade coating, hot-press carbonization, and secondary Joule-heating graphitization. The combined precursor was designed to mitigate gas-release-induced damage and support carbon-network reconstruction during high-temperature treatment. The optimized GF, with a thickness of approximately 25 μm, reached an in-plane thermal conductivity of 950.5 ± 20 W m^–1 K^–1 and an electrical conductivity of 2.31 × 10⁵ S m^–1. At a comparable thickness, this thermal conductivity was 26.6% higher than that of an additive-free RGO-2600-ref film prepared without GNs/CNF modification. In LED heat-dissipation tests, the surface-centre temperature decreased from 83.7 to 40.4 °C. Because individual-additive controls were not included, the respective contributions of GNs and CNF could not be separated. These results establish combined precursor modification as a route to thin, lightweight graphene heat spreaders. Such films may be useful for thermal management in compact electronics, foldable devices, and aerospace systems.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"56299–56308"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149151913","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}

{"title":"Direct Regeneration of Spent Graphite Electrodes Using an Organic Solvent-Free Approach: Evaluation of Aqueous- and Rapid Thermal Processing-Assisted Black Mass Delamination","authors":"Marco di Mauro,Yuhui An,Amogh Subramanya Barla,Hsin-Juei Wang,Anirudh Nandakumar,Emily Lopez Chilel,Wei Li,Zheng Chen,Yoon Hwa,Candace K. Chan","doi":"10.1021/acsami.6c15291","DOIUrl":"https://doi.org/10.1021/acsami.6c15291","url":null,"abstract":"Sustainable recycling of graphite anodes is critical for enabling closed-loop lithium-ion battery manufacturing, yet most direct recycling methods rely on organic solvents and corrosive acid treatments that increase costs and environmental impacts. Herein, we evaluate an organic solvent-free, direct recycling strategy that combines aqueous graphite recovery with boric acid-assisted regeneration. Water-based delamination of graphite black mass was investigated using two representative commercial end-of-life graphite anodes and a commercially manufactured uncycled graphite anode. The effectiveness of aqueous separation of the black mass from the Cu current collector was investigated along with rapid thermal processing (RTP), which has been proposed to improve graphite recovery through binder degradation. Both methods resulted in effective graphite recovery despite impurities originating from ceramic-coated separators, Ti-containing additives, and current collector corrosion. However, delamination of RTP-treated spent anodes was more difficult than pristine anodes, requiring pre-RTP washing and ultrasonication for efficient graphite recovery. Boric acid treatment followed by calcination at 1050 °C increased the degree of graphitization for all spent graphite samples while removing residual surface species and trapped lithium. Electrochemical testing showed that the regenerated graphite largely recovered its capacity and electrochemical activity, although residual metallic impurities may limit long-term cycling stability. Overall, aqueous delamination combined with boric acid-assisted regeneration provides an effective and more sustainable route for graphite recycling by eliminating organic solvents and strong mineral acids while preserving favorable structural and electrochemical properties. This process offers a promising pathway for scalable, environmentally responsible recovery of graphite from end-of-life lithium-ion batteries.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"14 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149225987","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}

{"title":"Robust Anomalous Hall Effect in Epitaxial Cubic D03-Fe3Ge Nanoplates Grown via Chemical Vapor Deposition","authors":"Mingxuan Chen,Chao Chen,Siqi Jiang,Shuxiang Qiao,Hongyan Lu,Di Zhang,Jiabei Huang,Fuzhuo Lian,Zhaochen Qu,Siqin Wang,Ziyi Wang,Shuai Zhang,Yulu Liu,Ronghua Liu,Xiaoxiang Xi,Renjun Du,Lei Wang,Geliang Yu","doi":"10.1021/acsami.6c14914","DOIUrl":"https://doi.org/10.1021/acsami.6c14914","url":null,"abstract":"Iron-based ferromagnetic materials have emerged as a promising system for spintronics due to their high Curie temperatures and the significant anomalous Hall effect (AHE) driven by Berry curvature. While there have been investigations into the epitaxial growth of nonlayered iron-based ferromagnetic materials, the realization of high-quality single crystal thin films continues to be a formidable obstacle. Meanwhile, issues such as grain boundary scattering further hinder their characterization and application. Here, we report the first chemical vapor deposition synthesis of single-crystalline cubic D03-Fe3Ge nanoplates. This compound represents a substantial departure from the conventional hexagonal phases typically observed in the Fe–Ge system. Structural characterizations confirm the cubic lattice and the stoichiometric purity of the crystals. Structural analysis identifies a strong epitaxial effect, resulting in a giant compressive strain of ∼4.16% at the interface that relaxes gradually toward the surface. The second-harmonic generation signals might further reveal that such interfacial strain disrupted the inherent centrosymmetry of the cubic phase. Superconducting quantum interference device magnetometry shows robust room-temperature ferromagnetism and clear magnetic anisotropy. Magneto-transport measurements reveal a robust AHE that remains stable at temperatures far exceeding the room temperature. The scaling observed between the anomalous Hall resistance and longitudinal resistance strongly suggests that this effect is dominated by the intrinsic Berry curvature mechanism. Furthermore, density functional theory calculations reveal that the huge epitaxial strain induces band reconstructions and creates dense spin–orbit coupling gaps near the Fermi level, effectively doubling the anomalous Hall conductivity to match our experimental observations.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"33 1","pages":""},"PeriodicalIF":9.5,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149226004","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}

