Physical sciences articles within Nature Chemistry

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  • News & Views |

    X-ray diffraction analysis typically affords the static 3D structures of given compounds or materials, but to understand chemical processes, the visualization of fast structural changes is desirable. Time-resolved femtosecond crystallography has now been used to monitor the structural dynamics of a photoactive metal–organic framework.

    • Lauren E. Hatcher
    •  & Paul R. Raithby

  • Research Briefing |

    The precision synthesis of cyclic polymers with ultrahigh molar mass (UHMM) and circularity is challenging. Now, a method that involves superbase-mediated living linear-chain growth followed by macromolecular cyclization triggered by protic quenching enables the on-demand production of UHMM cyclic polymers with a narrow dispersity and closed-loop chemical recyclability.

  • Article |

    Overcrowded alkene-derived molecular motors convert light and heat into chirality-directed unidirectional rotary motion, but the efficiency of their photochemical isomerization remains limited. Now formylation of the motor core has been shown to boost all aspects of motor photochemistry by improving photochemical efficiency, diminishing competing processes and redshifting absorption.

    • Jinyu Sheng
    • , Wojciech Danowski
    •  & Ben L. Feringa

  • Article |

    The construction of analogues of natural gap junctions would provide a bottom–up strategy for building intercellular communication pathways for synthetic cells. Now artificial intercellular gap junctions have been prepared from unimolecular tubular channels by mimicking the hydrophobic–hydrophilic–hydrophobic triblock structure of natural junction channels.

    • Yong-Hong Fu
    • , Yi-Fei Hu
    •  & Jun-Li Hou

  • Article
    | Open Access

    Advances in the development of cytoskeletal-like materials with modular structures and mechanics are pivotal for the engineering of synthetic cells. Now actin-mimetic supramolecular peptide networks have been designed using programmable peptide–DNA crosslinkers, giving rise to tunable tactoid-shaped bundles and mechanical properties that control spatial localization, the diffusion of payloads and shape changes within artificial cells.

    • Margaret L. Daly
    • , Kengo Nishi
    •  & Ronit Freeman

  • Article
    | Open Access

    Knots reduce the tensile strength of macroscopic threads and fibres. Now it has been shown that the presence of a well-defined overhand knot in a polymer chain can substantially increase the rate of scission of the polymer under tension, as deformation of the polymer backbone induced by the tightening knot activates otherwise unreactive covalent bonds.

    • Min Zhang
    • , Robert Nixon
    •  & David A. Leigh

  • Article |

    The selective synthesis of ultrahigh-molar-mass (UHMM) cyclic polymers from direct polymerization is elusive. Using a chemically recyclable polythioester as a model, it has now been shown that a common superbase mediates living linear-chain growth, followed by proton-triggered linear-to-cyclic topological transformation, producing UHMM cyclic polymers with a narrow dispersity.

    • Li Zhou
    • , Liam T. Reilly
    •  & Eugene Y.-X. Chen

  • News & Views |

    Chlorine-containing waste streams pose potential risks to human health and the environment, so their remediation represents a significant challenge. Now, chlorinated wastes have been successfully repurposed as chlorinating reagents for use in the preparation of organic chemicals and pharmaceutical ingredients.

    • Andrew Jordan

  • News & Views |

    Understanding the ways by which metal-containing catalysts carry out a reaction is a chemical puzzle. Now, investigations of a multi-metallic molecular system uncover how the self-assembly of molecular catalysts facilitates cooperation between active species and improves the conversion of water to hydrogen gas.

    • Ana Sonea
    •  & Jeffrey J. Warren

  • Article |

    Although metal-free catalysts, featuring defined active sites, represent alternatives to scarce or problematic metals, metal-free compounds rarely show activities as promising as metal-based materials. Now deprotonated 2-thiolimidazole is shown to serve as a metal-free electrocatalyst for selective acetylene hydrogenation and achieves competitive performances with metal-based catalysts.

