The development of a superior anode interlayer (AIL) has proved to be key to improving the efficiency and stability of organic solar cells (OSCs). In this work, conducting polypyrrole composite PPy:PMA was exploited to modify the commercially available PEDOT:PSS. With a small amount of PPy:PMA to dope PEDOT:PSS, the device efficiency for the PM6:L8-BO blend film can be improved from 17.7% for the pure PEDOT:PSS to 18.2% for the hybrid AIL. The enhanced performance can be attributed to better match energy levels between the electrode and the active layer, reduction on contact resistance, the inhibition of charge recombination, and increase in the electric conductivity of the AIL. In addition, compared with the devices with pure PEDOT:PSS, the devices based on the hybrid AIL exhibit better photostability and thermal stability. Collectively, our work demonstrates that a synergistic hybrid anode interlayer has great advantages in improving the performance and long-term stability of OSCs.
事实证明，开发优质阳极中间膜（AIL）是提高有机太阳能电池（OSC）效率和稳定性的关键。在这项工作中，利用导电聚吡咯复合材料 PPy:PMA 来改性市售的 PEDOT:PSS。用少量 PPy:PMA 掺杂 PEDOT:PSS，PM6:L8-BO 混合薄膜的器件效率可从纯 PEDOT:PSS 的 17.7% 提高到混合 AIL 的 18.2%。性能的提高可归因于电极和活性层之间能级的更好匹配、接触电阻的降低、电荷重组的抑制以及 AIL 导电性的提高。此外，与纯 PEDOT:PSS 器件相比，基于混合 AIL 的器件具有更好的光稳定性和热稳定性。总之，我们的工作表明，协同混合阳极中间膜在提高 OSC 性能和长期稳定性方面具有巨大优势。
{"title":"Polypyrrole-Decorated Hybrid Anode Interlayer for Enhancing Efficiency and Stability of Non-Fullerene Solar Cells","authors":"Jiafeng Zhang, Lianjie Zhang, Junwu Chen","doi":"10.1021/acsapm.4c01206","DOIUrl":"https://doi.org/10.1021/acsapm.4c01206","url":null,"abstract":"The development of a superior anode interlayer (AIL) has proved to be key to improving the efficiency and stability of organic solar cells (OSCs). In this work, conducting polypyrrole composite PPy:PMA was exploited to modify the commercially available PEDOT:PSS. With a small amount of PPy:PMA to dope PEDOT:PSS, the device efficiency for the PM6:L8-BO blend film can be improved from 17.7% for the pure PEDOT:PSS to 18.2% for the hybrid AIL. The enhanced performance can be attributed to better match energy levels between the electrode and the active layer, reduction on contact resistance, the inhibition of charge recombination, and increase in the electric conductivity of the AIL. In addition, compared with the devices with pure PEDOT:PSS, the devices based on the hybrid AIL exhibit better photostability and thermal stability. Collectively, our work demonstrates that a synergistic hybrid anode interlayer has great advantages in improving the performance and long-term stability of OSCs.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141520871","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}
Near-infrared (NIR)-responsive nanocomposite hydrogels are increasingly utilized in biomedical applications due to their ability to undergo remote-controlled deformation and the deep tissue penetration of NIR light. However, applying high-power lasers may cause skin injuries at the irradiation sites, raising safety concerns for clinical use. Also, the lack of dynamic features (such as self-healing) and processing capability (such as injectability) of the NIR-responsive nanocomposite hydrogels restricts their advanced applications. Here, we enhanced the photothermal efficiency of graphene oxide (GO) by attaching gold nanoparticles (AuNPs), creating a AuNP-decorated GO (GOAu). This GOAu was integrated into a thermoresponsive imine cross-linked hydrogel network made of polydextran aldehyde (PDA) and gelatin (Gel), resulting in PDA/Gel/GOAu nanocomposite hydrogels. The PDA/Gel/GOAu nanocomposite hydrogels were constructed through multiple cross-linking chemistries, including noncovalent chemistry (i.e., coordination, electrostatic interaction, and hydrogen bond) and dynamic covalent chemistry (i.e., imine bond). The structures and properties of the PDA/Gel/GOAu nanocomposite hydrogels were comprehensively investigated in comparison with the PDA/Gel hydrogels and PDA/Gel/GO nanocomposite hydrogels. Adding GOAu to the PDA/Gel network reduced the gelation time of hydrogel formation and improved the rheological and mechanical properties of the PDA/Gel network. The PDA/Gel/GOAu hydrogels exhibited a dose-dependent thermal response to NIR-II light (1064 nm), with the PDA/Gel/GOAu hydrogel containing 4 wt % GOAu achieving the highest temperature among the other hydrogels. The enhanced photothermal properties of the PDA/Gel/GOAu hydrogels were also applied in antibacterial applications based on their capability to perform thermal-induced bactericidal activity and controlled drug release under NIR-II light. Also, with their dynamic properties (i.e., NIR responsiveness, self-healing, and injectability), PDA/Gel/GOAu nanocomposite hydrogels are promising biomaterials for various applications.
