Changping Wang , Xin Gao , Zhan Li , Xinyu Wang , Yiwen Li , Yiyun Cheng
{"title":"Fluorous-tagged bortezomib supramolecular nanomedicine for cancer therapy","authors":"Changping Wang , Xin Gao , Zhan Li , Xinyu Wang , Yiwen Li , Yiyun Cheng","doi":"10.1016/j.supmat.2024.100080","DOIUrl":"10.1016/j.supmat.2024.100080","url":null,"abstract":"<div><div>Lipidation is a well-established post-translational modification strategy to modulate the structure and function of proteins and peptides. Lipids can improve the overall or local hydrophobicity of the biomolecule, boosting its affinity with the cell membranes. Lipidation, despite its great potential, remains an underutilized technique for translating bioactive molecules into the clinic. Herein, we have optimized the lipidation strategy by involving the fluorous lipidation combined with supramolecular engineering, which can be facilely achieved by grafting an anticancer peptide drug (bortezomib, BTZ) with a series of fluorous lipids bearing a catechol moiety <em>via</em> the dynamic catechol-boronate ester bond. Compared with BTZ, the fluorous-tagged BTZ nanomedicine exhibited an on-demand and traceless release behavior, and enhanced therapeutic effect and biocompatibility. More importantly, the fluorous tag could improve the serum stability of the supramolecular nanomedicine, which allowed efficient <em>in vivo</em> utilization of BTZ to kill cancer cells. This work introduces a novel lipidation strategy for bioactive peptides <em>via</em> the integration of fluorination chemistry and supramolecular engineering strategies.</div></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100080"},"PeriodicalIF":0.0,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142744028","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junxiao Qiu , Hude Ma , Mutian Yao , Manting Song , Liping Zhang , Jingkun Xu , Ximei Liu , Baoyang Lu
{"title":"Design of a supersoft, ultra-stretchable, and 3D printable hydrogel electrical bioadhesive interface for electromyography monitoring","authors":"Junxiao Qiu , Hude Ma , Mutian Yao , Manting Song , Liping Zhang , Jingkun Xu , Ximei Liu , Baoyang Lu","doi":"10.1016/j.supmat.2024.100079","DOIUrl":"10.1016/j.supmat.2024.100079","url":null,"abstract":"<div><div>Electromyography (EMG) monitoring has been extensively employed for critical applications in medicine, sports science, and rehabilitation. However, the mechanical mismatch between conventional EMG electrodes and the skin can lead to electrode detachment upon significant skin deformation. To address this limitation, we develop a PEDOT:PSS-based hydrogel electrical bioadhesive interface (EBI) that incorporates molecular doping and robust adhesion strategies to achieve excellent mechanical compatibility with biological tissues. This hydrogel EBI is fabricated using direct writing of printable inks followed by in-situ thermal initiation, enabling the creation of customizable patterns with high shape fidelity. The resultant 3D-printed PEDOT:PSS-based hydrogel EBI exhibits supersoft properties (Young's modulus 5–8.5 kPa), ultra-stretchability (1175 % strain), robust adhesion (>133 kPa), and outstanding electrochemical performance (CIC reduction by 0.45 % over 1,000,000 cycles). Additionally, we further develop a PEDOT:PSS-based hydrogel electrode specifically for stable EMG signal recording. This electrode outperforms superior signal-to-noise ratio (SNR) performance compared to commercial electrodes in EMG monitoring.</div></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100079"},"PeriodicalIF":0.0,"publicationDate":"2024-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142703232","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kunpeng Ma , Hongyu Yi , Yifan Gao , Yang Cao , Kongyu Ge , Ting Kuang , Hongjun Ji , Mingyu Li , Huanhuan Feng
{"title":"High-sensitivity and damage redundant detection capable gel-state [BMIM][BF4] electronic skin for aerospace applications","authors":"Kunpeng Ma , Hongyu Yi , Yifan Gao , Yang Cao , Kongyu Ge , Ting Kuang , Hongjun Ji , Mingyu Li , Huanhuan Feng","doi":"10.1016/j.supmat.2024.100077","DOIUrl":"10.1016/j.supmat.2024.100077","url":null,"abstract":"<div><div>Electronic skin (e-skin) holds significant potential for applications in robotics, Internet-of-things, and health monitoring. However, conventional e-skins often exhibit decreased sensitivity and delayed response in ultra-low temperature environments due to the freezing of conductive materials. Moreover, an increased brittleness can cause substrate damage, limiting their application in cryogenic conditions. To