{"title":"Defect-Engineered Core–Shell MOF Nanointerface Functionalized with Hemagglutinin for Target-Guided Anti-influenza Ligand Discovery","authors":"Hui Wang,&nbsp;Wei Zhao,&nbsp;Xiaoyun Liu,&nbsp;Xiaojing Liang,&nbsp;Rong Rong,&nbsp;Tiantian Si","doi":"10.1021/acsami.6c17733","DOIUrl":"10.1021/acsami.6c17733","url":null,"abstract":"<p>Preserving the biological function of conformationally dynamic proteins after immobilization remains a major challenge in biointerface engineering. Here, a defect-engineered hierarchical MOF nanointerface (D-MOF-808-HET@MOF-808@SiO₂) was constructed through evaporation-induced interfacial coordination assembly for hemagglutinin (HA) immobilization and target-guided ligand screening. XPS analysis supported coordination-mediated interactions between HA and accessible Zr sites of the defect-engineered interface, as indicated by altered Zr 3d and O 1s binding energies. The immobilized HA retained a hemagglutination titer above 5.0 log₂, indicating preservation of its biological activity. The HA-functionalized interface interfered with viral attachment to host cells during the early stage of H1N1 PR8 infection and was subsequently used as an affinity matrix to enrich HA-associated constituents from Mahuang-Xixin-Fuzi Decoction. Twelve candidate ligands were identified, of which hypaconitine, naringenin, ethyl caffeate, and vitexin were further evaluated by surface plasmon resonance and cellular antiviral assays. Hypaconitine exhibited the strongest HA-binding affinity (<em>K</em>_D = 1.72 μM) but showed relatively weak antiviral activity (EC₅₀ = 50.03 μM), whereas ethyl caffeate and vitexin displayed superior antiviral activities (EC₅₀ = 1.54 and 2.56 μM) despite moderate HA affinities (<em>K</em>_D = 11.06 and 12.20 μM, respectively), revealing an affinity–activity mismatch. Molecular docking predicted different ligand interaction patterns, with ethyl caffeate and vitexin showing interactions near the HA1–HA2 interdomain region, whereas hypaconitine and naringenin exhibited alternative predicted interaction regions. These differences in predicted binding modes may contribute to the observed functional disparity. These findings suggest that equilibrium affinity alone does not fully account for antiviral activity and support HA-functionalized MOF nanointerfaces as a platform for target-guided screening of bioactive constituents from complex natural-product mixtures.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"56015–56028"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149091553","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}

{"title":"Feedstock-Driven Design of CO2 Sorbents via Chemical Upcycling of Plastics and Elastomers","authors":"Seulchan Lee,&nbsp;Gwanho Park,&nbsp;Lance Khizner Dabu Gragasin,&nbsp;Soon Hyeok Hong","doi":"10.1021/acsami.6c14604","DOIUrl":"10.1021/acsami.6c14604","url":null,"abstract":"<p>Plastic and elastomer wastes are abundant, carbon-rich feedstocks. At the same time, carbon capture requires sorbents that perform under realistic temperatures, humidity, dilute CO₂, and repeated regeneration. This review surveys feedstock-driven chemical upcycling routes that transform waste polymers into CO₂ sorbents, while treating carbonization-derived physisorbents as a comparative benchmark and pragmatic fallback for chemically intractable or highly heterogeneous feedstocks. We frame “waste-to-sorbent” conversion as a feedstock-driven design problem in which inherited constitutional chemistry, network and morphology, formulation, and acquired chemistry—collectively termed chemical memory—govern feasible transformations and capture performance. We organize the literature by major feedstocks—PET, PVC, polystyrene, rubbers/tires, polyolefins, and mixed plastics—and compare physisorption- and chemisorption-dominant architectures with emphasis on binding-site accessibility, transport limits, humidity effects, impurity tolerance, oxidative stability, and regeneration windows. Because cross-study comparison is often hindered by inconsistent testing conditions and incomplete characterization of both starting feedstocks and resulting sorbents, we propose a mechanism-aware benchmarking framework and minimum reporting protocol centered on feedstock descriptors, application-relevant CO₂ partial pressures, working capacity, accessible-site metrics (e.g., effective nitrogen/amine efficiency), ultramicropore descriptors, and durability under humid/impure cycling. These guidelines connect feedstock chemistry to deployable sorbent design and accelerate translation beyond headline capacities.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"55769–55792"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092006","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}

