{"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}
{"title":"Behavior of supramolecular cross-links formed by host-guest interactions in hydrogels responding to water contents","authors":"Chiharu Ueda , Junsu Park , Kazuya Hirose , Subaru Konishi , Yuka Ikemoto , Motofumi Osaki , Hiroyasu Yamaguchi , Akira Harada , Masaru Tanaka , Go Watanabe , Yoshinori Takashima","doi":"10.1016/j.supmat.2021.100001","DOIUrl":"10.1016/j.supmat.2021.100001","url":null,"abstract":"<div><p>Reversible or movable cross-links based on host-guest interactions in supramolecular materials create functions such as enhanced mechanical properties and stimulus responsiveness. A supramolecular complex on a polymer side chain achieves the described functions as a reversible cross-link. Generally, 1:1 complex is utilized as a cross-link for the host-guest interaction based-supramolecular materials, but herein, the 1:2 complex between γ-cyclodextrin (γCD) and methyl viologen terminated undecyl acrylate (VC11) was chosen to cross-link three polymeric chains. The obtained supramolecular hydrogels γCD-VC11 (<em>x, y</em>) (<em>x</em> and <em>y</em> represent the mol% of the γCD and VC11 units in feeding, respectively) was prepared by radical copolymerization with acrylamide as a mainchain monomer. Tensile test revealed that toughness (<em>G</em><sub>f</sub>) of γCD-VC11 (<em>x, y</em>) maximized at water content (<em>W</em><sub>c</sub>) ≈ 40 wt.%. The maxima of <em>G</em><sub>f</sub> depended on the amount of γCD and VC11 units. Through dynamic mechanical analysis, Arrhenius style plots between horizontal shift factors and temperature determined activation energies (<em>E</em><sub>a</sub>) of each γCD-VC11 (<em>x, y</em>) and MBAAm (0.5). <em>E</em><sub>a</sub> of MBAAm (0.5) monotonically decreased with the increasing <em>W</em><sub>c</sub>. On the other hand, slope of <em>E</em><sub>a</sub> of γCD-VC11 (<em>x, y</em>) changed at <em>W<sub>c</sub></em> ≈ 40 wt.%. Simultaneously considering results of the tensile tests and DMA, the reversible cross-links formed by γCD and VC11 in γCD-VC11 (<em>x, y</em>) function effectively at appropriate <em>W</em><sub>c</sub>.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100001"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240521000015/pdfft?md5=20b04e0ce750dfaac2878b1832c00da9&pid=1-s2.0-S2667240521000015-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"73176122","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":"Multicolor fluorescent supramolecular adhesive gels based on a single molecule with aggregation-induced ratiometric emission","authors":"Hanwei Zhang, Hui Liu, Ziqing Hu, Xiaofan Ji","doi":"10.1016/j.supmat.2022.100018","DOIUrl":"10.1016/j.supmat.2022.100018","url":null,"abstract":"<div><p>Multicolor fluorescent materials, showing various fluorescent colors at the same time, have been applied in biomimetic materials, sensor arrays, and information storage. However, the vast majority of present multicolor fluorescent materials were prepared within a complicated as well as costly process, which was achieved by incorporating a variety of fluorophores. Herein, we designed multicolor fluorescent supramolecular adhesive gels (<strong>MSAGs</strong>) based on single pyrene benzohydrazonate (PBHZ) fluorophore. When the concentration of PBHZ groups was adjusted, the gel blocks that make up <strong>MSAGs</strong> exhibited distinct fluorescence colors ranging from blue to bright green due to the aggregation-induced ratiometric emission (AIRE) effect. In addition, as a consequence of 2-ureido-4-pyrimidone (UPy) units containing in the gel blocks, <strong>MSAGs</strong> could be facilely obtained through interfacial supramolecular adhesion between these gel blocks. Moreover, the resulting <strong>MSAGs</strong> with various patterns showed superiority in applying to encrypt multiple information.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100018"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2667240522000113/pdfft?md5=87708a97f89dec8400f27c02ed99f10c&pid=1-s2.0-S2667240522000113-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"79409449","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}
Yang Yang , Zhiqin Xia , Yuzheng Luo , Zhanpeng Wu , Shaowei Shi , Thomas P. Russell
{"title":"Reconfigurable structured liquids","authors":"Yang Yang , Zhiqin Xia , Yuzheng Luo , Zhanpeng Wu , Shaowei Shi , Thomas P. Russell","doi":"10.1016/j.supmat.2022.100013","DOIUrl":"https://doi.org/10.1016/j.supmat.2022.100013","url":null,"abstract":"<div><p>The past decades have witnessed the discovery and rapid development of adaptable, reconfigurable all-liquid systems where, by the interfacial assembly and jamming of nanoparticles (NPs), a liquid-liquid system can be structured, i.e., locked into a highly non-equilibrium spatial arrangement, maintaining all the inherent characteristics of the liquids but having the spatial organization and structural stability of a solid. Due to the nature of the interfacial jamming, external stimuli can be used to re-shape the liquids, imparting a responsiveness and malleability to the constructs. In general, the binding energy of a NP to the interface is small, so that compressive forces associated with the reduction in the interfacial area to minimize energy, are sufficient to expel the NPs from the interface. By generating nanoparticle surfactants (NPSs), where ligands dissolved in one liquid can interfacially interact with NPs dispersed in a second immiscible liquid, the binding energy of the NP is massively increased, enabling an interfacial jamming of the NPSs and an arresting of shape changes. Since the jamming is immune to the nature of the NPs, advantage can be taken of the inherent functionality of the NPs, e.g., catalytic, enzymatic, optical, electronic or magnetic, while chemical functionality, including selective functional group recognition, can be introduced through the ligands comprising the NPSs. NPS assemblies can be realized at the interface between any two immiscible liquids (oil-water, oil-oil, and water-water), underscoring the generality of this concept and the range of potential applications. Here, we review some of the basic principles underlying the formation of NPSs and the structuring of liquids, using examples drawn from work in our laboratories and elsewhere, and we provide a perspective on where challenges and applications of this unique state of matter exist.</p></div>","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"1 ","pages":"Article 100013"},"PeriodicalIF":0.0,"publicationDate":"2022-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S266724052200006X/pdfft?md5=f60dcc68baf161fe68ec5a691ae59c8d&pid=1-s2.0-S266724052200006X-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136553697","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":"","PeriodicalId":101187,"journal":{"name":"Supramolecular Materials","volume":"25 21 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"88874967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}