{"title":"Fabrication of NIR-II-Responsive Polydextran Aldehyde/Gelatin/Gold Nanoparticle-Decorated Graphene Oxide Nanocomposite Hydrogels for Antibacterial Applications","authors":"Xi-Er Chen, Chen-Jie Yan, Cheng-Hsun Lu, Yi-Cheun Yeh","doi":"10.1021/acsapm.3c03228","DOIUrl":"https://doi.org/10.1021/acsapm.3c03228","url":null,"abstract":"Near-infrared (NIR)-responsive nanocomposite hydrogels are increasingly utilized in biomedical applications due to their ability to undergo remote-controlled deformation and the deep tissue penetration of NIR light. However, applying high-power lasers may cause skin injuries at the irradiation sites, raising safety concerns for clinical use. Also, the lack of dynamic features (such as self-healing) and processing capability (such as injectability) of the NIR-responsive nanocomposite hydrogels restricts their advanced applications. Here, we enhanced the photothermal efficiency of graphene oxide (GO) by attaching gold nanoparticles (AuNPs), creating a AuNP-decorated GO (GOAu). This GOAu was integrated into a thermoresponsive imine cross-linked hydrogel network made of polydextran aldehyde (PDA) and gelatin (Gel), resulting in PDA/Gel/GOAu nanocomposite hydrogels. The PDA/Gel/GOAu nanocomposite hydrogels were constructed through multiple cross-linking chemistries, including noncovalent chemistry (i.e., coordination, electrostatic interaction, and hydrogen bond) and dynamic covalent chemistry (i.e., imine bond). The structures and properties of the PDA/Gel/GOAu nanocomposite hydrogels were comprehensively investigated in comparison with the PDA/Gel hydrogels and PDA/Gel/GO nanocomposite hydrogels. Adding GOAu to the PDA/Gel network reduced the gelation time of hydrogel formation and improved the rheological and mechanical properties of the PDA/Gel network. The PDA/Gel/GOAu hydrogels exhibited a dose-dependent thermal response to NIR-II light (1064 nm), with the PDA/Gel/GOAu hydrogel containing 4 wt % GOAu achieving the highest temperature among the other hydrogels. The enhanced photothermal properties of the PDA/Gel/GOAu hydrogels were also applied in antibacterial applications based on their capability to perform thermal-induced bactericidal activity and controlled drug release under NIR-II light. Also, with their dynamic properties (i.e., NIR responsiveness, self-healing, and injectability), PDA/Gel/GOAu nanocomposite hydrogels are promising biomaterials for various applications.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141521110","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}
Samuel Calderoni, Guillaume Bretel, Medy C. Nongbe, Marie Denis, Erwan Le Grognec, François-Xavier Felpin
This work describes an ultrafast and sustainable approach for the covalent functionalization of cellulose paper using diazo compounds under catalyst-free conditions. The methodology requires ca. 10 min of reaction to attain a level of grafting in the range of 8–17% which allows for significant modification of the physical properties of the cellulosic material. As an application, the work emphasizes the preparation of plastic- and fluorine-free hydrophobic cellulose paper. The grafting of hydrophobic diazo compounds based on cholesterol, an inexpensive, biosourced, abundant, and nontoxic compound, resulted in a material with excellent hydrophobicity and strong oleophobicity, making it suitable for applications in food packaging and textiles as an alternative to plastic and fluorine solutions.
