ACS Applied Polymer Materials最新文献

{"title":"Highly Mechanical Polyurethane Elastomers with UV-Assisted Self-Healing for Use as Conductive Polymer Substrates","authors":"Meng-Yu Hou,&nbsp;, ,&nbsp;Pei-Wen Li,&nbsp;, ,&nbsp;Yujie Zhang,&nbsp;, ,&nbsp;Chen Zhang,&nbsp;, ,&nbsp;Zhi-Hui Ren,&nbsp;, and ,&nbsp;Zheng-Hui Guan*,&nbsp;","doi":"10.1021/acsapm.5c02970","DOIUrl":"https://doi.org/10.1021/acsapm.5c02970","url":null,"abstract":"<p >Polymeric materials integrating high mechanical strength, electrical conductivity, and self-healing capabilities demonstrate significant potential for advanced flexible electronics. Nevertheless, concurrent optimization of these mutually exclusive properties remains a critical challenge in materials design. A UV-responsive self-healing polyurethane elastomer (HEOMC-0.5) was synthesized via one-pot copolymerization, incorporating multiple hydrogen bonds and coumarin-derived photoreversible cross-links. Subsequent integration of carbon nanotubes (CNTs, 5 wt %) yielded an electrically conductive composite (HEOMC-0.5-CNTs). The composite exhibited exceptional mechanical (a mechanical strength of 28.42 MPa and a tensile strain of 1528.57%) and self-healing properties (a healing efficiency of 88.99%). Upon doping with CNTs, it possessed an electrical conductivity of 0.2098 mS/cm. Due to the self-healing property of HEOMC-0.5-CNTs, it can act as a “switch” in the circuit to control the lighting on and off of small bulbs through its healing ability. This synergistic design combines dynamic covalent networks with supramolecular interactions, enabling multifunctional polyurethanes. The integrated mechanical, electrical, and self-healing performance establishes a versatile strategy for advanced flexible electronics.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12877–12885"},"PeriodicalIF":4.7,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Polymer Brush-Coated Magnetic Nanoparticles: Diels–Alder/Retro-Diels–Alder Chemistry-Mediated Dual Functionalization for Targeted Drug Delivery","authors":"Busra Cengiz,&nbsp;, ,&nbsp;Idil Itir Demiralp,&nbsp;, ,&nbsp;Aysun Degirmenci,&nbsp;, ,&nbsp;Nora Ejderyan,&nbsp;, ,&nbsp;Rana Sanyal,&nbsp;, and ,&nbsp;Amitav Sanyal*,&nbsp;","doi":"10.1021/acsapm.5c02378","DOIUrl":"https://doi.org/10.1021/acsapm.5c02378","url":null,"abstract":"<p >Polymer-coated magnetic nanoparticles play a vital role in many biomedical technologies ranging from disease diagnostics to therapeutic delivery. The effective postpolymerization functionalization of polymer brushes is important for enabling their utilization for intended applications. In this regard, the thiol-maleimide conjugation reaction provides an efficient tool for the attachment of bioactive molecules and ligands. In this study, maleimide-containing polymer brushes are fabricated on nanoparticle surfaces by using a graft-from approach. A furan-protected maleimide monomer is utilized during the polymerization, followed by deprotection of the thiol-reactive maleimide group using the retro-Diels–Alder cycloreversion. Using a thiol-containing fluorescent hydrophobic dye, we demonstrate effective functionalization of the maleimide-containing polymer brush-coated nanoparticles. Interestingly, the partial deprotection of the maleimide groups furnishes dual-functionalizable polymer brush-coated nanoparticles. While the maleimide groups provide a conjugation handle for thiol-containing molecules, the furan-protected bicyclic adduct undergoes cycloaddition with tetrazine-containing molecules through the inverse-electron-demand Diels–Alder reaction. Dual functionalization of the polymeric coating is demonstrated through the conjugation of two different fluorescent dyes in an orthogonal fashion. To highlight the utility of such dual-functionalizable platforms, a thiol-containing anticancer drug, doxorubicin, and a tetrazine-containing cyclic-peptide-based targeting group are conjugated. The targeted drug-conjugated polymer brush-coated nanoparticles show enhanced cytotoxicity and internalization into the MDA-MB-231 breast cancer cell lines. We envision that the dual-functionalizable polymer brush-coated nanoparticles reported here are amenable to facile functionalization and thus can be tailored for a variety of biomedical applications.