    • Lei Zhang
    • , Rui Bai
    •  & Jian Zhang

  • Article
    | Open Access

    Enantioconvergent reactions convert both enantiomers of a racemic starting material into a single enantioenriched product. All currently known enantioconvergent processes necessitate the loss or partial loss of the racemic substrate’s stereochemical information. Now, an alternative approach has been developed that proceeds with full retention of the racemic substrate’s configuration.

    • Steven H. Bennett
    • , Jacob S. Bestwick
    •  & Andrew L. Lawrence

  • Article |

    Phenols and their derivatives are ubiquitous in nature and important within the chemical industry. Their properties are linked to their substitution patterns, but meta-isomers are underrepresented due to the difficulty of their synthesis. Now we address this challenge by describing a 1,2-transposition of phenols that enables a formal para- to meta-isomerization.

    • Simon Edelmann
    •  & Jean-Philip Lumb

  • Article |

    Despite their intriguing photochemical activities, natural photoenzymes have not yet been repurposed for new-to-nature activities. Now, by leveraging the strongly oxidizing excited-state flavoquinone cofactor, fatty acid photodecarboxylases were engineered to catalyse unnatural decarboxylative radical cyclization with excellent chemo-, enantio- and diastereoselectivities.

    • Shuyun Ju
    • , Dian Li
    •  & Yang Yang

  • Article
    | Open Access

    Radical polymerizations yield polymers that cannot easily be degraded. The co-polymerization of cyclobutene-based monomers with conventional vinyl monomers has now been shown to result in co-polymers with cyclobutane mechanophores in their backbone, which facilitate on-demand degradation through a combination of mechanical activation and hydrolysis. This approach offers a promising avenue for the degradation of all-carbon-bond-backbone polymers.

    • Peng Liu
    • , Sètuhn Jimaja
    •  & Nico Bruns

  • Research Briefing |

    A non-radical proximity labelling platform — BAP-seq — is presented that uses subcellular-localized BS2 esterase to convert unreactive enol-based probes into highly reactive acid chlorides in situ to label nearby RNAs. When paired with click-handle-mediated enrichment and sequencing, this chemistry enables high-resolution spatial mapping of RNAs across subcellular compartments.

  • Article
    | Open Access

    The development of new methodologies to convert plastics into fuels without relying on noble metal-based catalysts is desirable. Now it is shown that a layered self-pillared zeolite enables the conversion of polyethylene to gasoline with a selectivity of 99% and yields of >80% without the need to use external hydrogen.

    • Ziyu Cen
    • , Xue Han
    •  & Buxing Han

  • Article |

    RNA localization is key to regulating cellular function but is challenging to measure in an unbiased manner. Now a combination of enol-masked acylating probes with a bioorthogonal esterase to locally unmask them provides a non-radical RNA proximity labelling platform—termed BAP-seq—that enables the generation of high-resolution spatial maps of RNA.

    • Shubhashree Pani
    • , Tian Qiu
    •  & Bryan C. Dickinson

  • Article |

    Chiral 1,2-benzazaborines are promising isosteres of naphthalene, but rarely explored due to the lack of efficient synthetic methods. Now, the copper-catalysed enantioselective hydroboration of alkenes with 1,2-benzazaborines has been developed, providing a general platform for the atom-economic and efficient construction of diverse chiral 1,2-benzazaborine compounds bearing a 2-carbon-stereogenic centre or allene skeleton.

    • Wanlan Su
    • , Jide Zhu
    •  & Qiuling Song

  • Article
    | Open Access

    Carbon capture, utilization and storage is key for climate change mitigation and developing more environmentally friendly technologies. Now it has been shown that CO2 capture in single-component water-lean solvents is accompanied by the self-assembly of reverse-micelle-like tetrameric clusters in solution that enable the formation of various CO2-containing compounds.

    • Julien Leclaire
    • , David J. Heldebrant
    •  & Jaelynne King

  • News & Views |

    Surface heterogeneities lead to friction between droplets and solid surfaces, limiting the performance of the latter in a number of applications. A combination of friction force measurements and atomistic molecular dynamics simulations now sheds light on the influence of molecular scale heterogeneities on droplet friction.

