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In this paper the crystal structure of glycinium tribromidoplumbate(II) (GlyH)PbBr 3 ( I ), where GlyH is a glycinium cation (NH 3 CH 2 COOH), is reported in the orthorhombic space group P 2 1 2 1 2 1 . The tribromidoplumbate anion (PbBr 3 ) − is located in a general position and forms a polymeric 1D-structure. Photoluminescence at ambient conditions using 405 nm laser excitation is observed in the crystal.

Liquid–liquid phase separation (LLPS) phenomena are ubiquitous in biological systems, as various cellular LLPS structures control important biological processes. Due to their ease of in vitro assembly into membraneless compartments and their presence within modern cells, LLPS systems have been postulated to be one potential form that the first cells on Earth took on. Recently, liquid crystal (LC)-coacervate droplets assembled from aqueous solutions of short double-stranded DNA (s-dsDNA) and poly-L-lysine (PLL) have been reported. Such LC-coacervates conjugate the advantages of an associative LLPS with the relevant long-range ordering and fluidity properties typical of LC, which reflect and propagate the physico-chemical properties of their molecular constituents. Here, we investigate the structure, assembly, and function of DNA LC-coacervates in the context of prebiotic molecular evolution and the emergence of functional protocells on early Earth. We observe through polarization microscopy that LC-coacervate systems can be dynamically assembled and disassembled based on prebiotically available environmental factors including temperature, salinity, and dehydration/rehydration cycles. Based on these observations, we discuss how LC-coacervates can in principle provide selective pressures effecting and sustaining chemical evolution within partially ordered compartments. Finally, we speculate about the potential for LC-coacervates to perform various biologically relevant properties, such as segregation and concentration of biomolecules, catalysis, and scaffolding, potentially providing additional structural complexity, such as linearization of nucleic acids and peptides within the LC ordered matrix, that could have promoted more efficient polymerization. While there are still a number of remaining open questions regarding coacervates, as protocell models, including how modern biologies acquired such membraneless organelles, further elucidation of the structure and function of different LLPS systems in the context of origins of life and prebiotic chemistry could provide new insights for understanding new pathways of molecular evolution possibly leading to the emergence of the first cells on Earth.

Cyanobacteria are vital photosynthetic prokaryotes, but some form harmful algal blooms (cyanoHABs) that disrupt ecosystems and produce toxins. The mechanisms by which these blooms form have yet to be fully understood, particularly the role of extracellular components. Here, we present a 2.4 Å cryo-EM structure of a pilus, termed the cyanobacterial tubular (CT) pilus, found in the cyanoHAB-forming Microcystis aeruginosa. The pilin exhibits a unique protein fold, forming a tubular pilus structure with tight, double-layer anti-parallel β-sheet interactions. We show that CT pili are essential for buoyancy by facilitating the formation of micro-colonies, which increases drag force and prevents sinking. The CT pilus surface is heavily glycosylated with ten monosaccharide modifications per pilin. Furthermore, CT pili can enrich microcystin, potentially enhancing cellular resilience, and co-localize with iron-enriched extracellular matrix components. Thus, we propose that this pilus plays an important role in the proliferation of cyanoHABs. This just discovered pilus family appears to be widely distributed across several cyanobacterial orders. Our structural and functional characterization of CT pili provide insights into cyanobacterial cell morphology, physiology, and toxin interactions, and identify potential targets for disrupting bloom formation.

Metal‐coordinated supramolecular nanoassemblies have recently attracted extensive attention as materials for cancer theranostics. Owing to their unique physicochemical properties, metal‐coordinated supramolecular self‐assemblies can bridge the boundary between traditional inorganic and organic materials. By tailoring the structural components of the metal ions and binding ligands, numerous multifunctional theranostic nanomedicines can be constructed. Metal‐coordinated supramolecular nanoassemblies can modulate the tumor microenvironment (TME), thus facilitating the development of TME‐responsive nanomedicines. More importantly, TME‐responsive organic–inorganic hybrid nanomaterials can be constructed in vivo by exploiting the metal‐coordinated self‐assembly of a variety of functional ligands, which is a promising strategy for enhancing the tumor accumulation of theranostic molecules. In this review, recent advancements in the design and fabrication of metal‐coordinated supramolecular nanomedicines for cancer theranostics are highlighted. These supramolecular compounds are classified according to the order in which the coordinated metal ions appear in the periodic table. Furthermore, the prospects and challenges of metal‐coordinated supramolecular self‐assemblies for both technical advances and clinical translation are discussed. In particular, the superiority of TME‐responsive nanomedicines for in vivo coordinated self‐assembly is elaborated, with an emphasis on strategies that enhance the accumulation of functional components in tumors for an ideal theranostic outcome. This review summarizes the recent progress made on metal‐coordinated supramolecular nanomedicines for cancer theranostic by classifying the coordination metal ions in the order of periodic table. Especially, the superiority of the tumor‐responsive nanomedicines for in vivo coordinated self‐assembling cancer theranostic is discussed, with an emphasis on how to realize high nanomedicine accumulation on tumor and therefore ideal theranostic outcome.