{"title":"Ultrafast and Sustainable Catalyst-Free Chemical Functionalization of Cellulose Paper with Diazo Compounds-Application to Hydrophobic Materials","authors":"Samuel Calderoni, Guillaume Bretel, Medy C. Nongbe, Marie Denis, Erwan Le Grognec, François-Xavier Felpin","doi":"10.1021/acsapm.4c01221","DOIUrl":"https://doi.org/10.1021/acsapm.4c01221","url":null,"abstract":"This work describes an ultrafast and sustainable approach for the covalent functionalization of cellulose paper using diazo compounds under catalyst-free conditions. The methodology requires ca. 10 min of reaction to attain a level of grafting in the range of 8–17% which allows for significant modification of the physical properties of the cellulosic material. As an application, the work emphasizes the preparation of plastic- and fluorine-free hydrophobic cellulose paper. The grafting of hydrophobic diazo compounds based on cholesterol, an inexpensive, biosourced, abundant, and nontoxic compound, resulted in a material with excellent hydrophobicity and strong oleophobicity, making it suitable for applications in food packaging and textiles as an alternative to plastic and fluorine solutions.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141521109","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}
Edwin J. González López, Yohana B. Palacios, Sol R. Martinez, Andrés M. Durantini, Edgardo N. Durantini, Gustavo A. Abraham, Silvestre Bongiovanni Abel, Daniel A. Heredia
A system composed of ethylcellulose (EC) nanofibers loading with [5,10,15,20-tetrakis(pentafluorophenyl)porphyrinato]zinc(II) (TPPF20-Zn) was developed as electrospun mats to contribute to the inactivation of resistant bacteria strains. This tetrapyrrolic macrocycle was chosen for its excellent photostability and straightforward large-scale preparation, which are crucial attributes for practical applications. The synthesis and subsequent characterization of TPPF20-Zn demonstrated scalability and its ability to generate reactive oxygen species (ROS). Subsequently, nanofibrous mats based on EC loaded with different amounts of the porphyrin were obtained using the single-nozzle electrospinning technique after dissolution in a binary solvent mix of N,N-dimethylacetamide/ethanol. The fibers exhibited an adequate morphology at the nanoscale, a narrow diameter distribution, and an absence of beads. Additionally, the thermal and surface properties of the systems were analyzed, revealing no significant changes upon porphyrin incorporation. The developed electrospun composite nanofibrous mats demonstrated the capability to photokill Escherichia coli, as confirmed in planktonic suspension and using advanced fluorescence microscopy. Considering all the studies reported herein, we believe that the EC/TPPF20-Zn mats show promise for practical application in the field of antimicrobial patches or self-sterilizing surfaces.
