Chemistry articles within Nature Chemistry

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  • Article |

    The Au2+ oxidation state is rarely stable in molecules or extended solids, where extreme synthetic conditions or exotic ligands are often necessary. Now, Au2+ has been stabilized with simple Cl− ligands in Cs4AuIIAuIII2Cl12, an extended solid with a perovskite-derived structure that is readily synthesized under mild conditions and is stable to ambient conditions.

    • Kurt P. Lindquist
    • , Armin Eghdami
    •  & Hemamala I. Karunadasa

  • Article |

    Monomeric N-heterocyclic carbenes (NHCs) can act as molecular modifiers of metal surfaces and thus affect heterogeneous catalytic behaviour. Now NHC polymers have been formed on gold surfaces, consisting of ballbot-type repeating units bound to single gold adatoms. Conformational, electronic and charge transport properties explain the high surface mobility of the incommensurate NHC polymers.

    • Jindong Ren
    • , Maximilian Koy
    •  & Frank Glorius

  • Article
    | Open Access

    Radiation damage in biology is largely mediated by radicals and low-energy electrons formed by water ionization and extensive, localized water ionization can be caused by ultrafast processes following the core-level ionization of hydrated metal ions. Now it has been shown that, for Al3+ ions, relaxation occurs via sequential solute–solvent electron transfer-mediated decay.

    • G. Gopakumar
    • , I. Unger
    •  & O. Björneholm

  • News & Views |

    Scientists have been studying how polymers break in solutions for decades, but the mechanism by which chains are stretched to the point of covalent bond scission is not trivial. Now, an experiment series provides ample support for a dynamic model in which chains uncoil from end to middle, while concurrently relaxing.

    • Charles E. Diesendruck

  • News & Views |

    Although light-driven conversion of carbon dioxide receives widespread attention, it is also criticized due to the challenge of discerning true product formation from that of impurities. Now, significantly advanced guidelines for proper product identification have been developed, so we can better trust in what we see.

    • Jennifer Strunk

  • Article
    | Open Access

    Although noble metal coordination complexes typically show promising photophysical properties that enable applications in lighting, photocatalysis and solar energy conversion, first-row transition metal complexes rarely display properties as attractive. Now, two Cr(0) complexes are shown to afford excited-state lifetimes of ~50 ns and photophysical properties analogous to noble metal complexes, enabling efficient photoredox catalysis.

    • Narayan Sinha
    • , Christina Wegeberg
    •  & Oliver S. Wenger

  • Article |

    The design and improvement of enzymes based on physical principles remain challenging. Now, the vibrational Stark effect has been used to demonstrate how an electrostatic model can unify the catalytic effects of distinct chemical forces in a quantitative manner and guide the design of enzyme variants that outperform their natural counterpart.

    • Chu Zheng
    • , Zhe Ji
    •  & Steven G. Boxer

  • Article
    | Open Access

    Pump–probe measurements conventionally achieve femtosecond time resolution for X-ray crystallography of reactive processes, but the measured structural dynamics are complex. Using coherent control techniques, we show that the ultrafast crystallographic differences of a fluorescent protein are dominated by ground-state vibrational processes that are unconnected to the photoisomerization reaction of the chromophore.

    • Christopher D. M. Hutchison
    • , James M. Baxter
    •  & Jasper J. van Thor

  • Article |

    Although gas bubble dynamics during electrochemical processes dramatically affect performance, the fundamental understanding and manipulation of such dynamics have been limited. Now, electrolyte composition is found to be a key factor in inducing a solutal Marangoni instability that impacts both H2 gas detachment and coalescence between H2 microbubbles.

    • Sunghak Park
    • , Luhao Liu
    •  & Marc T. M. Koper

  • Article
    | Open Access

    Bicyclic lactones are valuable motifs for the synthesis of natural products and bioactive molecules. Now, a palladium-catalysed protocol has been developed to access unsaturated bicyclic lactones in one step from corresponding carboxylic acids. The method demonstrates reverse site selectivity for C(sp3)–H activation to form diverse bicyclic cores.

