Supramolecular chemistry articles within Nature Chemistry

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  • Article |

    Despite mechanically axially chiral (MAC) catenanes being recognized in 1961, their stereoselective synthesis had not been disclosed until now. Closer inspection of the MAC stereogenic unit has also led to the identification of an analogous, but unremarked upon, form of rotaxane stereochemistry and the conceptualization of a general approach to prepare MAC molecules stereoselectively.

    • John R. J. Maynard
    • , Peter Gallagher
    •  & Stephen M. Goldup

  • Review Article |

    The emerging field of dissipative DNA nanotechnology aims at developing synthetic devices and nanomaterials with life-like properties such as directional motion, transport, communication or adaptation. This Review surveys how dissipative DNA systems combine the programmability of nucleic-acid reactions with the consumption of energy stored in chemical fuel molecules to perform work and cyclical tasks.

    • Erica Del Grosso
    • , Elisa Franco
    •  & Francesco Ricci

  • Article |

    Oscillations are widespread throughout the natural world and a number of fascinating inorganic oscillating reactions are known—but the formation and control of oscillating, self-replicating synthetic systems has remained challenging. Now, it has been shown that chemically fuelled oscillations within a network of organic replicators can drive supramolecular assembly and disassembly.

    • Michael G. Howlett
    • , Anthonius H. J. Engwerda
    •  & Stephen P. Fletcher

  • News & Views |

    The rational synthesis of organic nanotubes and their hierarchical architectures has remained challenging. Now, one-dimensional hollow covalent organic frameworks have been prepared that can further assemble into toroid-shaped materials.

    • Gabrielle A. Leith
    •  & Natalia B. Shustova

  • Article |

    Halogen-bonded co-crystals of a fluorinated azobenzene derivative and a volatile co-former can be cut, carved or engraved with micrometre-scale precision using low-power visible light. The proposed mechanism involves the local evaporation of the volatile component followed by recrystallization of the azobenzene co-former near the edge of the irradiation area.

    • T. H. Borchers
    • , F. Topić
    •  & C. J. Barrett

  • Article |

    A wide variety of covalent organic cages and two- and three-dimensional covalent organic frameworks have been obtained through dynamic covalent chemistry, yet the synthesis of their one-dimensional counterparts has remained challenging. Porous covalent organic nanotubes have now been prepared through reversible aldehyde–amine condensation and it has been shown that these can further assemble into toroidal architectures.

    • Kalipada Koner
    • , Shayan Karak
    •  & Rahul Banerjee

  • Article |

    Nanometre-sized polyaromatic hydrocarbons (nanographenes) have been largely explored as single-layer systems. Now a C64 nanographene comprising a planar core decorated with four terphenyl–imide moieties at its periphery has been shown to assemble with coronene to form bi- and trilayer host–guest complexes in solution, as well as tetra-, hexa- and multilayer stacks in the crystalline state.

    • Magnus Mahl
    • , M. A. Niyas
    •  & Frank Würthner

  • News & Views |

    The adsorption of molecules onto a surface from solution generally proceeds spontaneously by means of an equilibrium process. Now, it has been shown that macrocycles can be pumped onto a MOF substrate through the formation of mechanical bonds in a ratcheting mechanism that results in an out-of-equilibrium state.

    • Liang Zhang

  • News & Views |

    Why do bulky anions solubilize macromolecules in water but precipitate out the corresponding monomers? The answer lies in the differences in local water structure. Polymers have now been shown to disrupt water structure more than their monomers, leading to an accumulation of anions near the polymers that increases their solubility.

    • Aniket U. Thosar
    •  & Amish J. Patel

  • Article |

    DNA-encoded libraries facilitate the discovery of ligands that interact with biomolecules but such technologies do not take full advantage of the principles of Darwinian selection. Now, libraries of conformationally constrained peptides (Dsuprabodies) have been assembled using a strategy that allows for iterative cycles of selection, amplification and diversification. This method was validated with selections against streptavidin and PD-L1.

    • Balayeshwanth R. Vummidi
    • , Lluc Farrera-Soler
    •  & Nicolas Winssinger

  • Article |

    The synthesis of chiral interlocked molecules in which the mechanical bond provides the only source of stereochemistry remains challenging. Now, a chiral interlocked auxiliary approach to mechanically planar chiral rotaxanes has been developed and its potential demonstrated through the synthesis of a range of difficult targets with high enantioselectivity.