{"title":"Light-Activated Antibacterial Ethylcellulose Electrospun Nanofibrous Mats Containing Fluorinated Zn(II) Porphyrin","authors":"Edwin J. González López, Yohana B. Palacios, Sol R. Martinez, Andrés M. Durantini, Edgardo N. Durantini, Gustavo A. Abraham, Silvestre Bongiovanni Abel, Daniel A. Heredia","doi":"10.1021/acsapm.4c01167","DOIUrl":"https://doi.org/10.1021/acsapm.4c01167","url":null,"abstract":"A system composed of ethylcellulose (<b>EC</b>) nanofibers loading with [5,10,15,20-tetrakis(pentafluorophenyl)porphyrinato]zinc(II) (<b>TPPF</b><sub><b>20</b></sub><b>-Zn</b>) was developed as electrospun mats to contribute to the inactivation of resistant bacteria strains. This tetrapyrrolic macrocycle was chosen for its excellent photostability and straightforward large-scale preparation, which are crucial attributes for practical applications. The synthesis and subsequent characterization of <b>TPPF<sub>20</sub>-Zn</b> demonstrated scalability and its ability to generate reactive oxygen species (ROS). Subsequently, nanofibrous mats based on <b>EC</b> loaded with different amounts of the porphyrin were obtained using the single-nozzle electrospinning technique after dissolution in a binary solvent mix of <i>N,N</i>-dimethylacetamide/ethanol. The fibers exhibited an adequate morphology at the nanoscale, a narrow diameter distribution, and an absence of beads. Additionally, the thermal and surface properties of the systems were analyzed, revealing no significant changes upon porphyrin incorporation. The developed electrospun composite nanofibrous mats demonstrated the capability to photokill <i>Escherichia coli</i>, as confirmed in planktonic suspension and using advanced fluorescence microscopy. Considering all the studies reported herein, we believe that the <b>EC/TPPF</b><sub><b>20</b></sub><b>-Zn</b> mats show promise for practical application in the field of antimicrobial patches or self-sterilizing surfaces.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141520870","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}
Biodegradable and fluorescent polymer materials have attracted growing research interests due to their tunable properties and various applications such as bioimaging and photonic information technologies. Fluorescent materials obtained by physically blending polymers with organic fluorophores often face the problems of aggregation-caused quenching (ACQ) and photobleaching. We previously reported a series of bioinspired fluorescent polymers covalently linked with a single fluorophore in the middle of each polymer chain, reminiscent of the structure of fluorescent proteins. However, the impact of polymer matrices on the optical properties of these fluorescent polymers remains poorly understood. In this article, we report the influences of different polyesters, containing a common fluorophore of a red fluorescent diketopyrrolopyrrole (DPP) derivative in the middle of each polymer chain, on the optical absorption, fluorescence, and photostability of these polymers in different states, including dilute solutions in a good solvent such as tetrahydrofuran, colloidal nanoparticles in water, and solid films. We further demonstrate the applications of these polymers in the form of colloidal nanoparticles as contrast agents for the fluorescence bioimaging of cells.
{"title":"Influence of the Polymer Matrix on the Optical Properties of Bioinspired Fluorescent Polymers Containing Diketopyrrolopyrrole Chromophores","authors":"Xin Wei, Hang Zhang, Mingfeng Wang","doi":"10.1021/acsapm.4c00930","DOIUrl":"https://doi.org/10.1021/acsapm.4c00930","url":null,"abstract":"Biodegradable and fluorescent polymer materials have attracted growing research interests due to their tunable properties and various applications such as bioimaging and photonic information technologies. Fluorescent materials obtained by physically blending polymers with organic fluorophores often face the problems of aggregation-caused quenching (ACQ) and photobleaching. We previously reported a series of bioinspired fluorescent polymers covalently linked with a single fluorophore in the middle of each polymer chain, reminiscent of the structure of fluorescent proteins. However, the impact of polymer matrices on the optical properties of these fluorescent polymers remains poorly understood. In this article, we report the influences of different polyesters, containing a common fluorophore of a red fluorescent diketopyrrolopyrrole (DPP) derivative in the middle of each polymer chain, on the optical absorption, fluorescence, and photostability of these polymers in different states, including dilute solutions in a good solvent such as tetrahydrofuran, colloidal nanoparticles in water, and solid films. We further demonstrate the applications of these polymers in the form of colloidal nanoparticles as contrast agents for the fluorescence bioimaging of cells.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141521113","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}
Epoxy resins coming from biobased bisphenols have received significant attention; however, thymol-derived bisphenol epoxies are still essentially unknown so far. Here, a biobased bisphenol E (DHPF) intermediate was obtained from thymol and acetaldehyde via a highly efficient approach, followed by O-glycidylation to afford a bisphenol E epoxy monomer (DHEP) with a viscosity of only 3.5 Pa·s at 60 °C identical to that of a bisphenol A epoxy (DGEBA). Using 4,4′-diaminodiphenyl sulfone (44DDS) and methyltetrahydrophthalic anhydride (MTHPA) as curatives, cured DHEP thermosets were prepared through cast molding, and their properties are systematically studied and compared with DGEBA thermosets. DHEP delivers a lower dielectric constant to the resulting thermosets, especially for DHEP/MTHPA (1.9, 10 MHz). The DHEP-based thermoset also exhibits decreased water absorption, density, and thermal diffusivity and improved resistance to hygrothermal aging as indicated by storage modulus and Tg retention, and good bulk mechanical properties. Moreover, when formulated into an epoxy adhesive for bonding stainless steel sheets, DHEP endows the glue joint with a rather high lap shear strength up to 12.7 MPa. Overall, DHPF can be readily prepared in large quantities, and DHEP is potentially 100% biobased with good processability; the finalized DHEP thermosets have advantages in many properties of high interest, thereby illustrating its good prospects for real applications.
