Chemistry articles within Nature Materials

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  • Article |

    The turn-off time is generally faster than the turn-on time in accumulation mode organic electrochemical transistors (OECTs), but the mechanism is less understood. Here the authors find different transient behaviours of turn-on and turn-off in accumulation mode OECTs, and ion transport is the limiting factor of device kinetics.

    • Jiajie Guo
    • , Shinya E. Chen
    •  & David S. Ginger

  • Article |

    Ion exchange is a powerful method to access metastable materials for energy storage, but identifying lithium and sodium interchange in layered oxides remains challenging. Using such model materials, vacancy level and corresponding lithium preference are shown to be crucial for ion exchange pathway accessibility.

    • Yu Han
    • , Weihang Xie
    •  & Chong Liu

  • News & Views |

    Pentagonal polyhedral oligomeric silsesquioxane (POSS)-based giant atoms self-assemble into Frank–Kasper phases that have not been previously observed in soft-matter systems.

    • Pengyu Chen
    •  & Kevin D. Dorfman

  • Perspective |

    Molecular materials for computing progress intensively but the performance and reliability still lag behind. Here the authors assess the current state of computing with molecular-based materials and describe two issues as the basis of a new computing technology: continued exploration of molecular electronic properties and process development for on-chip integration.

    • R. Stanley Williams
    • , Sreebrata Goswami
    •  & Sreetosh Goswami

  • Article |

    Pre-intercalation with alkali-metal ions is attractive for accessing higher reversible capacity and improved rate performance in Li-ion batteries. Topochemical single-crystal transformations in a tunnel-structured positive electrode are used to clarify the effect of pre-intercalation in modifying the host lattice and altering diffusion pathways.

    • Yuting Luo
    • , Joseph V. Handy
    •  & Sarbajit Banerjee

  • Article
    | Open Access

    Suppressed Dexter transfer is needed to achieve efficient and stable hyperfluorescence, but complex matrices must be involved. A molecular design strategy has been proposed where Dexter transfer can be substantially reduced by an encapsulated terminal emitter, leading to ‘matrix-free’ hyperfluorescence.

    • Hwan-Hee Cho
    • , Daniel G. Congrave
    •  & Hugo Bronstein

  • Article
    | Open Access

    Oxygen redox cathodes deliver higher energy densities than those based on transition metal redox but commonly exhibit voltage fade on extended cycling. The loss of O-redox capacity and voltage fade is shown to arise from a reduction in O2−/O2 redox process reversibility and O2 loss.

    • John-Joseph Marie
    • , Robert A. House
    •  & Peter G. Bruce

  • Article
    | Open Access

    Active and stable catalysts to accelerate the transition from fossil fuel to renewable feedstocks, reduce energy consumption and minimize environmental footprints are needed. Electrocatalysts based on copper nanocrystals encapsulated in hybrid alumina shells stable against structural reconstruction during CO2 electroreduction are reported.

    • Petru P. Albertini
    • , Mark A. Newton
    •  & Raffaella Buonsanti

  • News & Views |

    Considering responsive materials as transient collective assemblies rather than individual shape-changing objects allows for emergent functionalities that cannot be derived from the properties of single objects but are driven by interactions between them.

    • Arri Priimagi

  • Article |

    Soft building blocks tend to be near spherical, limiting their packing structures to those found in metallic systems. Here the authors report the spontaneous generation of highly deformed mesoatoms using molecular pentagons and observe Frank–Kasper phases not found in metal alloys.

    • Xian-You Liu
    • , Xiao-Yun Yan
    •  & Stephen Z. D. Cheng

  • Article
    | Open Access

    Although silicon anodes are promising for solid-state batteries, they still suffer from poor electrochemical performance. Chemo-mechanical failure mechanisms of composite Si|Li6PS5Cl and solid-electrolyte-free silicon anodes are now revealed and should help in designing improved electrodes.

    • Hanyu Huo
    • , Ming Jiang
    •  & Jürgen Janek

  • Article
    | Open Access

    Hydrogen produced by water splitting using renewable electricity is key to achieve net-zero carbon emissions. Decoupling hydrogen and oxygen evolution reactions during electrolysis is attractive but efficiency and operational challenges remain. A process producing hydrogen and oxygen in separate cells and supporting continuous operation in a membraneless system is now proposed.

    • Ilya Slobodkin
    • , Elena Davydova
    •  & Avner Rothschild

  • Letter |

    Multiferroics can possess multiple ferroic orders, for example, electric polarization and magnetism, and are of interest for new device applications. Here thermal control is shown to manipulate electric and magnetic orders in a single-phase quasi-two-dimensional halide perovskite.