    • Abhinav Naga
    •  & Doris Vollmer

  • Research Briefing |

    Ether-based electrolytes are desired for lithium metal batteries owing to their low reduction potentials; however, they suffer from low anodic stability. Strategic methylation of ether solvents is shown to extend their electrochemical stability and facilitate the formation of LiF-rich interphases, enabling high-voltage lithium metal batteries while avoiding the use of fluorinated solvents.

  • Article
    | Open Access

    Despite the widespread utility of ruthenium catalysts, many protocols for their use require high temperatures or light irradiation. Now, the synthesis of an air- and moisture-stable ruthenium precatalyst has been reported. This versatile catalyst drives an array of transformations and enables rapid screening and optimization of reactions, revealing previously unknown in situ generated ruthenium complexes.

    • Gillian McArthur
    • , Jamie H. Docherty
    •  & Igor Larrosa

  • Article |

    Lithium metal batteries are an attractive energy storage technology, but their development relies on the complex interplay between the components’ chemical, physical and mechanical properties. Now, selective methylation of dimethoxyethane ether electrolytes is shown to improve electrolyte, electrode and solid–electrolyte interphase stabilities to enable high-performance 4.3 V lithium metal batteries.

    • Ai-Min Li
    • , Oleg Borodin
    •  & Chunsheng Wang

  • Article
    | Open Access

    α-Amino acids possessing β-stereocentres are difficult to synthesize. Now, an iridium-catalysed protocol allows the direct upconversion of simple alkenes and glycine derivatives to give β-substituted α-amino acids with exceptional levels of regio- and stereocontrol. The reaction design is based on exploiting the native directing ability of a glycine-derived N–H unit to facilitate enolization of the adjacent carbonyl.

    • Fenglin Hong
    • , Timothy P. Aldhous
    •  & John F. Bower

  • Article |

    The redox properties of visible-light-absorbing photosensitizers are limited by the energy of visible photons, but methods using sensitization-initiated electron transfer have recently been developed to address these challenges. Now a multiphoton dual-catalyst strategy has been used to enable the enantioselective de Mayo reaction for the synthesis of enantioenriched 1,5-diketones.

    • Xin Sun
    • , Yilin Liu
    •  & Zhiyong Jiang

  • Article |

    Key molecular features that drive protein liquid–liquid phase separation (LLPS) for biomolecular condensate have been reported. A spectrum of additional interactions that influence protein LLPS and material properties have now been characterized. These interactions extend beyond a limited set of residue types and can be modulated by environmental factors such as temperature and salt concentration.

    • Shiv Rekhi
    • , Cristobal Garcia Garcia
    •  & Jeetain Mittal

  • News & Views |

    Biological and synthetic catalysts often utilize iron in high oxidation states (+IV and greater) to perform challenging molecular transformations. A coordination complex featuring an Fe(VII) ion has now been synthesized through sequential oxidations of nonheme iron–nitrido precursors.

    • Adam T. Fiedler
    •  & Laxmi Devkota

  • Perspective |

    Lack of standardization, transparency and interaction creates information gaps in scientific publications. Through strategies such as voluntary information management, standardization of reaction set-ups, and smart screening approaches, this Perspective gives guidelines on how to improve data management in publications reporting chemical reactions, focusing on reproducibility, standardization and evaluation of synthetic transformations.

    • Malte L. Schrader
    • , Felix R. Schäfer
    •  & Frank Glorius

  • News & Views |

    Chiral amines possessing a stereogenic carbon atom bearing three carbon substituents and one nitrogen substituent are challenging structural motifs to prepare enantioselectively. Now, such motifs have been accessed in high enantiopurities by asymmetric Cu-catalysed propargylic amination using sterically confined ligands.

    • Joshua D. Sieber

  • News & Views |

    Expansion of the genetic code can enable precise manipulation of proteins through selective functionalization of specific residues. Now, control of tryptophan interactions in proteins can be established by encoding of a vinyl-caged tryptophan analogue that can be selectively decaged to rescue protein activity.

