2021 Top 25 Chemistry and Materials Sciences Articles

Research highlights

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  Mechanochemical synthesis of magnesium-based carbon nucleophiles in air and their use in organic synthesis

  Grignard reagents have widespread utility in organic chemistry, but their preparation is limited by several drawbacks, such as the use of dry organic solvents and long reaction times. Here, the authors report a general mechanochemical synthesis of Grignard reagents in paste form in air, using a ball milling technique.

  • Rina Takahashi
  • Anqi Hu
  • Hajime Ito

  ArticleOpen Access18 Nov 2021 Nature Communications
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  Programmable microbial ink for 3D printing of living materials produced from genetically engineered protein nanofibers

  Living cells can precisely assemble to build 3D functional architectures. Here the authors produce an extrudable microbial ink entirely from the engineered cells, which can be further programmed to 3D print functional living materials.

  • Anna M. Duraj-Thatte
  • Avinash Manjula-Basavanna
  • Neel S. Joshi

  ArticleOpen Access23 Nov 2021 Nature Communications
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  A novel mechanism for the loss of mRNA activity in lipid nanoparticle delivery systems

  Lipid nanoparticle delivery of mRNA vaccines has become of particular importance, however, mRNA stability is a major concern. Here, the authors report on a study of lipid impurity mRNA interactions using reverse phase ion pair HPLC to identify reactions which render the mRNA untranslatable, reducing vaccine efficiency.

  • Meredith Packer
  • Dipendra Gyawali
  • Phil White

  ArticleOpen Access22 Nov 2021 Nature Communications
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  Understanding Li-based battery materials via electrochemical impedance spectroscopy

  Electrochemical impedance spectroscopy is a key technique for understanding Li-based battery processes. Here, the authors discuss the current state of the art, advantages and challenges of this technique, also giving an outlook for future developments.

  • Miran Gaberšček

  CommentOpen Access11 Nov 2021 Nature Communications
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  A general strategy for C(sp³)–H functionalization with nucleophiles using methyl radical as a hydrogen atom abstractor

  When carbon-based units are functionalized in photoredox catalysis, electrophilic coupling partners are often used, such that the polarities of the two fragments are appropriately matched. Here the authors show a generalized methodology to instead use nucleophilic coupling partners, which are cheaper and often simpler, via successive hydrogen atom transfer and oxidative radical-polar crossover.

  • Isabelle Nathalie-Marie Leibler
  • Makeda A. Tekle-Smith
  • Abigail G. Doyle

  ArticleOpen Access29 Nov 2021 Nature Communications
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  Identifying molecules as biosignatures with assembly theory and mass spectrometry

  The search for life in the universe is difficult due to issues with defining signatures of living systems. Here, the authors present an approach based on the molecular assembly number and tandem mass spectrometry that allows identification of molecules produced by biological systems, and use it to identify biosignatures from a range of samples, including ones from outer space.

  • Stuart M. Marshall
  • Cole Mathis
  • Leroy Cronin

  ArticleOpen Access24 May 2021 Nature Communications
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  Tempering of cocoa butter and chocolate using minor lipidic components

  In chocolate production, a complicated tempering process is used to guide the crystallization of cocoa butter towards its most desirable polymorph, which gives the chocolate proper melting behavior, gloss, and snap—hallmarks of good quality chocolate. Here, the authors find that simply adding a specific phospholipid also directs crystallization towards this polymorph, producing chocolate with comparable microstructure and properties to tempered chocolate.

  • Jay Chen
  • Saeed M. Ghazani
  • Alejandro G. Marangoni

  ArticleOpen Access31 Aug 2021 Nature Communications
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  Production of high-energy Li-ion batteries comprising silicon-containing anodes and insertion-type cathodes

  Large-scale manufacturing of high-energy Li-ion cells is of paramount importance for developing efficient rechargeable battery systems. Here, the authors report in-depth discussions and evaluations on the use of silicon-containing anodes together with insertion-based cathodes.