    • Jayabrata Das
    • , Wajid Ali
    •  & Debabrata Maiti

  • Article |

    While chiral hybrid organic–inorganic perovskites are promising materials for optoelectronic applications, the synthesis of three-dimensional single crystals has proven challenging. Now, a general strategy has been shown to synthesize chiral, three-dimensional perovskites by heterogeneous nucleation. The single-crystalline materials contain no chiral component; their chiroptical activity arises from supercells formed by chiral patterns of the A-site cations.

    • Gaoyu Chen
    • , Xiaoyu Liu
    •  & Xun Wang

  • Article |

    The coupling of autocatalysis to compartment growth and division is a key step in the origin of life. Now it has been shown that compartmentalizing the formose reaction in emulsion droplets leads to several crucial properties of living and evolving systems (growth, division, variation, competition, rudimentary heredity and selection).

    • Heng Lu
    • , Alex Blokhuis
    •  & Andrew D. Griffiths

  • Article |

    Interpenetration—in which two or more lattices are catenated—is common in metal–organic frameworks (MOFs). Now a deliberate synthesis of hetero-interpenetrated MOFs, with two distinct lattices, has been developed. It can combine the different properties of the two sublattices in one material, as demonstrated with chirality and catalytic activity, delivering an asymmetric catalyst.

    • David Perl
    • , Seok J. Lee
    •  & Shane G. Telfer

  • Article |

    Functionalizing two-dimensional transition-metal carbide (MXene) surfaces can alter their properties, but covalent functionalization has been synthetically challenging. Now, it has been shown that various organic groups can be covalently attached to MXene surfaces through amido and imido bonds. The resulting hybrid organic–inorganic structures exhibit Fano resonances and superior stability compared with traditional MXenes with a mixture of –F, –O and –OH surface terminations.

    • Chenkun Zhou
    • , Di Wang
    •  & Dmitri V. Talapin

  • Research Briefing |

    A multimodal imaging approach is developed to interrogate microorganism–semiconductor biohybrids at the single-cell and single-molecule level for light-driven CO2 fixation. Application to lithoautotrophic bacterium Ralstonia eutropha biohybrids reveals the roles of two hydrogenases in electron transport and bioplastic formation, the magnitude of semiconductor-to-single-cell electron transport and the associated pathways.

  • Article |

    Understanding interfacial and cellular electron transport is essential for guiding efficiency optimization in microbe–semiconductor biohybrids for energy conversion. A multimodal imaging platform that combines optical imaging and photocurrent mapping can now interrogate such electron-transport pathways at the single-cell level, uncovering different roles of hydrogenases and a microbe’s large electron-uptake capacity.

    • Bing Fu
    • , Xianwen Mao
    •  & Peng Chen

  • News & Views |

    The synthesis of natural products with important biological properties has always fascinated chemists, but the development of rapid, efficient and stereoselective transformations remains challenging. Now, a strategy has been developed to produce several strychnan alkaloids through formation of a common bridged morphan core structure.

    • Sylvain Canesi

  • In Your Element |

    Fiona C. Meldrum and Helmut Cölfen chalk up some of the myriad forms and uses of calcium carbonate to burnish a ‘dull’ reputation.

    • Fiona C. Meldrum
    •  & Helmut Cölfen

  • Comment |

    Critical realism distinguishes the ‘real’ world from the ‘observable’ one, which scientists explore as actors rather than as passive, neutral observers. Through this lens, it is clear that a diverse community that interrogates the world from different angles is an asset to the practice of chemistry itself.

    • Margaret A. L. Blackie

  • Article
    | Open Access

    Three-protein conjugates, which have so far been produced using protein-engineering strategies, can now be generated using a chemical approach that enables the addition of small-molecule functionality. Checkpoint inhibitory T cell engagers (CiTEs) were assembled and shown to have enhanced in vitro potency compared to a traditional T cell engager.