    • Aidan K. Haney
    •  & T. Ashton Cropp

  • Article |

    Although the light-driven generation of hydrogen from water is a promising approach to renewable fuels, the H–H bond formation step represents a persistent mechanistic question. Now light-harvesting molecular catalysts have been shown to self-assemble into nanoscale aggregates that feature improved efficiency for photoelectrochemical H2 evolution.

    • Isaac N. Cloward
    • , Tianfei Liu
    •  & Alexander J. M. Miller

  • Article |

    Accessing longer-wavelength emitting organic fluorophores is critical for diagnostic imaging. Here a series of silicon-RosIndolizine fluorophores with emission maxima at 1,300 nm, 1,550 nm and 1,700 nm were synthesized. The fluorophores generate high-resolution in vivo fluorescence images in mice and establish design principles for future shortwave-infrared fluorophore designs.

    • William E. Meador
    • , Eric Y. Lin
    •  & Jared H. Delcamp

  • Article
    | Open Access

    Time-resolved femtosecond crystallography (TR-SFX) is a powerful technique to monitor structural transitions in protein crystals at the atomic level, but its use in non-protein synthetic materials remains limited. Now TR-SFX has been used to visualize the structural dynamics of metal–organic frameworks, showing the potential of this tool to study the dynamic motion of crystalline porous materials.

    • Jaedong Kang
    • , Yunbeom Lee
    •  & Hyotcherl Ihee

  • Article |

    Ribosomally synthesized and post-translationally modified peptides (RiPPs) can have vast structural diversity and biological functions enabled by disparate post-translational modifications (PTMs). However, unconventional PTMs derived from non-RiPP biosynthesis are rarely reported. Now a class of lipopeptides featuring a distinct fatty-acyl-modified N terminus and the responsible RiPP/fatty-acid hybrid biosynthetic machinery have been characterized.

    • Hengqian Ren
    • , Chunshuai Huang
    •  & Huimin Zhao

  • Research Briefing |

    We developed a high-throughput, unbiased strategy for the identification of endogenous biomolecular condensates by merging cell volume compression, sucrose density gradient centrifugation and quantitative mass spectrometry. We demonstrated the performance of this strategy by identifying both global condensate proteins and those responding to specific biological processes on a proteome-wide scale.

  • Article |

    Enantioenriched α-disubstituted α-ethynylamines are valuable synthons to chiral α-tertiary amines and azacycles, but their facile access remains challenging. Now, sterically confined pyridinebisoxazoline ligands have been developed to facilitate highly enantioselective Cu(I)-catalysed propargylic amination of both aliphatic and aryl ketone-derived propargylic carbonates to give α-tertiary ethynylamines. Related tandem sequences are reported to synthesize quaternary azacycles.

    • Zheng Zhang
    • , Ying Sun
    •  & Jian Zhou

  • Article
    | Open Access

    The spontaneous recombination of photogenerated radicals surrounded by solvent molecules is an important energy-wasting elementary step in photoredox reactions. Now the decisive role that cage escape plays in these reactions is shown in three benchmark photocatalytic reactions, with quantitative correlations observed between photoredox product formation rates and cage escape quantum yields.

    • Cui Wang
    • , Han Li
    •  & Oliver S. Wenger

  • Article |

    High-throughput proteome-wide methods for identifying endogenous proteins that phase separate or partition into condensates during certain physiological events are needed but remain a challenge. Now, a high-throughput, unbiased and quantitative strategy can identify endogenous biomolecular condensates and screen proteins involved in phase separation on a proteome-wide scale.

    • Pengjie Li
    • , Peng Chen
    •  & Yiwei Li

  • Article
    | Open Access

    The insertion of metal atoms and heteroaromatic units provides a way to tune the optical, electronic and magnetic properties of graphene nanoribbons. Now the synthesis of a porphyrin-fused graphene nanoribbon with a narrow bandgap and high charge mobility has been achieved, and this material used to fabricate field-effect and single-electron transistors.