{"title":"Scalable Synthesis of Thymol-Based Bisphenol E Epoxy Monomer and Related Thermosets with Low Dielectric Constant and Density and Improved Resistance to Hygrothermal Aging","authors":"Boyang Li, Rongsheng Li, Jinming Hao, Jingkui Cao, Xiaoxuan Duan, Qiang Feng, Peng Xu, Jintao Wan","doi":"10.1021/acsapm.4c01371","DOIUrl":"https://doi.org/10.1021/acsapm.4c01371","url":null,"abstract":"Epoxy resins coming from biobased bisphenols have received significant attention; however, thymol-derived bisphenol epoxies are still essentially unknown so far. Here, a biobased bisphenol E (DHPF) intermediate was obtained from thymol and acetaldehyde via a highly efficient approach, followed by O-glycidylation to afford a bisphenol E epoxy monomer (DHEP) with a viscosity of only 3.5 Pa·s at 60 °C identical to that of a bisphenol A epoxy (DGEBA). Using 4,4′-diaminodiphenyl sulfone (44DDS) and methyltetrahydrophthalic anhydride (MTHPA) as curatives, cured DHEP thermosets were prepared through cast molding, and their properties are systematically studied and compared with DGEBA thermosets. DHEP delivers a lower dielectric constant to the resulting thermosets, especially for DHEP/MTHPA (1.9, 10 MHz). The DHEP-based thermoset also exhibits decreased water absorption, density, and thermal diffusivity and improved resistance to hygrothermal aging as indicated by storage modulus and <i>T</i><sub>g</sub> retention, and good bulk mechanical properties. Moreover, when formulated into an epoxy adhesive for bonding stainless steel sheets, DHEP endows the glue joint with a rather high lap shear strength up to 12.7 MPa. Overall, DHPF can be readily prepared in large quantities, and DHEP is potentially 100% biobased with good processability; the finalized DHEP thermosets have advantages in many properties of high interest, thereby illustrating its good prospects for real applications.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141531419","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}
Simon van Hurne, Sagar Kumar Raut, Maarten Marinus Johannes Smulders
With an ever-increasing annual production of polymers and the accumulation of polymer waste leading to progressively adverse environmental consequences, it has become important that all polymers can be efficiently recycled at the end of their life cycle. Especially thermosets are intrinsically difficult to recycle because of their permanent covalent cross-links. A possible solution is to switch from using thermosets to covalent adaptable networks, sparking the rapid development of novel dynamic covalent chemistries and derived polymer materials. Next to development of these innovative polymer materials, there is also an evident advantage of merging the virtues of covalent adaptable networks with the proven material properties of widely used commodity plastics, by introducing dynamic covalent bonds in these original thermoplastic materials to obtain recyclable thermosets. Here we report the synthesis and characterization of a polystyrene polymer, functionalized with TetraAzaADamantanes and cross-linked with dynamic covalent boronic esters. The material properties were characterized for different degrees of cross-linking. The materials showed good solvent resistance with a high remaining insoluble fraction. In line with the typical behavior of traditional covalent adaptable networks, the prepared polystyrene-based boronate-TetraAzaADamantane materials were able to undergo stress relaxation. The material relaxation was also shown to be tunable by mixing with an acid catalyst. Lastly, the materials could be recycled at least 2 times.