    • Alberto de Juan
    • , David Lozano
    •  & Stephen M. Goldup

  • Thesis |

    Bruce C. Gibb reminds us that buffers are not necessarily innocent bystanders and that they can bind to biomacromolecules too.

    • Bruce C. Gibb

  • Article |

    In biological systems, controlled molecular motion along a particular path is realized by protein motors that travel along microtubule filaments. Now, control of motion with light has been achieved in a synthetic supramolecular system, in which anionic porphyrin molecules move along the fibres of a bis-imidazolium gel upon irradiation.

    • Mario Samperi
    • , Bilel Bdiri
    •  & David B. Amabilino

  • Article |

    Liquid–liquid phase separation plays an important role in creating cellular compartments and protocells, but designing small-molecule models remains difficult. A peptide-based synthon for liquid–liquid phase separation consisting of two stickers and a flexible, polar spacer has now been presented. Condensates formed by these synthons can concentrate biomolecules and catalyse anabolic reactions.

    • Manzar Abbas
    • , Wojciech P. Lipiński
    •  & Evan Spruijt

  • Article |

    Coulombic interactions can be used to assemble charged nanoparticles into higher-order structures, but this process typically requires similarly sized oppositely charged partners. Now, small anions or cations with as few as three charges have been shown to induce attractive interactions between oppositely charged nanoparticles in water, guiding the assembly of colloidal crystals.

    • Tong Bian
    • , Andrea Gardin
    •  & Rafal Klajn

  • News & Views |

    Although the natural lasso peptide microcin J25 remains an elusive target for total chemical synthesis itself, this topologically non-trivial building block has now been used to construct a range of interlocked molecular architectures including rotaxanes, catenanes and daisy chains.

    • Jan H. van Maarseveen

  • Article |

    The construction of mechanically interlocked molecules solely made from peptides is a great synthetic challenge because of a lack of effective templating strategies. Now it has been shown that by combining self-assembly and dynamic covalent chemistry, catenanes, daisy chains and other interlocked peptides can be synthesized from genetically engineered building blocks.

    • Hendrik V. Schröder
    • , Yi Zhang
    •  & A. James Link

  • News & Views |

    Self-organization — ubiquitous in living systems — occurs out-of-equilibrium, with dissipation of energy and matter. Researchers have now shown that slow proton dissipation switches the assembly of DNA-based fibres to a growth mechanism that heals their gaps, yielding tight nanocable architectures.

    • Mathieu Surin

  • News & Views |

    A new class of interwoven metal–organic containers, including one with a cubic architecture, twelve crossing points and a large internal volume, has now been reported. Interconversion between different self-assembled structures can be triggered by simply exchanging the associated anions.

    • Andrew W. Heard
    • , Natasha M. A. Speakman
    •  & Jonathan R. Nitschke

  • Article |

    Nature uses out-of-equilibrium systems to control hierarchical assembly. Now, a dissipative chemical system has been shown to slowly release monomer DNA strands from a high-energy reservoir, regulating self-assembly by switching the mechanism of supramolecular polymerization at the single-molecule level. This process heals fibre defects, converting branched, heterogeneous networks into nanocable superstructures.

    • Felix J. Rizzuto
    • , Casey M. Platnich
    •  & Hanadi F. Sleiman

  • Article |

    Porous materials are promising candidates for the cost- and energy-efficient separation of ethylene and ethane from gas mixtures: an important but challenging industrial process. Now, a hydrogen-bonded organic framework has been reported that is stable under harsh conditions and can take up ethylene at practical temperatures—with very high selectivity over ethane—through a gating mechanism.

    • Yisi Yang
    • , Libo Li
    •  & Banglin Chen

  • News & Views |

    Thirty years ago the assembly of molecular ‘tectons’ into organic networks with large chambers using directional non-covalent interactions — hydrogen bonds — provided a blueprint for the synthesis of porous functional materials through crystal engineering.

    • Andrew I. Cooper

  • Article |

    Single crystals of a helical covalent polymer have been obtained from an achiral monomer through spiroborate formation. Polymerization and crystallization occur simultaneously to give a network of pairs of entwined helical strands of the same handedness. No strong non-covalent interactions were observed between the two helical polymers forming a pair; instead, each interacts with neighbouring pairs through hydrogen bonding.

    • Yiming Hu
    • , Simon J. Teat
    •  & Wei Zhang

  • Article |

    In atomic solids, substitutional doping is a powerful approach to modulating materials properties. Now, three substitutional mixtures of {Co6Se8} and {Cr6Te8} clusters in a crystal lattice with C60 fullerenes have been prepared. At two Co:Cr mixing ratios, the solid solutions showed particularly high electrical conductivities and low activation barriers for electron transport, owing to their structural heterogeneity.