    • Peter A. Szijj
    • , Melissa A. Gray
    •  & Vijay Chudasama

  • Research Briefing |

    Despite advances, understanding of the quantum state-to-state scattering dynamics between charged ions and neutral molecules at low collision energies remains limited. A high-resolution crossed-beam experiment with quantum state-selected ions prepared by laser photoionization and supporting trajectory surface-hopping calculations now provides insight into the quantum state-to-state collisional dynamics of a model charge-transfer reaction.

  • Article |

    Quantum state-to-state understanding of collisional charge transfer is a long-time goal of chemical dynamics. Now, using high-resolution molecular-beam experiments with spin–orbit state-selected ions and surface-hopping calculations, a vibrational-state-specific mechanism has been observed for the reaction Ar+(2P3/2) + N2 → Ar + N2+(v′, J′). Besides the well-known long-range harpooning mechanism, a hard-collision glory scattering mechanism was also identified.

    • Guodong Zhang
    • , Dandan Lu
    •  & Hong Gao

  • Comment |

    Critical race theory — an academic framework that serves to understand systemic racism in the USA and beyond — can help inform endeavours to advance justice and equity in the chemistry community.

    • Terrell R. Morton

  • Article
    | Open Access

    The streamlined synthesis of multiple (proto)biomolecules from common starting materials is a key goal of prebiotic chemistry. Now, a one-pot synthesis of ribo-aminooxazoline (a precursor for prebiotic nucleotide synthesis) from HCN has been achieved. Additionally, the two moieties used in extant terpenoid biosynthesis have been accessed, with all carbon atoms also originating from HCN.

    • Dougal J. Ritson
    •  & John D. Sutherland

  • Article |

    Rapid solvent flows stretch dissolved polymer chains to their breaking point by hitherto-elusive molecular mechanisms. Now, analysis of competing mechanochemical reactions suggests a broad distribution of molecular geometries of fracturing chains. This occurs because, in each chain, fracture and kinetically destabilizing backbone stretching compete on submillisecond timescales.

    • Robert T. O’Neill
    •  & Roman Boulatov

  • Article |

    The kinetics of liquid–liquid phase separation (LLPS) in cell-like confinements remains poorly understood. Now it has been shown that it involves complex interplay between the incipient phases and the membrane boundary, which arrests phase coarsening, deforms the membrane and couples LLPS with lipid phase separation.

    • Wan-Chih Su
    • , James C. S. Ho
    •  & Atul N. Parikh

  • Article |

    Although Li–O2 batteries offer high theoretical capacities, redox mediators are necessary to control intermediate reaction kinetics and to limit electrode passivation. Now it has been shown that a family of triarylmethyl cations can rival top-performing quinone-based redox mediators. Cations with sluggish catalytic rates were found to suppress surface-mediated O2 reduction and achieve higher capacitances.

    • Erik J. Askins
    • , Marija R. Zoric
    •  & Ksenija D. Glusac

  • Article |

    In the atmosphere, photolysis of formaldehyde generates H and HCO radicals, which then react with O2 to form HO2 (important in converting atmospheric carbon to CO2). Now it has been shown that internally excited formaldehyde can also react with atmospheric O2 to make HO2 in a direct, one-step ‘photophysical oxidation’, a mechanism likely to be general in the troposphere.

    • Blair A. Welsh
    • , Maggie E. Corrigan
    •  & Scott H. Kable

  • Article
    | Open Access

    Allostery produces concerted functions of protein complexes by orchestrating the cooperative work between the constituent subunits. By restoring functions of pseudo-active sites that have been lost through evolution, allosteric sites have now been designed into a rotary molecular motor, V1-ATPase, resulting in its rotation being boosted allosterically.