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12500–12509"},"PeriodicalIF":4.7,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/pdf/10.1021/acsapm.5c02378","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134661","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"In Situ Enhancement in the β-Phase Content of a PVDF Film Achieved by Circumfluent Synergistic Blow Molding Technology","authors":"Haowei Jiang,&nbsp;, ,&nbsp;Nannan Bao,&nbsp;, ,&nbsp;ZhiKun Gao,&nbsp;, ,&nbsp;ZeXiang Xie,&nbsp;, ,&nbsp;Cong Fang,&nbsp;, and ,&nbsp;Jin-Ping Qu*,&nbsp;","doi":"10.1021/acsapm.5c01912","DOIUrl":"https://doi.org/10.1021/acsapm.5c01912","url":null,"abstract":"<p >High β-phase crystal content of PVDF is commonly achieved by a transition from the kinetically favorable α-phase via various treatments; however, directly enhancing β-phase content from melt crystallization still remains challenging. Especially, during traditional blown film processing, the large condensate depression and rapid cooling rate dominate the crystallization progress, greatly restraining the stretching effect caused by the draw ratio and blow-up ratio, which significantly hinders the α- to β-phase transition and restricts the development of PVDF blown films. Herein, this work introduces Circumfluent Synergistic Blow Molding Technology (CSBMT), which utilizes the rotation of a blow molding die to generate a circumferential shear flow field (CSFF). CSFF can induce molecular chain preorientation during the melt state in the die, which reduces the energy barrier for ordered chain arrangement. Then, the synergistic effect of stretching and CSFF facilitates conformational transitions, realizing an in situ enhancement of β-phase content, which has increased by 50%. Consequently, the PVDF film manifests benign dielectric constant (12 at 50 Hz), low dielectric loss (0.033 at 1 kHz), and high triboelectric voltage (105 V), which satisfies multiple electronic applications. Therefore, CSBMT establishes a paradigm for tailoring PVDF crystallization and broadens a pathway for the development of PVDF blown films.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12231–12239"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134718","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Light-Controlled Release of Water-Soluble Photosensitizers from a Biocompatible Polymer Based on Polyallylamine Functionalized with Folic Acid","authors":"Gerardo Armijos-Capa,&nbsp;, ,&nbsp;Jimena S. Tuninetti,&nbsp;, ,&nbsp;Mariana P. Serrano*,&nbsp;, and ,&nbsp;Andrés H. Thomas*,&nbsp;","doi":"10.1021/acsapm.5c02380","DOIUrl":"https://doi.org/10.1021/acsapm.5c02380","url":null,"abstract":"<p >We have synthesized a photoactive polymer capable of releasing, upon irradiation, fluorescent compounds with photosensitizing properties. Folic acid (PteGlu), a vitamin of the folate family, was covalently attached to polyallylamine (PAH), a biocompatible polymer. The functionalization was optimized to obtain a substitution degree of approximately 1% with 50% of conversion in less than 2 h of reaction time. The resulting modified polymer (PAH-PteGlu) was purified by size exclusion chromatography and characterized by NMR to confirm covalent binding. A detailed study of physicochemical and photochemical properties was carried out after functionalization. PAH-PteGlu is highly soluble and stable not only in water but also in acidic conditions. This is a significant improvement over its parent molecule, folic acid, which becomes insoluble at low pH. Upon excitation with UVA radiation (320–400 nm) in air-saturated aqueous solutions, the attached PteGlu underwent cleavage and oxidation, yielding H₂O₂ and 6-formylpterin (Fop), which, in turn, photooxidized to 6-carboxypterin (Cap). In this photochemical process, the pterin moiety was released, whereas the <i>p</i>-aminobenzoylglutamic acid (PABA-Glu) portion remained attached to PAH. To explore the functionality of PAH-PteGlu as a vehicle for photodynamic therapies (PDT), the photosensitizing properties were evaluated using the nucleoside 2′-deoxyguanosine (dG) as a model of oxidizable biological target. The nucleoside was consumed upon irradiation in the presence of PAH-PteGlu. However, dG was not photosensitized directly by PAH-PteGlu, but by Fop and Cap, released in the photolysis of PAH-PteGlu.