    • Jingjing Yang
    • , Jake C. Russell
    •  & Colin Nuckolls

  • Article |

    A supramolecular three-shell matryoshka-like complex di rects the functionalization of the C60 inner shell to the selective formation of a single trans-3 fullerene bis-adduct. The selectivity with this matryoshka-like approach could be useful for applications where regioisomerically pure C60 bis-adducts have been shown to have superior properties compared with isomer mixtures.

    • Ernest Ubasart
    • , Oleg Borodin
    •  & Xavi Ribas

  • Article |

    DNA G-quadruplexes can adopt a variety of secondary structures, but it is challenging to identify and classify them quickly. Multivariate analysis of different fluorescence enhancements—generated from an arrayed suite of synthetic hosts and cationic dyes—enables discrimination between G-quadruplex structures of identical length and similar topological types.

    • Junyi Chen
    • , Briana L. Hickey
    •  & Wenwan Zhong

  • Article |

    Molecular catalysts can be made more practical by anchoring them onto electrode surfaces, but such systems are less stable than standard heterogeneous electrocatalysts. Now, supramolecular hosts bound to electrode surfaces have enabled the immobilization of molecular electrocatalysts through host–guest interactions. Desorbed or degraded guest molecules can be replaced with fresh guest molecules, extending their lifetimes.

    • Laurent Sévery
    • , Jacek Szczerbiński
    •  & S. David Tilley

  • Article |

    Collagen-like peptides can self-assemble into hundreds of closely related triple helices. Now, an algorithm has been developed that predicts the most stable helix and the extent to which it will assemble to the exclusion of the competing helices. This information can help improve the understanding of triple helix design and assembly.

    • Douglas R. Walker
    • , Sarah A. H. Hulgan
    •  & Jeffrey D. Hartgerink

  • News & Views |

    The synthesis of molecular knots has been a major achievement in the field of chemical topology, but only a few relatively simple ones have been made so far. A route based on a weaving approach has now been used to make a seven-crossing knot and could offer a route to more complicated structures.

    • Dan Preston
    •  & Paul E. Kruger

  • Article |

    A combination of metal- and anion-template synthesis directs the weaving of molecular weft and warp strands in the assembly of a 3 × 3 interwoven grid. Connection of the ligand strands by alkene metathesis produces the topology of a seven-crossing endless knot, an important cultural and religious symbol.

    • David A. Leigh
    • , Jonathan J. Danon
    •  & Steffen L. Woltering

  • Article |

    Mirror-symmetry breaking in chiral systems by a chiral solvent has remained poorly understood for decades. Now, the supramolecular polymerization of triphenylene derivatives has shown that—through the additive effects of polymerization—the cumulative entropic effects of the interactions between chiral solvents and solutes create measurable differences in free enthalpy.

    • Marcin L. Ślęczkowski
    • , Mathijs F. J. Mabesoone
    •  & E. W. Meijer

  • News & Views |

    Artificial photosynthesis represents a promising method of generating hydrogen for our clean and sustainable energy needs. Now, photocatalytic nanofibres have been developed that incorporate photosensitizers and catalysts into well-defined self-assembled structures for efficient hydrogen production.

    • Gregory I. Peterson
    • , Sanghee Yang
    •  & Tae-Lim Choi

  • Article |

    The majority of discrete structures obtained by self-assembly possess high symmetry, and thus low complexity: all subunits relate to their neighbours in a similar manner. Now, the spontaneous formation of complex low-symmetry assemblies produced from a single building block has been demonstrated using a systems chemistry approach. The single building block oligomerizes to form specific homomeric cyclic macromolecules that adopt a folded conformation.

    • Charalampos G. Pappas
    • , Pradeep K. Mandal
    •  & Sijbren Otto

  • Article |

    Nature successfully uses supramolecular assemblies for efficient and robust solar energy harvesting; however, mimicking such material systems for applications in optoelectronic devices has been hampered by stability issues such as the fragility of the supramolecular structures used and the delicate nature of Frenkel excitons. Now, enabled by tunable cage-like scaffolds, stable supramolecular light-harvesting nanotubes have been composed that are robust even under heat stress.

