{"title":"Multicompartment polymer capsules","authors":"Zhiliang Gao , Xiaomiao Cui , Jiwei Cui","doi":"10.1016/j.supmat.2022.100015","DOIUrl":"10.1016/j.supmat.2022.100015","url":null,"abstract":"<div><p>The creation of nano- or micro-particles with separated domains has generated significant attention in the field of biomedicine, cosmetics, and chemical synthesis. Compared with phospholipid-based multicompartment vesicles, the introduction of polymers into multicompartment capsules can enhance their mechanical stability and broaden their applications. In this review, we highlight recent advances in polymer-based multicompartment capsules, including construction strategies (e.g., self-assembly, layer-by-layer assembly, and emulsion-mediated assembly) as well as their applications (e.g., drug delivery and micro-reactors). In addition, we also summarize the challenges associated with controllability and functionality of multicompartment capsules as well as future directions and developments in the field. This review is expected to help unravel fundamental understandings in artificial cells and guide the design of polymer multicompartment capsules for tailored applications.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100015"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240522000083/pdfft?md5=eb5f23834efd3d805754c533b3271641&pid=1-s2.0-S2667240522000083-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79978222","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":"Engineering coacervate droplets towards the building of multiplex biomimetic protocells","authors":"Hua Wu , Yan Qiao","doi":"10.1016/j.supmat.2022.100019","DOIUrl":"https://doi.org/10.1016/j.supmat.2022.100019","url":null,"abstract":"<div><p>The origin of life on Earth remains one of the biggest open questions in science. Despite recent advances in molecular mechanism of cell biology, a large blind spot still exists between non-living matter and the emergence of life which cannot be filled by biology alone. The quest to comprehend the cell origin inspires the construction of synthetic analogs (protocells) to mimic their life-like functionality and structural complexity. Among all kinds, coacervates formed by liquid-liquid phase separation featured by their dynamic structure, molecularly crowded interior and molecular sequestration capability, have been regarded as a protocell model for exploring the origin of life. Their biological counterparts in natural cells are also found to facilitate subcellular organization and spatiotemporal regulation of biological molecules. In this tutorial review, we summarize the recent progress on engineering coacervate protocells to potentially reproduce the function and structure of primitive life by multiphase organization, membranization and structural hybridization. Routes to high-ordered protocellular system comprising spatially arranged coacervates, as well as to the construction of tissue-like structures are also described. Finally, we deduce some perspectives of coacervate engineering in the direction of the emergence of life, from molecular scale to the emergence of integrated multicellular system.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100019"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240522000125/pdfft?md5=900a8735b5af9a45e2c13e35e9e59f82&pid=1-s2.0-S2667240522000125-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"72280167","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}
Yuanxi Liu , Peidong Du , Qiao Teng , Hao Sun , XiangYu Ye , Zhen-Gang Wang
{"title":"Self-assembly of fibril-forming histidine-rich peptides for cofactor-free oxidase-mimetic catalysis","authors":"Yuanxi Liu , Peidong Du , Qiao Teng , Hao Sun , XiangYu Ye , Zhen-Gang Wang","doi":"10.1016/j.supmat.2022.100012","DOIUrl":"10.1016/j.supmat.2022.100012","url":null,"abstract":"<div><p>Most oxidases rely on the cofactors for catalyzing the electron transfer reactions, while tend to suffer from externally-induced protein unfolding, cofactor dissociation and nonrecovery of the activities. We have previously demonstrated that the self-assembled oligohistidine peptides, without assistance of the heme cofactor, can mimic the catalytic function of the heme-dependent peroxidases that promoted H<sub>2</sub>O<sub>2</sub> reduction reactions. Herein, we conjugate a fibril-forming peptide to the oligohistidine, to guide the self-assembly of the heme-free catalyst into amyloid-like structures, which facilitate the association of the histidine residues. The modified oligohistidine materials are able to catalyze H<sub>2</sub>O<sub>2</sub> reduction reactions efficiently through the formation of reactive ternary complex intermediates, similar to the mechanism to the unmodified oligohistdine, but the catalytic efficiency is over one order of magnitude higher. Moreover, the catalyst can be switched between inactive and active state without loss of activity for more than ten cycles of heating/cooling treatments, and showed selective oxidation of benzidine substrates over phenolic substrates. These results may aid the future design of the robust cofactor-free supramolecular catalysts and support the evolutionary link between the primitive amyloids and modern-day enzymes.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100012"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240522000058/pdfft?md5=c9322c4bba9a0d4b8dd4bac06f650569&pid=1-s2.0-S2667240522000058-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79742597","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}