    • Tong Zhu
    • , Xue-Zeng Lu
    •  & Hiroshi Kageyama

  • News & Views |

    An important but difficult separation, the removal of carbon monoxide from humid gas mixtures comprising oxygen, nitrogen and hydrocarbons, is addressed by exploiting Cu(I) coordination chemistry and framework flexibility.

    • Michael J. Zaworotko

  • News & Views |

    Processible centimetre-scale porous glasses using zeolitic imidazolate framework (ZIF) materials are developed, while fine-tuning of the processing conditions allows control of pore size and molecular sieving properties.

    • Georgia R. F. Orton
    •  & Neil R. Champness

  • Article
    | Open Access

    Porosity of zeolitic imidazolate frameworks can be preserved beyond glass transition and melt processing. Here centimetre-scale porous glasses are demonstrated, whereas liquid processing enables fine-tuning of the size of the gas-transporting channels for molecular sieving.

    • Oksana Smirnova
    • , Seungtaik Hwang
    •  & Alexander Knebel

  • News & Views |

    Using an electrochemical continuous flow cell, nitrogen reduction to ammonia is rigorously demonstrated through a calcium-mediated approach.

    • Michael A. Yusov
    •  & Karthish Manthiram

  • Research Briefing |

    Hybrid organic–inorganic perovskite materials have promise as the photovoltaic technology of the future. A method for spectroscopic optical control reveals how the structural dynamics and vibrations of a perovskite’s organic cations affect the electronic performance of working photovoltaic devices.

  • Research Briefing |

    Polymers made by click chemistry with spirocyclic building blocks form membranes that separate the components of crude oil based on molecular size and type, potentially using far less energy than distillation. Key enablers of this separation are moderate levels of polymer dynamic motion and frustrated chain packing.

  • Article |

    Chemical adsorption of CO on open metal sites enables separation from other gases but leads to selectivity and stability issues. Quasi-open metal sites in metal–organic frameworks are proposed here, which are accessible only by CO-induced structural transformation, enabling CO separation to 9N purity.

    • Xue-Wen Zhang
    • , Chao Wang
    •  & Jie-Peng Zhang

  • Article |

    Gold nanoclusters show promise as photothermal materials, but are often thermally unstable. Here ligand engineering is used to integrate molecular rotors with gold nanoclusters to dissipate thermal energy and improve photothermal therapy performance.

    • Jing Chen
    • , Peilin Gu
    •  & Chunhai Fan

  • Article |

    Liquid electrolytes in batteries are considered to be macroscopically homogeneous ionic transport media despite having a complex chemical composition and atomistic solvation structures. A micelle-like structure in a localized high-concentration electrolyte for which the solvent acts as a surfactant is reported.

    • Corey M. Efaw
    • , Qisheng Wu
    •  & Bin Li

  • Article |

    The rational design and assembly of colloidal quasicrystals is achieved by exploring the hybridization of nanoscale decahedra nanoparticles functionalized with DNA linkers.

    • Wenjie Zhou
    • , Yein Lim
    •  & Chad A. Mirkin

  • Editorial |

    Integrated design assisted by materials and technology innovations can help a transition from traditional to sustainable electronics.

  • Article |

    The production of ammonia via the Haber–Bosch process is carbon-intensive and centralized, but electrochemical methods such as lithium-mediated processes in organic electrolytes could enable decentralized production using renewable energy. Calcium is now shown to mediate nitrogen reduction for ammonia synthesis.

    • Xianbiao Fu
    • , Valerie A. Niemann
    •  & Ib Chorkendorff

  • Article |

    Simultaneously highly elastic and deformable gels that maintain their mechanical properties have remained elusive. Here, using in situ polymerization confined within nanochannels, the authors prepare hysteresis-free gels insensitive to crack propagation.

    • Weizheng Li
    • , Xiaoliang Wang
    •  & Feng Yan

  • Article |

    Solid polymer electrolytes are crucial for the development of lithium batteries, but their lower ionic conductivity compared with liquid/ceramics at room temperature limits their practical use. Precise positioning of designed repeating units in alternating polymer sequences now allows the Li+ conductivity to be tuned by up to three orders of magnitude.

    • Shantao Han
    • , Peng Wen
    •  & Mao Chen

  • Article |

    Membrane/catalyst systems in the oxidative coupling of methane are promising for their high product selectivity but suffer from low volumetric chemical conversion rates, high capital cost and optimizing performance. A dual-layer additive manufacturing process, based on phase inversion, is now proposed to optimize a hollow-fibre membrane/catalyst system.

    • James Wortman
    • , Valentina Omoze Igenegbai
    •  & Suljo Linic

  • Article |

    Lithium-rich nickel manganese cobalt oxide cathodes are widely explored due to their high capacities related to their anionic redox chemistry. A compositional optimization pathway for these materials investigating the variation of using cobalt and nickel now provides valuable guidelines for future high-capacity cathode design.