{"title":"Electrolyte-Induced Band Bending and Barrier Tuning to Enhance Photodetection in Inkjet-Printed Organic–Inorganic Heterojunctions","authors":"Manvendra Singh,&nbsp;Mohammed Hadhi Pazhaya Puthanveettil,&nbsp;Subho Dasgupta","doi":"10.1021/acsami.6c12401","DOIUrl":"10.1021/acsami.6c12401","url":null,"abstract":"<p>Hybrid organic–inorganic heterojunctions have attracted considerable interest in optoelectronic applications, as they combine the excellent electronic transport of inorganic semiconductors with the ease of processing and tunability of organic conductors. While the performance of such heterojunctions is strongly governed by their built-in electric field and interfacial band alignment, strategies for actively tuning these parameters in printed bulk heterojunctions have remained largely unexplored. In this regard, here we show an inkjet-printed bulk heterojunction diode with semiconducting amorphous indium gallium oxide (a-IGO) and conducting poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS), whose interfacial barrier can be dynamically modulated by a solvent (dimethyl sulfoxide, DMSO) or a composite solid polymer electrolyte (CSPE). Systematic studies of pristine, DMSO-treated, and CSPE-treated devices reveal that DMSO enhances charge transport in PEDOT:PSS, while mobile ions of CSPE penetrate the polymer matrix and accumulate at the heterojunction interface. Capacitance–voltage measurements show that ionic screening increases the built-in potential from 0.36 to 0.70 eV by inducing additional band bending within a-IGO. Consequently, the off-current decreases by more than two orders of magnitude, accompanied by a substantial enhancement in rectification ratio. The strengthened junction field promotes efficient separation of photogenerated carriers under ultraviolet illumination, increasing the photosensitivity from 10³ to beyond 10⁶ while achieving a responsivity of 80 A/W, a specific detectivity of 0.25 × 10¹² Jones, and an external quantum efficiency of 27200%. This elevated built-in potential further enables zero-biased ultraviolet photodetection with a photosensitivity of ∼10⁴ and a responsivity of 45 mA/W. Furthermore, a three-terminal electrolyte-gated device can demonstrate ion-induced modulation of the interfacial barrier, enabling a transition from rectifying to near-Ohmic behavior and thereby realizing a tuneable diode. This electrolyte-assisted ionic-modulation strategy enables reconfigurable hybrid heterojunctions for next-generation, energy-efficient sensing and multifunctional optoelectronic applications.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"56287–56298"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149092016","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}

{"title":"Ferroelectric Properties of MBE Grown BTO/STO:Nb Layer","authors":"Kevin Nadaud,&nbsp;Mohamed Bounab,&nbsp;Lucio Martinelli,&nbsp;Maurizio De Santis,&nbsp;Anne D. Lamirand,&nbsp;Romain Bachelet,&nbsp;Anna K. Ott,&nbsp;Guillaume F. Nataf,&nbsp;Mustapha Zaghrioui,&nbsp;Mohamed-Ramzi Ammar,&nbsp;Clarisse Furgeaud,&nbsp;Guillaume Saint-Girons","doi":"10.1021/acsami.6c14883","DOIUrl":"10.1021/acsami.6c14883","url":null,"abstract":"<p>Barium titanate (BaTiO₃, BTO) is an archetypal ferroelectric of broad technological relevance. Molecular beam epitaxy (MBE) offers compelling advantages for BTO thin film growth, such as superior crystalline quality and epitaxial integration with semiconductor substrates. However, the low oxygen partial pressures inherent to MBE environments, together with the challenges associated with precise stoichiometry control when using elemental sources, promote composition imbalances and oxygen vacancy formation and make MBE-grown BTO films significantly less documented than their pulsed laser deposition (PLD) or sputtered counterparts. Here, we present a detailed study of the ferroelectric response of an epitaxial MBE-grown BTO thin film, combining synchrotron-based X-ray diffraction with temperature- and frequency-dependent electrical characterizations, including the first Rayleigh analysis reported for an MBE-grown BTO layer and only the third direct demonstration of ferroelectricity in such films based on macroscopic <em>P</em>(<em>E</em>) and ε(<em>E</em>) loops. The film exhibits a soft ferroelectric response—low coercive field (12 kV/cm), high tunability (≃65%), and a large Rayleigh coefficient reflecting significant irreversible domain wall motion. We show that this response is governed by a landscape of weak oxygen vacancy pinning centers, whose effect is amplified by the high structural quality, full plastic relaxation, and pure c-oriented single-domain state of the film. These results provide a physically grounded picture of the ferroelectric response of MBE-grown BTO thin films, offering a solid basis for device optimization.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"56318–56332"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149101000","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}

