Spherical colloidal particles generally self-assemble into hexagonal lattices in two dimensions. However, more complex, non-hexagonal phases have been predicted theoretically for isotropic particles with a soft repulsive shoulder but have not been experimentally realized. We study the phase behavior of microspheres in the presence of poly(N-isopropylacrylamide) (PNiPAm) microgels at the air/water interface. We observe a complex phase diagram, including phases with chain and square arrangements, which exclusively form in the presence of the microgels. Our experimental data suggests that the microgels form a corona around the microspheres and induce a soft repulsive shoulder that governs the self-assembly in this system. The observed structures are fully reproduced by both minimum energy calculations and finite temperature Monte Carlo simulations of hard core-soft shoulder particles with experimentally realistic interaction parameters. Our results demonstrate how complex, anisotropic assembly patterns can be realized from entirely isotropic building blocks by control of the interaction potential.
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http://dx.doi.org/10.1021/jacs.7b08503 | DOI Listing |
PLoS Comput Biol
January 2025
Genesupport, Avenue de Sévelin 18, Lausanne, Switzerland.
Catalysis and specifically autocatalysis are the quintessential building blocks of life. Yet, although autocatalytic networks are necessary, they are not sufficient for the emergence of life-like properties, such as replication and adaptation. The ultimate and potentially fatal threat faced by molecular replicators is parasitism; if the polymerase error rate exceeds a critical threshold, even the fittest molecular species will disappear.
View Article and Find Full Text PDFACS Nano
January 2025
College of Chemistry Chemical Engineering and Materials Science, Shandong Normal University, Jinan, Shandong 250014, China.
Coastal/offshore renewable energy sources combined with seawater splitting offer an attractive means for large-scale H electrosynthesis in the future. However, designing anodes proves rather challenging, as surface chlorine chemistry must be blocked, particularly at high current densities (). Additionally, waste seawater with increased salinity produced after long-term electrolysis would impair the whole process sustainability.
View Article and Find Full Text PDFACS Nano
January 2025
State Key Laboratory of Cardiology and Medical Innovation Center, Shanghai East Hospital, The Institute for Biomedical Engineering & Nano Science, School of Medicine, Tongji University, Shanghai 200092, P. R. China.
Despite significant progress in skin wound healing, it is still a challenge to construct multifunctional bioactive dressings based on a highly aligned protein fiber coated hydrogel matrix for antifibrosis skin wound regeneration that is indistinguishable to native skin. In this study, a "dual-wheel-driven" strategy is adopted to modify the surface of methacrylated gelatin (GelMA) hydrogel with highly aligned magnetic nanocomposites-protein fiber assemblies (MPF) consisting of photothermal responsive antibacteria superparamagnetic nanocomposites-fibrinogen (Fg) complexes as the building blocks. Whole-phase healing properties of the modified hydrogel dressing, GelMA-MPF (GMPF), stem from the integration of Fg protein with RGD peptide activity decorated on the surface of the antibacterial magnetic nanoactuator, facilitating facile and reproducible dressing preparation by self-assembly and involving biochemical, morphological, and biophysical cues.
View Article and Find Full Text PDFACS Synth Biol
January 2025
The Novo Nordisk Foundation Center for Biosustainability, Technical University of Denmark, Kongens Lyngby, 2800, Denmark.
Methyl ketones, key building blocks widely used in diverse industrial applications, largely depend on oil-derived chemical methods for their production. Here, we investigated biobased production alternatives for short-chain ketones, adapting the solvent-tolerant soil bacterium as a host for ketone biosynthesis either by whole-cell biocatalysis or using engineered minicells, chromosome-free bacterial vesicles. Organic acids (acetate, propanoate and butanoate) were selected as the main carbon substrate to drive the biosynthesis of acetone, butanone and 2-pentanone.
View Article and Find Full Text PDFInorg Chem
January 2025
Department of Chemistry, Anhui University, Hefei, Anhui 230601, P. R. China.
Icosahedral gold clusters with high-symmetry geometry and magic electronic shells are potential candidates for cluster-assembling, while their assembling rules are still awaiting further investigation. In this work, we use the all-metal icosahedral M@Au as a building block to assemble a series of bi-, tri-, tetra-, and penta-superatomic molecules with diverse superatomic bonding patterns via face-fusion, aiming to systemically explore the bonding rule of superatoms. Chemical bonding analyses indicate that these bi-, tri-, tetra-, and penta-superatomic molecules [M@Au] (M = Re, W, Ta, Ti, Hf, Ir, and Pt) can be considered electronic analogues to Cl, O, N, CO, O, CO, NCl, and CF molecules with single, double, triple, and multicenter bonds, respectively.
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