    • Biao Li
    • , Zengqing Zhuo
    •  & Jean-Marie Tarascon

  • News & Views |

    Quantum dots couple to form artificial molecules that allow for variable colour emission in response to an electric field.

    • James Cassidy
    • , Justin Ondry
    •  & Dmitri V. Talapin

  • Article |

    Polyethylene terephthalate (PET) tape is widely used for lithium-ion batteries but its chemical stability has been largely overlooked. Reversible self-discharge is now shown to be virtually eliminated in LiFePO4–graphite cells by replacing PET with polypropylene jellyroll tape.

    • Anu Adamson
    • , Kenneth Tuul
    •  & Michael Metzger

  • Article
    | Open Access

    Unit-cell-thick films of metal–organic frameworks with ordered porosity would be attractive for membrane applications as these thin systems combine large molecular flux with high selectivity. Here crystalline ZIF films are grown on a crystalline substrate with high H2/N2 gas separation performance.

    • Qi Liu
    • , Yurun Miao
    •  & Kumar Varoon Agrawal

  • Article |

    Trapped films of air known as plastrons are promising for underwater engineering but typically have short lifetimes. Here, aerophilic titanium alloy surfaces are developed with thermodynamically stabilized plastrons for antifouling applications.

    • Alexander B. Tesler
    • , Stefan Kolle
    •  & Wolfgang H. Goldmann

  • Article |

    Organic luminophores emit a bright near-infrared afterglow after X-ray irradiation and outperform commercially available radio sensitizers by producing higher levels of singlet oxygen, having potential applications in precision cancer theranostics.

    • Jingsheng Huang
    • , Lichao Su
    •  & Kanyi Pu

  • News & Views |

    By tracking the electrochromic doping front, a hole-limited electrochemical doping mechanism is discovered in organic mixed ionic–electronic conductors.

    • Ruiheng Wu
    • , Dilara Meli
    •  & Jonathan Rivnay

  • Article |

    Ethylene separation from ethane is the most energy-intensive separation in the chemical process industry, but so far membranes have not exceeded an ethylene/ethane selectivity of >20 in mixed gases. Here a carbon molecular sieve with an ethylene selectivity of ~100 and long-term stability under high-pressure gas is reported.

    • Khalid Hazazi
    • , Yingge Wang
    •  & Ingo Pinnau

  • News & Views |

    Photochromic molecular crystal arrays aligned in the micropores of a polymer membrane show high-performance actuation when stimulated by light. These soft composites might find applications in soft robotic devices.

    • Albert P. H. J. Schenning

  • Article |

    The development of solid-state Li-metal batteries has been limited by Li plating and stripping rates and the formation of dendrites at relevant current densities. Single-phase mixed ion- and electron-conducting garnet with comparable Li-ion and electronic conductivities is now proposed to tackle these issues.

    • George V. Alexander
    • , Changmin Shi
    •  & Eric D. Wachsman

  • Research Briefing |

    The transmission spectrum of single-molecule junctions provides fingerprint information on the charge-transport properties. A technique called single-molecule photoelectron tunnelling spectroscopy has been developed that enables mapping of the transmission spectrum beyond the highest occupied molecular orbital (HOMO)–lowest unoccupied molecular orbital (LUMO) gap at room temperature and can be used to explore the energy-dependent charge transport through single-molecule junctions.

  • Article
    | Open Access

    The two-dimensional layered crystal structure of niobium oxide polymorph T-Nb2O5 exhibits fast Li-ion diffusion that is promising for energy storage applications. Epitaxial growth of single-crystalline T-Nb2O5 thin films with ionic transport channels oriented perpendicular to the surface are now demonstrated.

    • Hyeon Han
    • , Quentin Jacquet
    •  & Stuart S. P. Parkin

  • Article
    | Open Access

    Electrochemical doping is assumed to be limited by ion motion due to large mass in mixed ionic-electronic conductors. Here, the authors reveal in a typical polythiophene that electrochemical doping speeds are limited by poor hole transport at low doping levels, leading to much slower switching speeds than expected.

    • Scott T. Keene
    • , Joonatan E. M. Laulainen
    •  & George G. Malliaras

  • Comment |

    The study of point defects in non-metallic crystals has become relevant for an increasing number of materials applications. Progress requires a foundation of consistent definitions and terminology. This Comment clarifies the underlying definitions of point defects, encourages the correct use of relative charge for their description and emphasizes their recognition as quasiparticles.

    • Roger De Souza
    •  & George Harrington

  • News & Views |

    A two-dimensional conjugated polymer is synthesized that demonstrates low electron effective masses and high mobility. These properties show that this material could act as a viable alternative to silicon-based semiconductors.

    • Shu Seki
    •  & Zhuowei Li

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