{"title":"Recyclable Covalent Adaptable Polystyrene Networks Using Boronates and TetraAzaADamantanes","authors":"Simon van Hurne, Sagar Kumar Raut, Maarten Marinus Johannes Smulders","doi":"10.1021/acsapm.4c01633","DOIUrl":"https://doi.org/10.1021/acsapm.4c01633","url":null,"abstract":"With an ever-increasing annual production of polymers and the accumulation of polymer waste leading to progressively adverse environmental consequences, it has become important that all polymers can be efficiently recycled at the end of their life cycle. Especially thermosets are intrinsically difficult to recycle because of their permanent covalent cross-links. A possible solution is to switch from using thermosets to covalent adaptable networks, sparking the rapid development of novel dynamic covalent chemistries and derived polymer materials. Next to development of these innovative polymer materials, there is also an evident advantage of merging the virtues of covalent adaptable networks with the proven material properties of widely used commodity plastics, by introducing dynamic covalent bonds in these original thermoplastic materials to obtain recyclable thermosets. Here we report the synthesis and characterization of a polystyrene polymer, functionalized with TetraAzaADamantanes and cross-linked with dynamic covalent boronic esters. The material properties were characterized for different degrees of cross-linking. The materials showed good solvent resistance with a high remaining insoluble fraction. In line with the typical behavior of traditional covalent adaptable networks, the prepared polystyrene-based boronate-TetraAzaADamantane materials were able to undergo stress relaxation. The material relaxation was also shown to be tunable by mixing with an acid catalyst. Lastly, the materials could be recycled at least 2 times.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141531443","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}
Wearable dry electrodes are the foundation for the development of long-term, real-time biopotential monitoring devices. However, the physiological signals collected by common electrodes often accompany high noise and motion artifacts due to difficulties in conforming to skin deformations and poor contact between electrodes and skin. In contrast to them, PEDOT:PSS-based dry electrodes become a promising material with adjustable stretchability, conductivity, and adhesion properties to achieve high-quality signal delivery. Herein, we report a highly stretchable self-adhesive film prepared by the conductive polymers PEDOT:PSS, ethylene glycol (EG), poly(vinyl alcohol) (PVA), and d-sorbitol (SOR). In the blending system, SOR will disrupt the dense hydrogen bond interactions within PVA and PSS chains, while PEDOT:PSS/PVA physically cross-linked networks can dissipate strain energy, providing toughness to the films. In addition, the hydroxyl groups on the surface enable the film to be self-adhesive by forming hydrogen bonds with the N and O atoms of the skin stratum corneum. The blended electrode exhibits a conductivity of 200 S/cm and an elongation at break of 120%. Moreover, the electrical properties are still maintained after cyclic stretching (R/R0 ≈ 1.09). The maximum adhesion force of the film on glass and skin is 1.20 and 0.36 N/cm, respectively. The electrode has good biocompatibility, and its excellent stretchability and adhesiveness are conducive to comply with the skin deformation under different conditions. The contact impedance between dry electrodes and skin is only 77 kΩ cm2, which ensures the accurate monitoring of physiological signals including electromyogram (EMG) and electrocardiogram (ECG) during rest or exercise. The signal quality is significantly higher than that of standard Ag/AgCl electrodes. This highly stretchable self-adhesive dry electrode provides a feasible idea for the research of next-generation health monitoring devices.
