Chemical engineering articles within Nature Chemistry

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  • 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

  • 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

  • Article |

    Cells spatially organize biochemical reactions within membrane-bound and membraneless compartments. The extent to which intrinsically disordered proteins themselves can form discrete compartments or condensed phases is poorly understood. Now a pair of model IDRs that display orthogonality in condensation and the chain features governing selective assembly have been identified.

    • Rachel M. Welles
    • , Kandarp A. Sojitra
    •  & Matthew C. Good

  • Article |

    The heterogeneous catalytic dehydrogenation of hydrocarbons usually suffers from a negative pressure dependence on H2. Now it has been shown that for propane dehydrogenation on gallium oxide-based catalysts, a positive activity dependence on H2 partial pressure arises from a metastable hydride-mediated catalysis in which gallium hydrides promote C–H activation.

    • Guodong Sun
    • , Zhi-Jian Zhao
    •  & Jinlong Gong

  • Article
    | Open Access

    Late-stage functionalization of complex drug molecules is challenging. To address this problem, a discovery platform based on geometric deep learning and high-throughput experimentation was developed. The computational model predicts binary reaction outcome, reaction yield and regioselectivity with low error margins, enabling the functionalization of complex molecules without de novo synthesis.

    • David F. Nippa
    • , Kenneth Atz
    •  & Gisbert Schneider

  • News & Views |

    Gas bubble accumulation at interfaces is a barrier to achieving more efficient electrochemical devices. A clever model system to understand bubble formation during electrochemical hydrogen evolution now reveals similarities between the forces at play during their detachment from the catalyst surface and those involved in wine climbing up a glass.

    • Gaurav Ashish Kamat
    •  & Michaela Burke Stevens

  • 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

  • Article |

    The advantages and disadvantages of building a nanosystem using one, two or more molecular components are poorly understood. Now, using structural and catalytic DNA-based nanosystems and theoretical simulations, it has been shown that the assembly of trimeric nanosystems displays much higher levels of programmability and functionality than the monomeric or dimeric counterparts.

    • D. Lauzon
    •  & A. Vallée-Bélisle

  • Article |

    Automated systems, nowadays more commonly used in laboratory settings, are typically fixed to a narrow set of reactions and used within a complex laboratory environment. Now, a portable platform has been developed for the on-demand and on-site multistep synthesis of organic molecules, oligonucleotides and oligopeptides mapped into reactionware systems.

    • J. Sebastián Manzano
    • , Wenduan Hou
    •  & Leroy Cronin

  • News & Views |

    Aqueous organic redox flow batteries are promising for low-cost and large-scale energy storage, but the redox-active molecules they rely on degrade prematurely. Now, a facile electrochemical protocol to regenerate them has been proposed, resulting in extended battery lifetimes.

    • Antoni Forner-Cuenca

  • News & Views |

    A grand challenge for bio-based plastics is the ability to cost-effectively manufacture high-performance polymers directly from renewable resources that are also recyclable-by-design. A one-step conversion of xylose to polyesters has been reported, combining a sustainable lifecycle with impressive materials performance.

    • Robin M. Cywar
    •  & Gregg T. Beckham

  • Article |

    Synthetic chemical networks with far-from-equilibrium dynamics akin to genetic regulatory networks in living cells could precisely regulate the kinetics of chemical synthesis or self-assembly. Now standardized excitable chemical regulatory elements, termed genelets, that enable predictive bottom-up construction of in vitro networks with designed temporal and multistable behaviour have been developed.

    • Samuel W. Schaffter
    • , Kuan-Lin Chen
    •  & Rebecca Schulman

  • Article |

    Aqueous organic redox flow batteries offer a safe and inexpensive solution to the problem of storing electricity produced from intermittent renewables. However, decomposition of the redox-active organic molecules that they rely on limits their lifetimes, preventing commercialization. Now it has been shown that these redox molecules can be electro-recomposed in situ, rejuvenating their function.

    • Yan Jing
    • , Evan Wenbo Zhao
    •  & Michael J. Aziz

  • Article |

    The cost-effective use of platinum as a catalyst has led to an evolving set of systems ranging from nanoparticles to single atoms on a variety of solid supports. It has now been shown that the dissolution of platinum atoms in a liquid gallium matrix generates a liquid catalyst that functions at low temperature with high activity.