    • Takahiro Kosugi
    • , Tatsuya Iida
    •  & Nobuyasu Koga

  • In Your Element |

    Martin Johansen and Abhik Ghosh reflect on the unusual chemistry of carbones — whose central carbon atom bears two lone pairs — and their role as double-dative ligands.

    • Martin A. L. Johansen
    •  & Abhik Ghosh

  • News & Views |

    Pharmacologically inactive prodrugs that can be activated by near-infrared light are attractive candidates for clinical applications. Now, platinum-based photo-oxidants have been shown to eradicate tumours in mice with a new mode of action.

    • Gloria Vigueras
    •  & Gilles Gasser

  • News & Views |

    The concepts of multistep processes and regioselectivity — fundamental in covalent synthesis — have now been applied to the non-covalent synthesis of sequence-controlled multiblock supramolecular polymers.

    • Ghislaine Vantomme

  • Comment |

    Fires are relatively common yet underreported occurrences in chemical laboratories, but their consequences can be devastating. Here we describe our first-hand experience of a savage laboratory fire, highlighting the detrimental effects that it had on the research group and the lessons learned.

    • Mitchell P. Jones
    • , Kathrin Weiland
    •  & Alexander Bismarck

  • Article
    | Open Access

    Inspired by the design of peptide and nucleic acid sequences to adopt particular three-dimensional shapes, natural glycan motifs have now been combined to construct a glycan that adopts a hairpin conformation in water. Thus a designed glycan can now autonomously fold into a stable secondary structure absent in nature.

    • Giulio Fittolani
    • , Theodore Tyrikos-Ergas
    •  & Martina Delbianco

  • Article |

    Scandium is challenging and expensive to isolate in pure form using conventional solvent extraction. Now a covalent organic framework (COF) has been synthesized that can incorporate scandium coordination complexes; subsequent removal of the scandium ions generates open coordination sites, and the resulting ‘metal-imprinted’ COF can be used for highly selective, cyclable scandium capture.

    • Ye Yuan
    • , Yajie Yang
    •  & Guangshan Zhu

  • Article |

    The design and construction of a stereo-defined DNA-encoded chemical library, featuring the four different 4-amino-proline stereoisomers as a central scaffold, has now enabled the discovery of potent ligands to proteins of pharmaceutical interest. Parallel screening with closely related isoforms (anti-targets) facilitated the isolation of hits with high selectivity ratios.

    • Sebastian Oehler
    • , Laura Lucaroni
    •  & Gabriele Bassi

  • Article
    | Open Access

    An enzymatic reaction installs endogenous β-amino acids in proteins with unique reactivity. Now it has been shows that this reaction can be used for site-specific modification with tetrazine dienophiles to introduce labels onto target proteins. Applications include generation of a radiolabel chelator-modified Her2-binding Affibody and intracellular, fluorescently labelled cell division protein FtsZ.

    • Daniel Richter
    • , Edgars Lakis
    •  & Jörn Piel

  • Article |

    Aluminium and silicon, two Earth-abundant, well-understood elements, typically form weak Al–Si bonds. Now, complexes featuring an anionic Al–Si core stabilized by bulky substituents and a Si–Na interaction have been isolated. This Al–Si interaction possesses partial double bond character, which can be increased by sequestration of the sodium counterion.

    • Moritz Ludwig
    • , Daniel Franz
    •  & Shigeyoshi Inoue

  • Article |

    Visualizing single-molecule reactions using electron microscopy can be difficult because of potential radiation damage from the electron beam. Now, however, it has been shown that a high-energy electron beam can be used to synthesize metallo-azafullerenes. Atomic-resolution, time-resolved transmission electron microscopy, with the help of computational calculations, is used to monitor the metal-encapsulation dynamics.