    • Kara Ng
    • , Megan Webster
    •  & Dorthe M. Eisele

  • Article |

    Layered COFs are attractive precursors for two-dimensional materials but they are difficult to cleave into mono- or few-layer sheets. Pseudorotaxane moieties have now been embedded into layered COFs to facilitate their cleavage into sheets of uniform thickness. Crown-ether macrocycles within the COF backbone bind to ionic viologen guests, leading to electrostatic repulsion between layers.

    • Xing Li
    • , Hai-Sen Xu
    •  & Kian Ping Loh

  • Q&A |

    Manza B. J. Atkinson talks to Nature Chemistry about his path to become a chemist, and how he applies the scientific method to all aspects of his life — from financial analysis to coaching youth sports teams.

    • Anne Pichon

  • News & Views |

    Controlling the formation of ordered and predictable patterns in dissipative reaction–diffusion processes is challenging. Now, liquid vibrations induced by audible sound have been shown to direct the formation of spatiotemporal patterns in switchable chemical systems and assemblies.

    • Charalampos G. Pappas

  • Meeting Report |

    Chemical systems can show complex behaviour that is not seen in individual molecules or reactions. Helena S. Azevedo, Sarah L. Perry, Peter A. Korevaar, and Dibyendu Das report on the emergence of this complex behaviour, which was discussed at the Virtual Symposium on Systems Chemistry

    • Helena S. Azevedo
    • , Sarah L. Perry
    •  & Dibyendu Das

  • Article |

    Patterns formed by artificial out-of-equilibrium chemical oscillating networks (such as the Belousov–Zhabotinsky reaction) are difficult to control with any precision. Now, it has been shown that low-intensity audible sound can be used to generate spatiotemporal patterns with a programmable distribution of redox- and pH-responsive chemical systems and supramolecular assemblies in solution.

    • Ilha Hwang
    • , Rahul Dev Mukhopadhyay
    •  & Kimoon Kim

  • Article |

    Reversible nanoscale knotting and unknotting of a molecular strand can be used to control the handedness of helical organizations at macroscopic length scales. Dopant knotted and unknotted strands induce supramolecular helical structures of opposite handedness in achiral liquid crystals, and the left- and right-handed forms can be switched in situ.

    • Nathalie Katsonis
    • , Federico Lancia
    •  & Fredrik Schaufelberger

  • Thesis |

    Despite the romantic mythology that often accompanies stories of scientific discovery, pinpointing the exact moment in history when a new concept emerged is often a matter of debate — and the hydrogen bond is no exception explains Bruce C. Gibb.

    • Bruce C. Gibb

  • Article |

    Molecular rotors have been engineered within the bicyclopentane–dicarboxylate struts of a metal–organic framework—the bicyclic unit is the rotator and the carboxylate groups serve as the stator. In a zinc-based metal–organic framework, the crossed conformation of the strut–metal nodes enables fast rotation of the bicyclic moiety, but in the corresponding zirconium metal–organic framework a change in the conformation results in much slower rotation.

    • Jacopo Perego
    • , Silvia Bracco
    •  & Piero Sozzani

  • News & Views |

    It’s not known how life’s essential properties of replication, metabolism and compartmentalization were first integrated. Two recent articles now shed light on how metabolic characteristics may be incorporated into replicating systems, harnessing an external energy source to increase their rate of replication and acquiring catalytic activity.

    • Pablo Solís-Muñana
    •  & Jack L. Y. Chen

  • Article |

    Water plays an active role in modulating guest recognition by both artificial and biological hosts, but how this role can be controlled is unclear. Now, the de-wetting of the non-polar pockets of cavitands is shown to be affected by the orientation of methyl groups encircling the portal, which moderate the enthalpic and entropic contributions driving recognition.

    • J. Wesley Barnett
    • , Matthew R. Sullivan
    •  & Henry S. Ashbaugh

  • News & Views |

    A series of mesoscale supramolecular hexagonal grids have been constructed in solution through stepwise intra- then intermolecular coordination-driven self-assembly, and characterized with atomic resolution by scanning tunnelling microscopy and spectroscopy.

    • Ruoning Li
    •  & Yongfeng Wang

  • Article |

    The distortion of an amide group away from a planar conformation typically enhances its reactivity and such activation is usually achieved through the chemical synthesis of twisted amides. Now, it has been shown that a non-covalent activation strategy leading to accelerated hydrolysis can be achieved by binding a reactive twisted amide conformer inside a molecular cage.

    • Hiroki Takezawa
    • , Kosuke Shitozawa
    •  & Makoto Fujita

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