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12569–12580"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134680","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Flexible Biosensor Based on Electrospun H3PO4@PVP Nanofibers with Improved Detection Range for Wearable Pressure Sensing","authors":"Huixin Yu,&nbsp;, ,&nbsp;Qingzhou Wang,&nbsp;, ,&nbsp;Dengzun Yao*,&nbsp;, ,&nbsp;Zhongxiang Yu,&nbsp;, ,&nbsp;Rajendra Dhakal*,&nbsp;, ,&nbsp;Qihui Zhou*,&nbsp;, ,&nbsp;Yuanyue Li*,&nbsp;, ,&nbsp;Zhao Yao*,&nbsp;, and ,&nbsp;Xuewei Li*,&nbsp;","doi":"10.1021/acsapm.5c02552","DOIUrl":"https://doi.org/10.1021/acsapm.5c02552","url":null,"abstract":"<p >Flexible pressure sensors are gaining increasing attention in areas such as human movement monitoring and human–computer interaction. However, maintaining good sensitivity over a wide detection range is still very challenging. This paper introduces a flexible capacitive pressure sensor distinguished by its high performance and broad detection range. The H₃PO₄@PVP composite nanofibers membrane is created using the electrospun technique, which resulted in an extensive detection range (0–800 kPa) and maintains a high sensitivity over this range (0.506 kPa^–1@ 0–100 kPa, 0.230 kPa^–1@ 100–600 kPa, and 0.041 kPa^–1@ 600–800 kPa). In addition, the proposed biosensor exhibits a short response time of ∼44 ms and remains stable after undergoing 3500 load-unload cycles. Consequently, the biosensor captures physiological signals from various locations on the human body, detects body movements, and monitors interactions between the human body and the external environment. Furthermore, with the assistance of the developed Microcontroller Unit (MCU) detection and display system, the proposed biosensor can accurately perceive external ambient pressure, making it a true tactile biosensor that demonstrates exceptional sensitivity to both ultralow and high pressures generated by human activities.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 19","pages":"13147–13157"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enhancing the Seebeck Coefficient and Power Factor of PEDOT:PSS Thermoelectric Films through MXene Incorporation and Post-Treatment","authors":"Yabo Xu,&nbsp;, ,&nbsp;Jingshuang Ma,&nbsp;, ,&nbsp;Zhao Nan,&nbsp;, ,&nbsp;Yanfang Wang,&nbsp;, ,&nbsp;Yaowei Han,&nbsp;, ,&nbsp;Hua Wang*,&nbsp;, ,&nbsp;Bo Zhao*,&nbsp;, and ,&nbsp;Lu Jia,&nbsp;","doi":"10.1021/acsapm.5c02162","DOIUrl":"https://doi.org/10.1021/acsapm.5c02162","url":null,"abstract":"<p >Combining the conductive polymer of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) with two-dimensional nanomaterials is an effective approach to develop a thermoelectric composite film and generator. Herein, we exfoliated n-type few-layer MXene nanosheets and explored the effect of the MXene content on the thermoelectric properties of the composite films prepared by vacuum-assisted filtration. When the MXene content reaches 6 wt %, the Seebeck coefficient improves to 28.5 μV/K with an increase ratio of 43.9%. Additionally, a solvent post-treatment method was employed to address the reduced electrical conductivity of the composite film caused by the MXene incorporation. The power factor of the PEDOT:PSS/6 wt % Ti₃C₂T_<i>x</i> composite film could be enhanced from 30.1 to 41.3 μW/m K² after post-treatment with a dimethyl sulfoxide (DMSO) solvent at 333 K. A six-leg generator fabricated from the DMSO-treated composite film achieves an open-circuit voltage of 2.56 mV and a power density of 42.6 μW/cm² under a temperature difference of 30 K. The results reveal the synergy of hybrid and post-treatment and demonstrate that the composite film of PEDOT:PSS/MXene has great potential in wearable thermoelectric fields.