{"title":"Highly Stretchable Self-Adhesive PEDOT:PSS Dry Electrodes for Biopotential Monitoring","authors":"Saiyin Hou, Dong Lv, Yinghan Li, Zonglin Li, Mengmeng Liu, Xinhong Yu, Yanchun Han","doi":"10.1021/acsapm.4c01233","DOIUrl":"https://doi.org/10.1021/acsapm.4c01233","url":null,"abstract":"Wearable dry electrodes are the foundation for the development of long-term, real-time biopotential monitoring devices. However, the physiological signals collected by common electrodes often accompany high noise and motion artifacts due to difficulties in conforming to skin deformations and poor contact between electrodes and skin. In contrast to them, PEDOT:PSS-based dry electrodes become a promising material with adjustable stretchability, conductivity, and adhesion properties to achieve high-quality signal delivery. Herein, we report a highly stretchable self-adhesive film prepared by the conductive polymers PEDOT:PSS, ethylene glycol (EG), poly(vinyl alcohol) (PVA), and <span>d</span>-sorbitol (SOR). In the blending system, SOR will disrupt the dense hydrogen bond interactions within PVA and PSS chains, while PEDOT:PSS/PVA physically cross-linked networks can dissipate strain energy, providing toughness to the films. In addition, the hydroxyl groups on the surface enable the film to be self-adhesive by forming hydrogen bonds with the N and O atoms of the skin stratum corneum. The blended electrode exhibits a conductivity of 200 S/cm and an elongation at break of 120%. Moreover, the electrical properties are still maintained after cyclic stretching (<i>R</i>/<i>R</i><sub>0</sub> ≈ 1.09). The maximum adhesion force of the film on glass and skin is 1.20 and 0.36 N/cm, respectively. The electrode has good biocompatibility, and its excellent stretchability and adhesiveness are conducive to comply with the skin deformation under different conditions. The contact impedance between dry electrodes and skin is only 77 kΩ cm<sup>2</sup>, which ensures the accurate monitoring of physiological signals including electromyogram (EMG) and electrocardiogram (ECG) during rest or exercise. The signal quality is significantly higher than that of standard Ag/AgCl electrodes. This highly stretchable self-adhesive dry electrode provides a feasible idea for the research of next-generation health monitoring devices.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141531422","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}
Lithium–sulfur (Li–S) batteries, possessing substantial capacity, present a promising successor to current lithium-ion batteries, but the “shuttle effect” during cycling and deficient lithium-ion conductivity in Li–S batteries limit their practical applications. One potential remedy to these issues lies in the use of functional binders. In this study, building on the exceptional electrochemical stability of poly(vinylidene fluoride) (PVDF), we strategically grafted the cationic monomer 1-butyl-3-vinylimidazole with bis(trifluoromethanesulfonyl)imide (TFSI–) coordination from the chain of PVDF, thereby engineering the ionomer binder PVDF-g-(1-butyl-3-vinylimidazolium bis((trifluorompropyl)sulfonyl)imide) (BVIM). Density-functional theory (DFT) calculations affirmed that these cationic polymer branches, possessing a high binding energy with lithium polysulfides (LiPSs), are effective in trapping the LiPSs generated at the cathode. Moreover, while adsorbing LiPSs the TFSI– originally coordinated with the branched chain will be displaced, forming a dynamic small molecule pathway in the cathode that promotes lithium-ion conduction. As a result, Li–S batteries with BVIM binders deliver a persistent reversible capacity of 792.5 mAh g–1 over 250 cycles at a rate of 0.5C. Concurrently, at a high sulfur loading of 5.5 mg cm–2, a specific capacity of 3.3 mAh cm–2 was maintained after 50 cycles at 0.2C.