Yukun Jian , Baoyi Wu , Xuxu Yang , Yu Peng , Dachuan Zhang , Yang Yang , Huiyu Qiu , Huanhuan Lu , Jiawei Zhang , Tao Chen
{"title":"Stimuli-responsive hydrogel sponge for ultrafast responsive actuator","authors":"Yukun Jian , Baoyi Wu , Xuxu Yang , Yu Peng , Dachuan Zhang , Yang Yang , Huiyu Qiu , Huanhuan Lu , Jiawei Zhang , Tao Chen","doi":"10.1016/j.supmat.2021.100002","DOIUrl":"10.1016/j.supmat.2021.100002","url":null,"abstract":"<div><p>With the ability to deform in response to specific stimuli, polymeric hydrogel actuators are important bionic materials. However, because shape deformation is derived from the diffusion of water molecules, the response rate of hydrogel actuators is usually slow, which severely limits their potential applications. In this work, a thermo-responsive PNIPAm hydrogel sponge is developed, and the hydrogel sponge shows ultrafast de-swelling/swelling capacity (equilibrium time 7 s) and large deformation degree (40%) due to the assistance of capillary force. Hydrogel sponge actuator with rapid response performance is further constructed, and the hydrogel sponge actuator could be used to capture moving objects and living creatures. Moreover, light-controlled directional movement can be achieved by incorporating photothermal functional components into the hydrogel sponge actuator. This work would promote the application of hydrogel actuators in soft robots.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100002"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240521000027/pdfft?md5=2740fa7c5da8f7236805e676d7169404&pid=1-s2.0-S2667240521000027-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79079997","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":"Supramolecular microgels/microgel scaffolds for tissue repair and regeneration","authors":"Kai Wang, Zhaoyi Wang, Haijun Hu, Changyou Gao","doi":"10.1016/j.supmat.2021.100006","DOIUrl":"10.1016/j.supmat.2021.100006","url":null,"abstract":"<div><p>Biomedical microgels are a novel type of materials with promising perspectives for repair and regeneration of multi-types of tissues and organs due to their highly hydrated nature, tunable microporous structure, ability to encapsulate bioactive factors, and tailorable properties such as stiffness and composition. In particular, the reversible bonding in supramolecular microgels leads to their ease of injectability and self-healing ability, which are essential for therapeutic delivery of cells and drugs, assembly to generate scaffolds, and bioinks for 3D printing. <em>In vivo</em> studies of microgels have pioneered the clinical relevance of these novel and innovative materials for regenerative medicine. In this review, the important supramolecular interactions such as hydrogen bonding, ionic bonding, and host-guest and hydrophobic interactions, and metal coordination are summarized with respect to the formation of supramolecular microgels for biomedical applications, highlighting their advantages over the traditional bulk ones. The applications of supramolecular microgels in the fields of cardiac tissue repair, osteoarthritis therapy, and bone and neuronal tissue engineering are discussed.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100006"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240521000064/pdfft?md5=6173a8fc8e74a873a7ddfeed58000f18&pid=1-s2.0-S2667240521000064-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"91499568","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":"Light-induced assembly of colloidal nanoparticles based on photo-controlled metal–ligand coordination","authors":"Xiaolong Zeng , Yannick Nyquist , Qijin Zhang , Hans-Jürgen Butt , Si Wu","doi":"10.1016/j.supmat.2021.100004","DOIUrl":"10.1016/j.supmat.2021.100004","url":null,"abstract":"<div><p>Self-assembly of colloidal nanoparticles is a promising approach for the fabrication of functional materials. Zeta potential strongly influences the self-assembly processes of nanoparticles. Light-induced zeta potential manipulation provides spatiotemporal resolution. However, current studies on photo-controllable zeta potential are based on ultraviolet (UV) light. In comparison with UV light, visible light is better suited to control the zeta potential of colloidal nanoparticles. In the present study, we applied visible light-responsive ruthenium (Ru) complexes, grafted onto the surface of silica nanoparticles (Ru-SNPs), to control their assembly. The Ru complexes were photoresponsive. Irradiation of Ru-SNPs induced the release of Ru complexes from the nanoparticle surface. The released Ru caused a decrease in the zeta potential of colloidal Ru-SNPs that further changed the assembly behavior and led to the aggregation of Ru-SNPs.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100004"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240521000040/pdfft?md5=14f8a828cdd2800716e72b078177dba4&pid=1-s2.0-S2667240521000040-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"82455507","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}
Junsheng Zhang , Hai Lei , Meng Qin , Wei Wang , Yi Cao