    • Md. Arifur Rahim
    • , Jianbo Tang
    •  & Kourosh Kalantar-Zadeh

  • News & Views |

    Understanding how surface structure affects catalyst selectivity is limited by the ability to synthesize atomically precise active-site ensembles. Now, by using intermetallic Pd–Zn, a series of well-defined multinuclear Pd–metal–Pd catalytic sites have been generated and studied, providing insights into their selectivity for the semi-hydrogenation of acetylene.

    • Max Mortensen
    •  & Siris Laursen

  • Review Article |

    Enzymes, either purified or as whole-cell biocatalysts, can be concatenated into catalytic cascades and used to produce pharmaceutically relevant molecules. This Review discusses the advantages and requirements of multistep enzyme cascades and also highlights how they can be harnessed to achieve highly sustainable and cost-efficient syntheses.

    • Ana I. Benítez-Mateos
    • , David Roura Padrosa
    •  & Francesca Paradisi

  • Article |

    Advances in the design of heterogeneous catalysts are limited by our ability to synthesize atomically precise active-site ensembles. Now, the controlled synthesis of Pd–M–Pd catalytic sites (M = Zn, Pd, Cu, Ag and Au) has been demonstrated. Stoichiometric control identifies that Pd–Pd–Pd sites are active for ethylene hydrogenation, whereas Pd–Zn–Pd sites are not.

    • Anish Dasgupta
    • , Haoran He
    •  & Robert M. Rioux

  • News & Views |

    Innovations in instrumentation together with new strategies of data collection and processing have been shown to solve the problem of data quality for time-resolved in situ X-ray diffraction studies on ball milling, opening new horizons in mechanochemistry.

    • Elena Boldyreva

  • Article |

    Automated synthesis technologies are often highly specialized, focusing only on a narrow set of reaction classes. Now, solid-phase peptide synthesis, iterative Suzuki–Miyaura cross-coupling and diazirine chemistry have all been automated using the same universal platform architecture. A convergent 12-step synthesis demonstrates the utility of the reported Chemputer system.

    • Davide Angelone
    • , Alexander J. S. Hammer
    •  & Leroy Cronin

  • News & Views |

    Interactions between two bodies that are both attractive and repulsive — such as predators chasing prey — are common in nature. Similar chasing behaviour has now been engineered in self-propelling microdroplets and controlled through fundamental physical and chemical mechanisms.

    • Corinna C. Maass

  • Article |

    Artificial intrinsically disordered proteins (A-IDPs) have now been shown to form exclusionary, intracellular droplets that can be designed using simple principles that are based on the aromatic/aliphatic ratio and molecular weight. Droplets that sequester an enzyme and modulate enzyme efficiency on the basis of the molecular weight of the A-IDPs were also engineered using A-IDPs as a minimal condensate scaffold.

    • Michael Dzuricky
    • , Bradley A. Rogers
    •  & Ashutosh Chilkoti

  • Article |

    A stable zinc-based metal–organic framework known to retain its porosity and crystallinity after exposure to moisture has been shown to undergo structural changes at the molecular level on adsorbing water. This dynamic and reversible response to the presence of water, including the rearrangement of bonds, is suggested to be the reason for the hydrolytic stability of this particular metal–organic framework.

    • Nicholas C. Burtch
    • , Ian M. Walton
    •  & Krista S. Walton

  • Article |

    The electroreduction of CO2-derived CO is a promising technology for the sustainable production of value-added chemicals. Now, it is shown how C–N bonds can be formed electrochemically through CO electroreduction on a Cu surface in the presence of amines. The formation of acetamides is observed through nucleophilic addition to a ketene intermediate.

    • Matthew Jouny
    • , Jing-Jing Lv
    •  & Feng Jiao

  • Article |

    Conventional chemical reactors are subject to the equilibrium limitations imposed by the overall reaction. It has now been shown that this limitation can be overcome if reactants are fed separately to a reactor and a non-stoichiometric oxygen carrier is used to transfer both oxygen and key chemical information across a reaction cycle.