  • Gebrekidan Gebresilassie Eshetu
  • Heng Zhang
  • Egbert Figgemeier

  Review ArticleOpen Access15 Sep 2021 Nature Communications
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  Proliferating coacervate droplets as the missing link between chemistry and biology in the origins of life

  Coacervate droplets (CDs) are a model for protocells formed by liquid-liquid phase separation (LLPS), but protocell models able to proliferate remain undeveloped. Here, the authors report a proliferating peptide-based CD using synthesised amino acid thioesters as monomers, which could concentrate RNA and lipids, enabling RNA to protect the droplet from dissolution by lipids.

  • Muneyuki Matsuo
  • Kensuke Kurihara

  ArticleOpen Access24 Sep 2021 Nature Communications
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  Nickel-catalyzed electrochemical carboxylation of unactivated aryl and alkyl halides with CO₂

  Electrochemistry is a promising approach to make existing chemical protocols milder, but many simple transformations of feedstocks are still out of reach. Here, the authors transform unactivated aryl and alkyl (pseudo)halides into carboxylic acids, via nickel catalysis and electricity, using atmospheric CO₂ as the carbon source.

  • Guo-Quan Sun
  • Wei Zhang
  • Da-Gang Yu

  ArticleOpen Access6 Dec 2021 Nature Communications
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  Gene editing enables rapid engineering of complex antibiotic assembly lines

  Engineering biosynthetic assembly lines is a powerful path to new natural products but is challenging with current methods. Here the authors use CRISPR-Cas9 to exchange subdomains within NRPS to alter substrate selectivity.

  • Wei Li Thong
  • Yingxin Zhang
  • Jason Micklefield

  ArticleOpen Access25 Nov 2021 Nature Communications
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  Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

  Developing green and delocalized routes for ammonia synthesis is highly important but still very challenging. Here the authors report an efficient ammonia synthesis process via nitrate reduction to ammonia on Fe single atom catalyst.

  • Zhen-Yu Wu
  • Mohammadreza Karamad
  • Haotian Wang

  ArticleOpen Access17 May 2021 Nature Communications
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  Coordination environment dependent selectivity of single-site-Cu enriched crystalline porous catalysts in CO₂ reduction to CH₄

  Crystalline porous catalysts with single Cu sites are dedicated to exploring the dependence of CO₂ electroreduction selectivity on the coordination environment of catalytic sites. The conductive MOF Cu-DBC with oxygen-coordinated Cu sites shows a high Faradaic efficiency ~80% of CO₂-to-CH₄.

  • Yu Zhang
  • Long-Zhang Dong
  • Ya-Qian Lan

  ArticleOpen Access4 Nov 2021 Nature Communications
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  6 nm super-resolution optical transmission and scattering spectroscopic imaging of carbon nanotubes using a nanometer-scale white light source

  The authors present a super-resolution hyperspectral imaging technique using a nanoscale white light source generated by superfocusing light from a tungsten-halogen lamp. They achieve 6 nm resolution, measuring longitudinal and transverse optical electronic transitions in single-walled carbon nanotubes.

  • Xuezhi Ma
  • Qiushi Liu
  • Ming Liu

  ArticleOpen Access25 Nov 2021 Nature Communications
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  Electrochemical C–N bond activation for deaminative reductive coupling of Katritzky salts

  Electrochemical transformations use electrons and electron holes instead of chemical oxidants and reductants as reagents. Here, the authors report an electrochemical reductive deaminative cross-coupling of Katrizky salts with various radical acceptors, including examples of fluoroalkenylation, alkynylation and thiolation.

  • Yeqing Liu
  • Xiangzhang Tao
  • Yi Pan

  ArticleOpen Access19 Nov 2021 Nature Communications
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  Ultra-thin self-healing vitrimer coatings for durable hydrophobicity

  By now a plethora of ultrathin hydrophobic coatings are available but their durability are not well developed. Here, the authors present a thin, durable and fluorine-free PDMS-based vitrimer coating that implements many desirable aspects like energy efficiency, durability and sustainability.

  • Jingcheng Ma
  • Laura E. Porath
  • Christopher M. Evans

  ArticleOpen Access1 Sep 2021 Nature Communications
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  A saccharide-based binder for efficient polysulfide regulations in Li-S batteries

  The long-term cycling of Li-S batteries depends on the polysulfides shuttling regulation. Here, the authors present a saccharide-based binder system to control the polysulfides migration and improve the cycle life of a Li-S pouch cell.