    • Helen Hoelzel
    • , Sol Lee
    •  & Dominik Lungerich

  • News & Views |

    Lactams and pyridines are privileged scaffolds, but strategies for combining these groups into one molecule are lacking. Now, N–N pyridinium ylides have been shown to form triplet state diradicals under photoinduced energy transfer, and subsequent [3+2] cycloaddition with the tethered alkene enables the synthesis of diverse ortho-pyridyl lactams.

    • Peng-Zi Wang
    •  & Jia-Rong Chen

  • Article |

    The morphan core is central to strychnan alkaloid synthesis and is typically formed during the middle or later stages of the process. Now it has been shown that an allene/ketone-equipped morphan core can be constructed early in the synthesis through ketone α-allenylation and then used to introduce other rings and functionalities, enabling access to nine targets including strychnine and geissolosimine.

    • Wenqiang Zhou
    • , Song Xi
    •  & Min Zhang

  • Article |

    There is currently a lack of effective synthetic strategies for combining lactams and pyridines within a single molecular structure. Now, diastereoselective pyridyl lactamization has been developed using a photoinduced [3+2] cycloaddition of triplet diradical N–N pyridinium ylides with pendant alkenes. This method provides a useful synthon for preparing pyridyl γ- and δ-lactam scaffolds with syn-configuration.

    • Wooseok Lee
    • , Yejin Koo
    •  & Sungwoo Hong

  • Article |

    Stabilization of RNAs for storage, transport and biological application remains a profound challenge. Now, it has been shown that reversible 2′-OH acylation with easily accessible acylimidazoles unlocks efficient protection of RNA. RNA can be deprotected by non-basic nucleophiles or spontaneously in cells to restore RNA functions.

    • Linglan Fang
    • , Lu Xiao
    •  & Eric T. Kool

  • Research Briefing |

    Challenges in the synthesis of heparan sulfate (HS) glycosaminoglycans have limited access to defined HS oligosaccharides bearing a diverse array of sulfation sequences. A concise, divergent synthetic approach now provides a library of 64 HS tetrasaccharides displaying a comprehensive set of sulfation sequences, offering insight into the elusive sulfation code of glycosaminoglycans.

  • Article |

    Traditionally, ozone has been primarily used to oxidatively deconstruct carbon–carbon bonds. Now, it has been shown that ozone can be used for the construction of carbon–oxygen bonds without oxidative cleavage of the olefin substrate through capturing primary ozonides. Furthermore, intercepting primary ozonides with nucleophiles in continuous flow enabled the green, syn-dihydroxylation of olefins to be realized.

    • Danniel K. Arriaga
    •  & Andy A. Thomas

  • Article |

    Conventional photo-driven cancer treatment agents require oxygen and visible light to induce cell death, limiting their efficacy in deep, oxygen-poor tumours. Now, a class of NIR-activatable Pt(IV) photooxidants that target the endoplasmic reticulum have been shown to effectively overcome these limitations by directly oxidizing intracellular biomolecules in an oxygen-independent fashion, presenting a promising new direction for next-generation metal-based drug development.

    • Zhiqin Deng
    • , Huangcan Li
    •  & Guangyu Zhu

  • Article |

    Large collections of defined glycosaminoglycan (GAG) structures have been synthetically challenging to obtain but are required to understand this important class of biomolecules. Now, an efficient platform for synthesizing large libraries of heparan sulfate oligosaccharides has been developed, providing a detailed view into the sulfation code of GAGs.

    • Lei Wang
    • , Alexander W. Sorum
    •  & Linda C. Hsieh-Wilson

  • Article |

    Exciton–exciton annihilation is conventionally assumed to be limited by diffusion. Now, using time-resolved photoluminescence microscopy to determine exciton diffusion constants and annihilation rates in two substituted perylene diimide aggregates, along with a microscopic model, it has been shown that annihilation can be suppressed through quantum interference of the spatial phase of delocalized excitons.

    • Sarath Kumar
    • , Ian S. Dunn
    •  & Libai Huang

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