Stimuli‐responsive systems play a crucial role in biological processes. Research on supramolecular cages formed via noncovalent interactions contributes to the development of receptors that mimic these natural systems. Recently, anion‐coordination‐driven assembly (ACDA) employing oligourea ligands and trivalent phosphate ions (PO43−) has emerged as a promising strategy for constructing responsive supramolecular architectures. These assemblies are stabilized through multiple hydrogen bonds and are capable of undergoing structural transformations in response to external stimuli, offering a conceptual framework for understanding flexibility and environmental adaptability in biological contexts. This mini‐review highlights the stimuli‐responsive properties of anionic self‐assemblies, with a focus on systems involving oligourea ligands and PO43− ion. Organized by stimulus type, it discusses multistimuli responsiveness, guest‐induced transformations, solvent sensitivity, and light‐responsive behaviors. Current challenges and identifying future opportunities in the study of ACDA‐based stimuli‐responsive systems are discussed. This mini‐review summarizes recent developments in stimuli‐responsive supramolecular assemblies based on anion‐coordination‐driven assembly using oligourea ligands and phosphate anions. The content is organized by stimulus type: multistimuli, guest/template, solvent, and light. This review highlights multistimuli adaptability and structural transformations. Remaining challenges and future directions are also outlined.

Chirality is a fundamental property in nature, which is essential for the existence and survival of living organisms. Smart responsive chiroptical materials have garnered increasing attention due to their unique structural characteristics and potential applications. Among these, azobenzene (Azo), as a typical photoresponsive chromophore, plays a crucial role in constructing and controlling chiral structures. The unique cis‐trans isomerization, liquid crystallinity, and other physicochemical properties allow for a wide range of tunability in stimuli‐responsive chiroptical materials. Herein, we review the research studies in the field of chiral/achiral Azo building blocks for multilevel chiral generation as well as chiral switching, and summarize the recent advances on the applications of the chiral Azo structures from micro to macro levels. Finally, we aim to provide an overview of the potential challenges and new research opportunities for the development of novel smart responsive chiroptical materials. The unique cis‐trans isomerization, liquid crystallinity and other physicochemical properties of azobenzene allow for a wide range of tunability in stimuli‐responsive chiroptical materials, which endows azobenzene chiroptical aggregates with the ability of chirality switches (“on/off,” “inversion” and “amplification” switches) from microscopic to macroscopic scales as well as provides a bright prospect for the further applications of azobenzene chiroptical materials.

Aggregation‐induced emission (AIE) is a phenomenon in which fluorescence is enhanced rather than quenched upon molecular assembly. AIE fluorogens (AIEgens) are flexible, conjugated systems that are limited in their dynamics when assembled, which improves their fluorescent properties. This intriguing feature has been incorporated in many different molecular assemblies and has been extended to nanoparticles composed of amphiphilic polymer building blocks. The integration of the fascinating AIE design principle with versatile polymer chemistry opens up new frontiers to approach and solve intrinsic obstacles of conventional fluorescent materials in nanoscience, including the aggregation‐caused quenching effect. Furthermore, this integration has drawn significant attention from the nanomedicine community, due to the additional advantages of nanoparticles comprising AIEgenic molecules, such as emission brightness and fluorescence stability. In this regard, a range of AIEgenic amphiphilic polymers have been developed, displaying enhanced emission in the self‐assembly/aggregated state. AIEgenic assemblies are regarded as attractive nanomaterials with inherent fluorescence, which display promising features in a biomedical context, for instance in biosensing, cell/tissue imaging and tracking, as well as (photo) therapeutics. In this review, we describe recent strategies for the design and synthesis of novel types of AIEgenic amphiphilic polymers via facile approaches including direct conjugation to natural/synthetic polymers, polymerization, post‐polymerization and supramolecular host−guest interactions. Their self‐assembly behavior and biomedical potential will be discussed. The recent advances in the design and synthesis of AIEgenic amphiphilic polymers are discussed. Their self‐assembly leads to particles with very high fluorescence intensity. The versatility of polymer science allows the creation of a wide variety of particles which show much potential for biomedical applications.