address existing challenges, an ionic liquid [BMIM][BF<sub>4</sub>] is cross-linked with N,N'-Bis(2-hydroxyethyl)oxamide to form an ionic gel for this study. The gel exhibits excellent electrical performance at −71 °C, significantly expanding the operating temperature range of e-skins. Additionally, gelation decreases resistive drift and leakage inherent to ionic liquids. The prepared sensing units demonstrate high sensitivity to pressure loading across an ultra-wide temperature range of −50–50 °C, with linear sensing within the range of 48–32,000 Pa and a rapid response time of 0.05 s. Integration of the units into large-scaled e-skin enables precise recognition of static and dynamic pressure loads in ultra-low temperature environments (−50 °C). Furthermore, a space glove model assembled using the sensing units achieves accurate recognition of hand gestures in extreme conditions. The sensing units retain over 60 % of their pressure response even when damaged, and demonstrate resilience to environmental factors including low temperatures and vacuum conditions. Along with exceptional performance and environmental resilience under harsh conditions, the gel-state [BMIM][BF<sub>4</sub>] e-skin shows great potential in deep space exploration, polar expeditions, and other challenging environments.</div></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100077"},"PeriodicalIF":0.0,"publicationDate":"2024-11-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142703231","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Poly[2]catenanes-based hydrogels prepared by hydroxyl-yne click chemistry","authors":"Jinsa Li, Ziqing Hu, Hanwei Zhang, Xiaofan Ji","doi":"10.1016/j.supmat.2024.100076","DOIUrl":"10.1016/j.supmat.2024.100076","url":null,"abstract":"<div><div>Polycatenanes as a typical type of mechanically interlocked polymers (MIP), composing of some interlocked cycles through topology bonding has been extensively investigated. However, the comprehension regarding polycatenanes-based materials still lags behind other kinds of MIP. Therein, polyrotaxanes and slide-ring gels were able to fabricate in water to produce hydrogel. Hydrogel materials play an important role in tissue engineering, cell culture, flexible devices and other fields because of their softness and good biocompatibility. However, there was rare reports concerning polycatenanes-based hydrogels. Here, we prepared poly[2]catenanes-based hydrogel <strong>G12</strong> incorporating hydrogen bonds through hydroxyl‑yne click reactions from <strong>M1</strong> and <strong>M2</strong>. Comparative tests of substituting <strong>M2</strong> with <strong>M3</strong> involving mechanical bonds only, hydrophobic alkyl diols <strong>M4</strong> and hydrophilic ethylene glycol <strong>M5</strong> demonstrated that the mechanical bonds and hydrogen bonds could significantly enhance the hydrogel properties. Besides, temperature and acid responsiveness of <strong>G12</strong> was elucidated.</div></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100076"},"PeriodicalIF":0.0,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142703230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Dynamic covalent epoxy network of hyperbranched-synergistic-supramolecular: Catalyst-free reprocessing, and application in carbon fiber composites recycling","authors":"Yueran He, Yanlin Liu, Zhen Yu, Xiangyu Zhou, Jin Zhu, Zhaobin Tang","doi":"10.1016/j.supmat.2024.100078","DOIUrl":"10.1016/j.supmat.2024.100078","url":null,"abstract":"<div><div>Plastic recycling, especially the recycling of thermosets, is a crucial step towards improving waste management and achieving economic recycling. Here, a method utilizing non-covalent supramolecular interactions and synergistic hyperbranched structures is reported to endow transesterification-based thermosetting materials with recyclability in the absence of a catalyst. A hyperbranched epoxy resin curing agent (HPCA) containing amide bonds, terminated by amine and ester, was designed and synthesized, and further cured with bisphenol A epoxy resin. The hyperbranched topological structure and its abundant amide bonds contribute to the formation of a dense hydrogen bonding network, enhancing the reprocessability, thermal, and mechanical properties of the material. As a result, the resin can be reprocessed by hot pressing at 190 °C and 10 MPa for 40 min without catalyst. Moreover, amide and ester bonds endow resin materials with excellent degradation performance in alkaline solutions, laying the foundation for the recycling and utilization of carbon fibers in composite materials.</div></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100078"},"PeriodicalIF":0.0,"publicationDate":"2024-10-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142586696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Andrey I. Koptyaev , Ekaterina D. Rychikhina , Yury A. Zhabanov , Vlad V. Travkin , Georgy L. Pakhomov