  • Yingyi Huang
  • Mahdokht Shaibani
  • Mainak Majumder

  ArticleOpen Access10 Sep 2021 Nature Communications
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  Sustained enzymatic activity and flow in crowded protein droplets

  Living cells can harvest environmental energy to drive chemical processes. Here the authors design a minimal artificial system that achieves steady states at similar metabolic densities to microorganisms.

  • Andrea Testa
  • Mirco Dindo
  • Paola Laurino

  ArticleOpen Access1 Nov 2021 Nature Communications
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  Freezing of few nanometers water droplets

  Ice nucleation in confined geometries is a ubiquitous phenomenon, but difficult to characterize. Here the authors investigate experimentally the freezing of water nanodroplets surrounded by octane in nanopores down to 2 nm, and demonstrate that the soft curved oil-water interface suppresses heterogeneous ice nucleation, which occurs at a lower temperature than homogenous bulk nucleation.

  • Alireza Hakimian
  • Mohammadjavad Mohebinia
  • Hadi Ghasemi

  ArticleOpen Access30 Nov 2021 Nature Communications
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  Transition metal-doped Ni-rich layered cathode materials for durable Li-ion batteries

  Long-term efficient cycling stability is of paramount importance for the development of high-energy Li-ion batteries. Here, the authors investigate the effect of transition metal dopants on the electrochemical, morphological, and structural properties of Ni-rich cathode active materials.

  • H. Hohyun Sun
  • Un-Hyuck Kim
  • Yang-Kook Sun

  ArticleOpen Access12 Nov 2021 Nature Communications
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  Divergent functionalization of aldehydes photocatalyzed by neutral eosin Y with sulfone reagents

  Acyl radicals represent a reactive species that allow for aldehyde subunits to be nucleophilic instead of their typical electrophilic behavior; however, these species are difficult to access in mild conditions. Here the authors show a method to generate acyl radicals using only an organic photocatalyst and light, and these species are shown as competent nucleophiles in a variety of couplings.

  • Jianming Yan
  • Haidi Tang
  • Jie Wu

  ArticleOpen Access10 Dec 2021 Nature Communications
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  Engineering single-atomic ruthenium catalytic sites on defective nickel-iron layered double hydroxide for overall water splitting

  Rational design of single atom catalyst is critical for efficient sustainable energy conversion. Single-atomic-site ruthenium stabilized on defective nickel-iron layered double hydroxide nanosheets achieve superior HER and OER performance in alkaline media.

  • Panlong Zhai
  • Mingyue Xia
  • Jungang Hou

  ArticleOpen Access28 Jul 2021 Nature Communications
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  Artificial intelligence-enhanced quantum chemical method with broad applicability

  Artificial intelligence is combined with quantum mechanics to break the limitations of traditional methods and create a new general-purpose method for computational chemistry simulations with high accuracy, speed and transferability.

  • Peikun Zheng
  • Roman Zubatyuk
  • Pavlo O. Dral

  ArticleOpen Access2 Dec 2021 Nature Communications
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  Controlled self-assembly of plant proteins into high-performance multifunctional nanostructured films

  Green use of plant derived proteins in functional materials has been limited by inefficient methods to control micro and nanoscale structure. Here, the authors use nanoscale assembly of water-insoluble plant proteins to make meter scale films with comparable properties to conventional plastics.

  • Ayaka Kamada
  • Marc Rodriguez-Garcia
  • Tuomas P. J. Knowles

  ArticleOpen Access10 Jun 2021 Nature Communications
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  Moving beyond bimetallic-alloy to single-atom dimer atomic-interface for all-pH hydrogen evolution

  While single, dispersed atoms enable efficient atomic utilization, controllably preparing single-atom dimers remains challenging. Here, authors prepare nickel-cobalt single-atom dimers as high-performance pH-universal H₂ evolution electrocatalysts.

  • Ashwani Kumar
  • Viet Q. Bui
  • Hyoyoung Lee

  ArticleOpen Access19 Nov 2021 Nature Communications