{"title":"A Tumor Microenvironment-Triggered Calcium Ion and Hydroxyl Radical Amplifier with Near-Infrared Absorption for Photoacoustic Imaging-Guided Calcium Overload-Synergized Multimodal Cancer Therapy","authors":"Yuzhen Ma,&nbsp;Caiying Li,&nbsp;Min He,&nbsp;Lixian Huang,&nbsp;Fanggui Ye,&nbsp;Jingjin Zhao,&nbsp;Shengqiang Hu,&nbsp;Shulin Zhao","doi":"10.1021/acsami.6c16377","DOIUrl":"10.1021/acsami.6c16377","url":null,"abstract":"<p>Calcium overload therapy represents a highly promising therapeutic strategy and has attracted extensive attention in the field of tumor treatment. Nevertheless, the challenge of achieving high-concentration and precise enrichment of calcium ions inside tumors seriously hinders the clinical translation of this therapy. Moreover, monotherapy fails to deliver superior anti-tumor efficacy. To address such issues, a tumor microenvironment (TME)-triggered calcium ion and hydroxyl radical amplifier with near-infrared absorption (CuMPB@CaCO₃@HA) is presented to process calcium overload-synergized multimodal combination therapy. It can bind to the CD44 receptor on the surface of cancer cells, thereby accumulating in tumor tissues, where it is decomposed by the TME to release Ca²⁺ and copper-doped mesoporous Prussian blue (CuMPB). The released Ca²⁺ triggers intracellular calcium overload. The released CuMPB has a characteristic absorption peak in the range of 650–900 nm, which enables photoacoustic (PA) imaging and photothermal therapy of the tumor. In addition, Cu²⁺ in CuMPB undergoes a cascade reaction with highly abundant glutathione and H₂O₂ in the TME, producing hydroxyl radicals (·OH); additionally, the Fe²⁺ ion in MPB also undergoes a Fenton reaction with H₂O₂ to generate ·OH, achieving highly efficient chemodynamic therapy (CDT). Moreover, laser irradiation promotes the generation of ·OH, thereby further enhancing CDT. Both in vitro and in vivo experiments verified that CuMPB@CaCO₃@HA enables in situ PA diagnosis of tumors to visualize tumor accumulation and optimize the treatment window and enables PA imaging-guided synergistic calcium overload-chemodynamic-photothermal antitumor therapy based on TME characteristics, thus providing a new strategy for the development of tumor-targeted nanotheranostic agents, highlighting the untapped potential of nanoassembly.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"55988–56004"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149126040","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}

{"title":"Architecture-Driven Supramolecular Assembly in Bottlebrush Hydrogels","authors":"Xiaoxiao Ma,&nbsp;Baiqiang Huang,&nbsp;Jinchang Zhu,&nbsp;Ka Un Lao,&nbsp;Li-Heng Cai","doi":"10.1021/acsami.6c12705","DOIUrl":"10.1021/acsami.6c12705","url":null,"abstract":"<p>Supramolecular materials are traditionally designed by strengthening noncovalent interactions or increasing the number of binding motifs. Here, we demonstrate a fundamentally different strategy: using macromolecular architecture to amplify weak molecular interactions into robust material functions. Bottlebrush poly(ethylene glycol) (PEG) polymers, consisting of a linear backbone densely grafted with short side chains, transform tetrazine π–π interactions that are insufficient to gel linear polymers into stable supramolecular hydrogels without covalent crosslinking. The resulting networks remain stable up to ∼65 °C, undergo shear-reversible solid–liquid transitions, and disassemble upon tetrazine deactivation. Density functional theory calculations reveal unusually strong antiparallel tetrazine–tetrazine interactions (∼17 <em>k</em>_B<em>T</em> at room temperature), supporting the hypothesis that the bottlebrush architecture promotes molecular alignment and cooperative association. By varying polymer concentration and tetrazine grafting ratio, we uncover a universal scaling relationship between hydrogel stiffness and the distance from the percolation threshold, with two distinct regimes that deviate from classical percolation theory. The hydrogels are cytocompatible and, unlike linear PEG hydrogels, exhibit minimal fibrotic encapsulation following implantation in immunocompetent mice. These findings establish molecular architecture as a design principle for supramolecular assembly, demonstrating that robust material function can emerge from the architectural amplification of weak interactions and enabling a class of injectable antifibrotic biomaterials.</p>","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"18 41","pages":"55845–55856"},"PeriodicalIF":7.8,"publicationDate":"2026-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149126086","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}