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12356–12366"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134707","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Conversion of Waste PET Plastic to Aramid Fiber","authors":"Darrell D. Mayberry*,&nbsp;, ,&nbsp;Yelin Ni,&nbsp;, ,&nbsp;Yuan Jiang,&nbsp;, ,&nbsp;Nicole R. Overman,&nbsp;, ,&nbsp;Angel Ortiz,&nbsp;, ,&nbsp;Kumari Sushmita,&nbsp;, ,&nbsp;Jotheeswari Kothandaraman,&nbsp;, and ,&nbsp;Daniel R. Merkel*,&nbsp;","doi":"10.1021/acsapm.5c02336","DOIUrl":"https://doi.org/10.1021/acsapm.5c02336","url":null,"abstract":"<p >A three-step synthesis was used to convert waste poly(ethylene terephthalate) (PET) into the high-value polymer, poly-<i>para</i>-phenylene terephthalamide (PPTA), used in the production of high-strength aramid fiber, such as Kevlar. Improvements to the polymerization reaction by the addition of calcium chloride to the solvent, <i>N</i>-methyl-2-pyrrolidone, and rigorous anhydrous conditions enabled the production of PET-derived PPTA with a 4.15 dL/g inherent viscosity in sulfuric acid that is amenable to fiber spinning. PPTA fibers were spun using a wet spinning apparatus under varied process parameters to assess their impact on fiber surface morphology, diameter, and the mechanical properties of the fibers. Select fibers were subjected to a postspinning heat treatment at 150 °C, which improved the tensile strength and modulus by 100% and 30%, respectively, relative to the as-spun fibers. Techno-economic and life-cycle analyses were conducted to evaluate the economic feasibility and the life-cycle greenhouse gas emissions of the approach. The results suggest the potential for up to a 30% cost reduction and comparable greenhouse gas emissions against conventional petroleum-based processes.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12480–12490"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134695","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Effects of Aluminum Alloy and Steel Molds on the Productivity, Mechanical Properties, and Surface Quality of Semicrystalline PP Molded Parts","authors":"Kunpeng Deng,&nbsp;, ,&nbsp;Guoqun Zhao*,&nbsp;, and ,&nbsp;Jiachang Wang,&nbsp;","doi":"10.1021/acsapm.5c02436","DOIUrl":"https://doi.org/10.1021/acsapm.5c02436","url":null,"abstract":"<p >Aluminum alloy mold (abbreviated as Al mold) is gradually replacing steel mold as an important development direction in the injection mold industry due to its light weight and efficient heat transfer. However, the disparities in the heat transfer performance of molds exert distinct influences on the crystallization behavior of the polymers. To evaluate the potential of an Al mold for molding crystalline polymer, this study carried out the injection molding of semicrystalline polypropylene (PP) by a steel mold and an Al mold, respectively. The differences in the cooling and crystallization behaviors of PP in the two molds were elucidated through multidimensional characterization and numerical simulation. The results demonstrate that the low volumetric heat capacity and high thermal conductivity of the aluminum alloy minimize heat storage, enhancing both the heat exchange efficiency and the cavity temperature uniformity of the mold. Compared to the steel mold, the cavity temperature uniformity of the Al mold is improved by approximately 75%, and the temperature fluctuation is reduced by about 52%. The Al mold augments the temperature gradient and shear rate gradient in the melt thickness direction, which enhances the crystal orientation and molecular chain entanglement density at the shear region of the molded parts. Consequently, the tensile, flexural, and impact strengths of the PP molded parts are improved by about 3.33%, 7.78%, and 12.5%, respectively. Meanwhile, the high cooling rate of the Al mold can significantly increase the thickness of the freezing layer and reduce the uneven shrinkage of the surface layer of the PP molded part, which makes the replication accuracy of the PP polymer on the cavity surface of the Al mold better than that on the cavity surface of the steel mold. In addition, the Al mold offers additional advantages of shorter processing time, reduced wear of equipment, and low manufacturing costs.