    • Ian S. Metcalfe
    • , Brian Ray
    •  & John S. O. Evans

  • Article |

    While much effort has been devoted to understanding how nanoparticle morphology can be leveraged to improve catalytic activity, engineering their microstructure from first principles to this end has remained difficult. Now a methodology for designing the optimal structure of a solid catalyst with the aim of achieving the highest possible activity for surface-sensitive reactions has been developed.

    • M. Núñez
    • , J. L. Lansford
    •  & D. G. Vlachos

  • Article |

    Symmetrical protein oligomers perform key structural and catalytic functions in nature, but engineering such oligomers synthetically is challenging. Now, oppositely supercharged synthetic variants of normally monomeric proteins have been shown to assemble via specific, introduced electrostatic contacts into symmetrical, highly well-defined oligomers.

    • Anna J. Simon
    • , Yi Zhou
    •  & Andrew D. Ellington

  • Article |

    The creation of a viable technology that enables precise control over the monomer sequence in synthetic polymers remains a significant challenge. High-purity sequence-defined polyethers with readily tailored side-chain functionalities have now been made through liquid-phase iterative synthesis combined with size-exclusion molecular sieving and real-time monitoring.

    • Ruijiao Dong
    • , Ruiyi Liu
    •  & Andrew G. Livingston

  • Article |

    Chemically depolymerizing biomass polysaccharides to simple sugars is often controlled by the balance between depolymerization and degradation kinetics, which has limited the concentration of solutions that can be obtained and overall yields. The reversible stabilization of carbohydrates by acetal formation pushes back these limits and creates stabilized sugars that have advantageous properties for further upgrading.

    • Ydna M. Questell-Santiago
    • , Raquel Zambrano-Varela
    •  & Jeremy S. Luterbacher

  • Article |

    Membranes with high selectivity and high permeance that allows rapid passage of solvent molecules are desirable for efficient separation processes. Microporous conjugated-polymer membranes have now been fabricated through surface-initiated polymerization. These membranes are capable of ultrafast organic-solvent nanofiltration because of the high porosity and pore interconnectivity originating from the rigid skeleton.

    • Bin Liang
    • , Hui Wang
    •  & Zhiyong Tang

  • Article |

    As of yet, no clear structure–performance descriptors have been developed to tune the catalytic activity of zeolitic methanol-to-olefin catalysts. Now it has been shown that introducing Lewis acidity into Brønsted acidic zeolites boosts their performance. Although Brønsted acidity is found to define propylene selectivity, Lewis acidity is responsible for prolonging lifetime.

    • Irina Yarulina
    • , Kristof De Wispelaere
    •  & Jorge Gascon

  • Article |

    Isotope effects provide deep insight into mechanisms of chemical and biochemical processes. Now, it has been shown that the pattern of isotopic substitution of the isomerizing bond of the retinal chromophore in the visual pigment rhodopsin significantly alters the reaction quantum yield—revealing a vibrational phase-dependent isotope effect.

    • C. Schnedermann
    • , X. Yang
    •  & R. A. Mathies

  • Article |

    Understanding how a supporting material can change the surface chemistry of the nanoparticle catalysts that it hosts is critical to tuning catalytic properties. Experimental Hammett studies and density functional theory calculations show that differences in reactivity can be attributed to differences in the electron density at metal active sites, which arises from differences in electron donation from the support.

    • Gaurav Kumar
    • , Luke Tibbitts
    •  & Bert D. Chandler

  • Article |

    A practical realization of selective IR-driven reaction-rate control has been hampered by competing processes leading to sample heating. Now, the acceleration of a bimolecular ground-state reaction in solution using the IR excitation of a vibration connected to the reaction coordinate is demonstrated. The behaviour is monitored and understood using a combination of femtosecond IR-pump IR-probe spectroscopy and theoretical calculations.

    • Till Stensitzki
    • , Yang Yang
    •  & Karsten Heyne

  • Article |

    Creating systems that merge some of the advantages of both heterogeneous and molecular catalysis is a useful approach to developing improved catalysts. Following this strategy, a liquid mixture of gallium and palladium supported on porous glass has now been shown to form an active catalyst for alkane dehydrogenation that is resistant to coke formation and is thus highly stable.