{"title":"Optical absorption of supramolecular aggregates of vanadyl etioporphyrin-III in solutions and thin films","authors":"Andrey I. Koptyaev , Ekaterina D. Rychikhina , Yury A. Zhabanov , Vlad V. Travkin , Georgy L. Pakhomov","doi":"10.1016/j.supmat.2024.100075","DOIUrl":"10.1016/j.supmat.2024.100075","url":null,"abstract":"<div><div>Relative abundance of vanadyl etio-porphyrin-III, VO-EtioP-III, a typical geoporphyrin, reaches its maximum in solid fossil fuels (coals). This determines the interest in studying supramolecular structure and solid-state properties of this compound. Unlike planar etio-type porphyrins, the visible absorption spectra of VO-EtioP-III undergo significant transformation in transition from a solution to solid films, which is associated with formation of supramolecular aggregates. In this work, we compare the spectra of VO-EtioP-III films deposited by thermal evaporation of powder in vacuum (VTE) or by spin-coating of dissolved compound (SC) to prove that they are similar to those observed for binary solutions in which adding water to methanol also initiates aggregation. The absorption spectra of VTE-films are very sensitive to the film thickness and deposition conditions. The spectral studies are supplemented with analysis of the microscopic morphology and conducting properties of the films. While the photoconductivity of solution-processed VO-EtioP-III films suffers due to the inhomogeneity of their structure, the VTE-films behave as good photoconductors with a lateral current response to sunlight up to 10<sup>5</sup>.</div></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100075"},"PeriodicalIF":0.0,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142532399","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Erratum for previously published articles","authors":"","doi":"10.1016/j.supmat.2024.100074","DOIUrl":"10.1016/j.supmat.2024.100074","url":null,"abstract":"","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100074"},"PeriodicalIF":0.0,"publicationDate":"2024-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240524000126/pdfft?md5=9c0127021dd46e93c2b7a99e4d08a010&pid=1-s2.0-S2667240524000126-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141961203","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xiaowei Wang , Boyu Wu , Chen He , Yifan Bai , Chao Gao , Anchao Feng , San H. Thang
{"title":"Versatile preparation of jellyfish-inspired color transition hydrogels via polymerization induced supramolecular geletion (PISG)","authors":"Xiaowei Wang , Boyu Wu , Chen He , Yifan Bai , Chao Gao , Anchao Feng , San H. Thang","doi":"10.1016/j.supmat.2024.100072","DOIUrl":"https://doi.org/10.1016/j.supmat.2024.100072","url":null,"abstract":"<div><p>Supramolecular hydrogels based on host–guest interactions constitute a class of intriguing soft matter and have attracted great attention due to their unique properties, etc. In this study, we successfully synthesized 4-methylene-7-diethylaminocoumarin methacrylate (DEACMMA) monomer and carried out reversible addition-fragmentation chain transfer (RAFT) polymerization using methylated <em>β</em>-cyclodextrin via a host-guest encapsulation mechanism. This process led to the formation of ternary copolymer hydrogel supramolecular photoresponsive hydrogels through polymerization induced supramolecular gelation (PISG). The encapsulation of coumarin monomers by methylated cyclodextrins was confirmed using 2D ROESY NMR and fluorescence spectroscopy. We have carefully analyzed the microstructure of these supramolecular hydrogels by rheological profiles and scanning electron microscopy (SEM). Stimulated by UV light, the copolymers transition from non-luminescence to a bright fluorescent blue color, which is reminiscent of the self-transforming colors observed in jellyfish. The development of photostimuli-responsive hydrogels based on methylated <em>β</em>-cyclodextrin-coated coumarin esters opens new avenues in the fields of smart materials and clinical medicine.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100072"},"PeriodicalIF":0.0,"publicationDate":"2024-05-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240524000102/pdfft?md5=b10d7130ebe87cac6f8822cbe22b865d&pid=1-s2.0-S2667240524000102-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140950154","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wei Huang , Xuan Nie , Xiao-Hong Zhou , Lei Qiao , Hong-Jie Gao , Jing Zang , Long-Kang Yu , Long-Hai Wang , Ye-Zi You