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12550–12568"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134694","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Warpage-Resistant, Under-Extrusion-Free, High-Surface-Quality Additive Manufacturing Process for Polyethylene-Based Composite Radiation Shielding Material","authors":"Duo Xu,&nbsp;, ,&nbsp;Volodymyr Korolovych,&nbsp;, ,&nbsp;You Lyu,&nbsp;, ,&nbsp;Jacqueline Aslarus,&nbsp;, ,&nbsp;Domingo R. Flores-Hernandez,&nbsp;, ,&nbsp;Simo Pajovic,&nbsp;, ,&nbsp;William T. Heller,&nbsp;, ,&nbsp;Lembit Sihver,&nbsp;, and ,&nbsp;Svetlana V. Boriskina*,&nbsp;","doi":"10.1021/acsapm.5c02057","DOIUrl":"https://doi.org/10.1021/acsapm.5c02057","url":null,"abstract":"<p >Polyethylene (PE) is one of the best shielding materials for primary space radiation due to its high hydrogen content. For effective secondary neutron shielding, boron-rich fillers are incorporated to enhance performance. The semicrystalline nature and high thermal expansion coefficient of PE impede its adoption for in situ additive manufacture in space via the fused deposition modeling (FDM) 3D printing. We developed an optimized PE blend to mitigate the effects of under-extrusion and warpage. Guided by studies on extrusion and warpage, we developed an optimal set of printing parameters for the proposed PE blend. The optimum PE blend─both in its pure form and when doped with fillers─has been tested on different FDM printers. The printed structures exhibit high and uniform density, smooth surfaces, no warpage, and competitive mechanical properties. The FDM-printed plates demonstrate efficient shielding from thermal neutrons, predicted via modeling and confirmed experimentally using extended Q-range small-angle neutron scattering.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12304–12320"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134714","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Directional Natural Rubber Latex–Polyacrylamide/Graphene–PNIPAM Bi-Hydrogel for Programmable Complex Stimuli-Responsive Actuations","authors":"Xueliang Feng,&nbsp;, ,&nbsp;Jie-Wei Wong,&nbsp;, ,&nbsp;Mingjin Yang,&nbsp;, ,&nbsp;Qing Zhang,&nbsp;, ,&nbsp;Xiaoxue Liao,&nbsp;, ,&nbsp;Daquan Kek,&nbsp;, ,&nbsp;Zhenzhong Liu*,&nbsp;, ,&nbsp;Jize Liu,&nbsp;, ,&nbsp;Chunxin Ma*,&nbsp;, ,&nbsp;Qingrong Wei,&nbsp;, and ,&nbsp;Tuck-Whye Wong*,&nbsp;","doi":"10.1021/acsapm.5c02849","DOIUrl":"https://doi.org/10.1021/acsapm.5c02849","url":null,"abstract":"<p >Intelligent hydrogels can provide various biomimetic actuations in response to external stimuli, but it is still difficult to program their actuating complexity, which severely limits their further applications. Herein, a stimuli-responsive actuating bi-hydrogel with a directional negative layer and a homogeneous positive layer has been explored. The stretched natural rubber latex–polyacrylamide (NRL-PAAm) hydrogel layer can partly maintain this directional structure, which can further integrate with the photothermal-responsive graphene-poly(<i>N</i>-isopropylacrylamide) (G-PNIPAM) hydrogel layer to obtain the anisotropic bilayer hydrogel. First of all, different from bilayer PNIPAM-based hydrogels, which commonly only achieve two-dimensional (2D) complex actuations, this bi-hydrogel can achieve various not only 2D but also three-dimensional (3D) complex programmable actuations, especially because of its double anisotropy of both bilayer and directional structures. Furthermore, this bi-hydrogel can own a rapid actuating speed reaching 27.7°/s of bending and 18.0°/s of folding in response to non-contact near-infrared (NIR) irradiation, mainly owing to the high photothermal conversion efficiency of composited graphene. Last but not least, thanks to the highly enhanced mechanical performance of the directional NRL-PAAm hydrogel layer, this bi-hydrogel is robust, reaching 4.0 times the tensile strength of pure G-PNIPAM, which owns a relatively powerful force to lift more than 50 times its self-weight. This work provides a promising intelligent hydrogel integrating programmable 2D/3D complex actuation, rapid actuating speed, and powerful force, which will also inspire exploration of other soft intelligent materials.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 18","pages":"12868–12876"},"PeriodicalIF":4.7,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}