{"title":"Quantifying cation-π interactions in marine adhesive proteins using single-molecule force spectroscopy","authors":"Junsheng Zhang , Hai Lei , Meng Qin , Wei Wang , Yi Cao","doi":"10.1016/j.supmat.2021.100005","DOIUrl":"10.1016/j.supmat.2021.100005","url":null,"abstract":"<div><p>In marine adhesives, cation-π interactions play an important role in their liquid-liquid phase separation process and underlying their strong interfacial bonding. However, it remains challenging to study the strength of cation-π interactions at the single-molecule level. Here, we engineer a recombinant chimeric polyprotein containing the mussel foot proteins-5 (MFP5) and a finger print domain GB1 to unambiguiously quantify the strength of cation-π interactions using atomic force microscopy (AFM)-based single-molecule force spectroscopy. Our results show that the formation of intermolecular cation-π interactions can be triggered at elevated salt concentrations, consistent with previous ensemble studies. Individual cation-π interaction ruptures at about 70 pN at a pulling speed of 1.6 μm s<sup>−1</sup>, comparable to the strength of other non-covalent interactions. The strength of cation-π interactions is weakly dependent on pH, which is in stark contrast with the hydrogen bonding and charge-charge interactions. Moreover, we find that the position of the cation-π bonds are formed randomly along the polyprotein chains. The propensity of forming long range cation-π interactions increases considerably when increasing the pH from 4 to 8, presumably due to the neutralization of the positive changes of MFP5. Our study directly quantifies the mechanical strength of cation-π bonds in the biological relavent settings and reveals key design parameters that may inspire the design of biomimetic strong underwater adhesives.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100005"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240521000052/pdfft?md5=76b77905bf3d11637b83f0e1cd57cb36&pid=1-s2.0-S2667240521000052-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"84334508","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}
Qianhui Cheng , Hetong Fang , Rui Cao , Zhuoyuan Ma , Shun Wang , Renguo Xie , Haibing Xia , Dayang Wang
{"title":"Interfacial self-assembly of nanoparticles into macroscopic, monolayered films","authors":"Qianhui Cheng , Hetong Fang , Rui Cao , Zhuoyuan Ma , Shun Wang , Renguo Xie , Haibing Xia , Dayang Wang","doi":"10.1016/j.supmat.2022.100021","DOIUrl":"https://doi.org/10.1016/j.supmat.2022.100021","url":null,"abstract":"<div><p>This article offers an overview of recent advances in directing self-assembly of nanoparticles (NPs) at the interfaces between two immiscible fluids, which is aimed at emphasizing that the fluidic interfaces can endow NPs with sufficient mobility to minimize far-from-equilibrium effects and thus direct the self-assembly of NPs into monolayered films with single crystalline domains potentially being macroscopically large. It commences with a brief review of the interfacial adsorption behavior of NPs, which plays the central role in interfacial self-assembly of NPs, and the interaction balance between the NPs adsorbing at fluidic interfaces. The following section is an overview of the state-of-the-art of directed self-assembly of nanoparticles at the interfaces between vapor and liquid and between two immiscible liquids. Subsequently, it will focus on several key variables governing the NP self-assembly at the interfaces and elaboration of their impacts on the structural features of the resulting NP monolayered films. Finally, the technical benefits of interfacial NP self-assembly are outlined, followed by an outlook of the upcoming technical challenges and emerging perspectives in the field.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100021"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240522000149/pdfft?md5=1f8dc757713c0ce747edb31bed35b495&pid=1-s2.0-S2667240522000149-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"72280168","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-Pin Huang, Jia-Qi Hu, Hong-Lin Qian, Ke-Feng Ren, Jian Ji
{"title":"Dynamic structural controlment for the functionalization of polyelectrolyte multilayer films","authors":"Wei-Pin Huang, Jia-Qi Hu, Hong-Lin Qian, Ke-Feng Ren, Jian Ji","doi":"10.1016/j.supmat.2022.100016","DOIUrl":"10.1016/j.supmat.2022.100016","url":null,"abstract":"<div><p>Polyelectrolyte multilayer films (PEMs) fabricated from the layer-by-layer (LbL) assembly technique have attracted wide interests in the past several decades. Driven and stabilized by electrostatic interaction, the PEMs are sensitive with the external stimuli, contributing to the dynamic tunability of film structures. Compared with adjusting the film structures during assembled procedures, it is more convenient and flexible to control the physical structures of PEMs employing post-treatments. In this review, the different strategies for effectively regulating PEMs’ structures based on the post-treatment, as well as the functionalization of these prepared structural films are discussed. At last, perspectives are provided for the future development directions, aiming to provide opportunities and a novel pathway for microstructural PEMs.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100016"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240522000095/pdfft?md5=41ada6741b0e3446cd915b54c8090fdf&pid=1-s2.0-S2667240522000095-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"73772234","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}