{"title":"Cationic Polymer Binder for Simultaneously Propelling Ion Transfer and Promoting Polysulfide Conversion in Lithium–Sulfur Batteries","authors":"Yuanhao Shi, Dongxia Li, Xiangfeng Sun, Yuxin Xue, Zhiqi Li, Yulin Fu, Chongxian Luo, Qiong Lin, Xuefeng Gui, Kai Xu","doi":"10.1021/acsapm.4c00668","DOIUrl":"https://doi.org/10.1021/acsapm.4c00668","url":null,"abstract":"Lithium–sulfur (Li–S) batteries, possessing substantial capacity, present a promising successor to current lithium-ion batteries, but the “shuttle effect” during cycling and deficient lithium-ion conductivity in Li–S batteries limit their practical applications. One potential remedy to these issues lies in the use of functional binders. In this study, building on the exceptional electrochemical stability of poly(vinylidene fluoride) (PVDF), we strategically grafted the cationic monomer 1-butyl-3-vinylimidazole with bis(trifluoromethanesulfonyl)imide (TFSI<sup>–</sup>) coordination from the chain of PVDF, thereby engineering the ionomer binder PVDF-<i>g</i>-(1-butyl-3-vinylimidazolium bis((trifluorompropyl)sulfonyl)imide) (BVIM). Density-functional theory (DFT) calculations affirmed that these cationic polymer branches, possessing a high binding energy with lithium polysulfides (LiPSs), are effective in trapping the LiPSs generated at the cathode. Moreover, while adsorbing LiPSs the TFSI<sup>–</sup> originally coordinated with the branched chain will be displaced, forming a dynamic small molecule pathway in the cathode that promotes lithium-ion conduction. As a result, Li–S batteries with BVIM binders deliver a persistent reversible capacity of 792.5 mAh g<sup>–1</sup> over 250 cycles at a rate of 0.5C. Concurrently, at a high sulfur loading of 5.5 mg cm<sup>–2</sup>, a specific capacity of 3.3 mAh cm<sup>–2</sup> was maintained after 50 cycles at 0.2C.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141505845","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}
Yun Chen, Boxue Du, Rundong Xue, Yunqi Xing, Xiaoxiao Kong
The poor interfacial adhesion between aramid fiber and epoxy resin is the main issue affecting the dielectric properties of the aramid fiber-reinforced composite (AFRC). In this paper, the bioinspired polydopamine (PDA) coating method is used to modify the aramid fiber surface, which is already activated by plasma treatment. Various aramid fiber/epoxy composite samples are prepared, and the effects of the PDA concentration on the dielectric properties are studied. It is indicated that the interfacial bonding strength between the fiber and epoxy resin could be improved, thus contributing to higher mechanical strength and enhanced dielectric properties. Results show that the DC conductivity, dielectric constant and integration charge Q(t) of the modified composites are significantly reduced, while the dielectric breakdown strength is increased. Under an optimized dopamine concentration of 2 g/L, the breakdown strength is enhanced by 25.1%, while the charge accumulation rate is decreased by 46.5%. Meanwhile, the interfacial shear strength of the composite is increased from 29.5 to 65.2 MPa, showing great application potential in high voltage power equipment.
{"title":"Polydopamine-Enabled Surface Modification to Improve the Dielectric Property of Aramid Fiber/Epoxy Composites for Insulation Rod","authors":"Yun Chen, Boxue Du, Rundong Xue, Yunqi Xing, Xiaoxiao Kong","doi":"10.1021/acsapm.4c00914","DOIUrl":"https://doi.org/10.1021/acsapm.4c00914","url":null,"abstract":"The poor interfacial adhesion between aramid fiber and epoxy resin is the main issue affecting the dielectric properties of the aramid fiber-reinforced composite (AFRC). In this paper, the bioinspired polydopamine (PDA) coating method is used to modify the aramid fiber surface, which is already activated by plasma treatment. Various aramid fiber/epoxy composite samples are prepared, and the effects of the PDA concentration on the dielectric properties are studied. It is indicated that the interfacial bonding strength between the fiber and epoxy resin could be improved, thus contributing to higher mechanical strength and enhanced dielectric properties. Results show that the DC conductivity, dielectric constant and integration charge <i>Q</i>(<i>t</i>) of the modified composites are significantly reduced, while the dielectric breakdown strength is increased. Under an optimized dopamine concentration of 2 g/L, the breakdown strength is enhanced by 25.1%, while the charge accumulation rate is decreased by 46.5%. Meanwhile, the interfacial shear strength of the composite is increased from 29.5 to 65.2 MPa, showing great application potential in high voltage power equipment.","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":null,"pages":null},"PeriodicalIF":5.0,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141520877","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}
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