{"title":"Phosphatidylserine-targeting bis(zinc-dipicolylamine) farnesol inhibits ATP production in cancer cells to overcome multidrug resistance","authors":"Wei Huang , Xuan Nie , Xiao-Hong Zhou , Lei Qiao , Hong-Jie Gao , Jing Zang , Long-Kang Yu , Long-Hai Wang , Ye-Zi You","doi":"10.1016/j.supmat.2024.100068","DOIUrl":"10.1016/j.supmat.2024.100068","url":null,"abstract":"<div><p>Multidrug resistance significantly impedes the efficacy of cancer chemotherapy. Resistance often arises from the reduced cellular uptake of chemotherapeutic drugs, a process crucial for their cytotoxic effects. This reduction is frequently due to transmembrane efflux pumps powered by ATP from mitochondria and the cytoplasmic matrix, leading to lower intracellular concentrations of these drugs. This study introduces an amphiphilic molecule, bis(zinc-dipicolylamine) farnesol (Bis-ZnDPA), which targets phosphatidylserine (PS) – a negatively charged phospholipid prominently displayed on the outer leaflet of cancer cell plasma membranes. Integrating the hydrophobic segment of Bis-ZnDPA into the plasma membrane disrupts its integrity, potentially leading to hole formation and facilitating the uptake of chemotherapeutic drugs. Furthermore, the binding of Bis-ZnDPA to phosphatidylserine inhibits ATP production caused by Ca<sup>2+</sup> influx and deregulation of the phosphoinositide 3-kinase/protein kinase B (PI3K/AKT) signaling pathway, reducing the efflux of drugs from cells. The results indicate the potent synergistic effect of Bis-ZnDPA with chemotherapeutic agents, suggesting that targeting PS is a viable strategy for overcoming multidrug resistance in cancer chemotherapy.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100068"},"PeriodicalIF":0.0,"publicationDate":"2024-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240524000060/pdfft?md5=9e33a692665c2f861924388c7f5e6efd&pid=1-s2.0-S2667240524000060-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140762684","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Stretchable and self-healable lithium-ion batteries with all-in-one configuration","authors":"Zhen Li, Yue Guo, Xiaokong Liu","doi":"10.1016/j.supmat.2024.100073","DOIUrl":"10.1016/j.supmat.2024.100073","url":null,"abstract":"<div><p>Stretchable lithium-ion batteries (LIBs) are highly desirable to serve as the power sources of stretchable and wearable electronic devices. Furthermore, endowing stretchable LIBs with self-healability can prolong their life-time and enhance their reliability. However, previously reported self-healable LIBs were flexible rather than stretchable, while the stretchable LIBs were unable to self-heal. Herein, we present a novel strategy to fabricate stretchable and self-healable LIBs with all-in-one configuration, by exploiting dynamic covalent polymers as both the electrolyte and the binder of electrodes. The developed polymer electrolyte exhibits a room-temperature ionic conductivity as high as 3.6 × 10<sup>−4</sup> S cm<sup>−1</sup> and possesses an elongation-at-break of 250 ± 30 %. Moreover, the stretchable electrolyte is highly resilient and its ionic conductivity shows minimal changes at different strains. The electrolyte exhibits an autonomous self-healing property at room temperature, making the cut sample easily recover its original performance. Importantly, the electrolyte and electrodes can be fused together at the interface to construct a healable LIB with all-in-one configuration, through the exchange of the dynamic imine bonds that exist in both the electrolyte and electrodes. As a result, the as-developed LIB possesses an elongation-at-break of 220 ± 20 % and can supply power in the course of stretching and releasing. Furthermore, the cut and then healed LIB can still deliver an average discharge capacity of 126.4 mAh <em>g</em> <sup>−</sup> <sup>1</sup> and steadily provide power for LED. This work offers a new avenue for the development of stretchable and self-healable LIBs for the stretchable and wearable electronic devices.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"3 ","pages":"Article 100073"},"PeriodicalIF":0.0,"publicationDate":"2024-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240524000114/pdfft?md5=e6047ec8ce0539ba5d2f2e3083f5d7e4&pid=1-s2.0-S2667240524000114-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"140761269","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}