    • Qiang Chen
    • , Alessandro Lodi
    •  & Harry L. Anderson

  • Article
    | Open Access

    Although hydrogels with complex, heterogeneous and reconfigurable structures are promising materials for use in intelligent systems, fabricating such hydrogels is challenging. Now it has been shown that they can be fabricated by reversibly gluing different hydrogel units using a photocontrolled metallopolymer adhesive. This method can be used to design hydrogels with customized functions.

    • Jiahui Liu
    • , Yun-Shuai Huang
    •  & Si Wu

  • Article
    | Open Access

    Atomistic simulations have a broad range of applications from drug design to materials discovery. Machine learning interatomic potentials (MLIPs) have become an efficient alternative to computationally expensive ab initio simulations. Now a general reactive MLIP (called ANI-1xnr) has been developed and validated against a broad range of condensed-phase reactive systems.

    • Shuhao Zhang
    • , Małgorzata Z. Makoś
    •  & Justin S. Smith

  • In Your Element |

    Ciro Romano, Jack I. Mansell, and David J. Procter have explored the versatility and selectivity of samarium diiodide, and its use as a radical relay catalyst.

    • Ciro Romano
    • , Jack I. Mansell
    •  & David J. Procter

  • Article
    | Open Access

    A previous investigation of the anti-aromatic dianion of [18]annulene concluded that it consists of a mixture of two isomers. Now it has been shown that this dianion exists as a single isomer, with a different geometry from neutral [18]annulene, and that it can be reduced further to an aromatic tetraanion.

    • Wojciech Stawski
    • , Yikun Zhu
    •  & Harry L. Anderson

  • Review Article |

    Nanopore label-free sequencing of DNA and RNA at the single-molecule level offers rapid readout, high accuracy, low cost and portability. This Review surveys technologies underpinning commercial and academic nanopore sequencing, and examines how underlying biochemical advances can fuel future developments in nanopore-based protein sequencing.

    • Adam Dorey
    •  & Stefan Howorka

  • Article |

    The rapid generation of molecular complexity from a given molecular scaffold is crucial to drug discovery and development. Now the chemodivergent molecular editing of indoles using fluoroalkyl carbenes has been developed to modularly access four different types of fluorine-containing N-heterocyclic compound with high molecular complexity.

    • Shaopeng Liu
    • , Yong Yang
    •  & Xihe Bi

  • Perspective |

    Although generally perceived as an old-fashioned and unselective tool to build molecules, the photochemistry community is now re-discovering the power of UV light and is using key mechanistic information to develop new catalytic processes driven by visible light. This Perspective discusses the progress and impact of UV light in organic synthesis.

    • Giulio Goti
    • , Kavyasree Manal
    •  & Luca Dell’Amico

  • Article |

    Electrolysers can upgrade CO2 into high-value chemicals, but there are few tools capable of tracking the reactions that occur within these devices during operation. Now an electrolysis optical coherence tomography platform has been developed to visualize the electrochemical conversion of CO2 to CO, plus the movement of components, within the device.

    • Xin Lu
    • , Chris Zhou
    •  & Curtis P. Berlinguette

  • News & Views |

    Electrocatalytic transformations often involve the concerted transfer of electrons and protons at electrode interfaces; however, these processes are not well understood. Now, experiments on an electrode that features well-defined molecular sites deepen fundamental understanding of such transfers to pave the way for future catalysts.

    • Siyuan L. Xie
    •  & Eva M. Nichols

  • Article |

    Developing a generalizable method for blocking and rescuing tryptophan (Trp) interactions would enable the gain-of-function manipulation of various Trp-containing proteins but has so far been challenging. Now a genetically encoded N1-vinyl-caged Trp capable of rapid and bioorthogonal decaging enables site-specific activation of Trp on a protein of interest within living cells.

    • Yuchao Zhu
    • , Wenlong Ding
    •  & Peng R. Chen

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