New concept for the development of supramolecular assemblies from intricate interactions between different classes of biomacromolecules (polysaccharides, proteins and lipids) is yet to come, due to their intrinsic chemical and structural complexity and incompatibility. Herein, we report an interaction mechanism among multiple biomacromolecules, and the structural and digestive properties of their assemblies using amylose (AM), lauric acid (LA), and β‐lactoglobulin (βLG) as exemplars. AM, LA, and βLG interact to form a water‐soluble ternary complex through van der Waals forces between AM and LA and high affinity binding between AM and βLG, which can further assemble into uniform‐sized, semi‐crystalline nanospheres under certain thermodynamic conditions. These nanospheres are substantially resistant to amylolysis, thus can be well utilized by gut microbiota, including increasing short‐chain fatty acid levels and shaping bacterial communities. Illustrating the complexation of AM, LA, and βLG and their assemblies from disorder to order, this work offers potential rationale of assemblies for multiple biomacromolecules driven by non‐covalent interactions and substantial potentials for supramolecular biomaterials development. On the basis of revealing the ternary interaction mechanism of multiple biomacromolecules (amylose [AM], lauric acid [LA], and β‐lactoglobulin [βLG]) through experiments and simulation calculations, a thermally controlled hierarchical strategy was firstly reported for self‐assembly of AM–LA–βLG complex into uniform‐sized nanospheres with well‐defined crystalline structure and stability. These nanospheres were substantially resistant to amylolysis and presented great fermentation functions by gut microbiota, including production of short‐chain fatty acids and regulating the bacterial composition and diversity.

Dissipative self‐assembly (DSA) system requires a continuous supply of fuels to maintain the far‐from‐equilibrium assembled state. Living organisms exist and operate far from the thermodynamic equilibrium by continuous consumption of energy taken from the surroundings, so how to realize the construction of the artificial DSA system has attracted much attention by researchers all over the world. Owing to dynamic controllable noncovalent interactions, artificial supramolecular DSA systems have achieved higher functions fueled by various types of energy, such as chemical fuels, light, electric energy, acoustic energy, and mechanical energy. Upon the input of external fuels, nonactive precursors can be activated to form building blocks at higher energy levels and then self‐assemble into transient supramolecular structures. As the proceeding of deactivation reaction, the building blocks with higher energy level dissipate back to the initial precursors, resulting in the disassembly process, to complete a full cycle. In this review, we summarize the recent advances of artificial supramolecular DSA systems on its construction strategies and energy‐fueled regulation approaches. The applications of supramolecular DSA systems in luminescence modulating, information encryption, self‐regulating gels, drug delivery, and catalysis are also discussed. We hope that this review article will facilitate further understanding and development of DSA systems. Dissipative self‐assembly system leads to far‐from‐equilibrium materials. In this review, we summarize chemical, light, electricity, mechanical energy, and acoustic energy fueled supramolecular dissipative self‐assembly systems, and their applications on luminescence modulation, self‐erasable materials, self‐regulating hydrogels, controllable delivery system, and dynamic catalysis.

A striking feature of living systems is their ability to produce motility by amplification of collective molecular motion from the nanoscale up to macroscopic dimensions. Some of nature's protein motors, such as myosin in muscle tissue, consist of a hierarchical supramolecular assembly of very large proteins, in which mechanical stress induces a coordinated movement. However, artificial molecular muscles have often relied on covalent polymer-based actuators. Here, we describe the macroscopic contractile muscle-like motion of a supramolecular system (comprising 95% water) formed by the hierarchical self-assembly of a photoresponsive amphiphilic molecular motor. The molecular motor first assembles into nanofibres, which further assemble into aligned bundles that make up centimetre-long strings. Irradiation induces rotary motion of the molecular motors, and propagation and accumulation of this motion lead to contraction of the fibres towards the light source. This system supports large-amplitude motion, fast response, precise control over shape, as well as weight-lifting experiments in water and air.