    • N. Taccardi
    • , M. Grabau
    •  & P. Wasserscheid

  • Article |

    A programmable model of membraneless organelles comprised of intrinsically disordered proteins (IDPs) containing sequences of low complexity has now been developed. The rules governing the assembly of archetypal IDPs into biologically inspired mixed, layered and size-controlled configurations provides a new means for understanding intracellular phase behaviour of IDPs.

    • Joseph R. Simon
    • , Nick J. Carroll
    •  & Gabriel P. López

  • Article |

    Efficiently and selectively activating the C–H bonds within the light alkanes of natural gas is a challenge that must be overcome if we are to make the most of Earth's abundant reserves. An oxybromination method that functionalizes methane under mild conditions has now been developed and vanadium phosphate was identified as the best catalyst for this reaction.

    • Vladimir Paunović
    • , Guido Zichittella
    •  & Javier Pérez-Ramírez

  • Commentary |

    Developing cleaner chemical processes often involves sophisticated flow-chemistry equipment that is not available in many economically developing countries. For reactions where it is the data that are important rather than the physical product, the networking of chemists across the internet to allow remote experimentation offers a viable solution to this problem.

    • Ryan A. Skilton
    • , Richard A. Bourne
    •  & Martyn Poliakoff

  • News & Views |

    Creating chemical systems that can model living systems is far from easy. However, the evolution of oil droplets in water through the application of artificial selective pressure to produce droplets with dramatically different — yet specific — behaviours, is an encouraging step in this direction.

    • Andrew J. Bissette
    •  & Stephen P. Fletcher

  • Article |

    Substituted aspartic acids are highly valuable as tools for biological research and as chiral building blocks for pharmaceuticals. Here, engineering of the enzyme methylaspartate ammonia lyase to accept a large variety of substituted amines and fumarates and catalyse the asymmetric synthesis of aspartic acid derivatives is described.

    • Hans Raj
    • , Wiktor Szymański
    •  & Gerrit J. Poelarends

  • Article |

    A low-cost 3D printer is used to combine chemical reactions and the reactor to produce an active ‘reactionware’ system for organic and inorganic synthesis. Active elements such as catalysts can be incorporated into the walls of printed reactors, and other printed-in components that enable electrochemical and spectroscopic analysis can also be included.

    • Mark D. Symes
    • , Philip J. Kitson
    •  & Leroy Cronin

  • Perspective |

    When cells interact with an artificial surface, the result is a rapidly evolving and complex interface. This Perspective discusses how expressing the properties of both the cell and the substrate in chemical terms can aid in future material design. We also explore the importance of using multifunctional surfaces with quantitative, dynamic capabilities.

    • Morgan D. Mager
    • , Vanessa LaPointe
    •  & Molly M. Stevens

  • Article |

    The reaction of enols and enolates with electrophiles is used extensively in synthesis. Here, protein engineering — substituting amino acid residues in an enzyme active site — is used to produce biocatalysts for the control of enolate chemistry. The adapted enzymes enable stereoselective C–C bond formation yielding N-heterocycles in high diastereomeric excess by the reaction of trisubstituted-enolates.

    • Refaat B. Hamed
    • , J. Ruben Gomez-Castellanos
    •  & Christopher J. Schofield

  • Article |

    The co-existence of superconductivity and magnetism in single compounds is rare, and heterostructures containing both properties have only been made with complex techniques. Now, a molecular-building-block approach has been applied to match organic and inorganic layers to produce multifunctional materials.

    • Eugenio Coronado
    • , Carlos Martí-Gastaldo
    •  & Peter J. Baker

  • Article |

    A Lewis-acid-catalysed 1,3-dipolar cycloaddition provides rapid access to a variety of substituted spirooxindoles. Initial cellular evaluations supports the view that compound collections based on natural-product-inspired scaffolds constructed with complex stereochemistry, and decorated with assorted substituents, will be a rich source of compounds with diverse bioactivity.

    • Andrey P. Antonchick
    • , Claas Gerding-Reimers
    •  & Herbert Waldmann

  • Article |

    Usable electronic devices exploiting the attractive properties of graphene will require narrow ‘nanoribbons’ of the atom-thin carbon sheets. Ribbons narrower than 5 nm are desirable for effective devices, but conventional lithography is limited to 20 nm. Now, a gas-phase chemical approach for etching graphene from the edges has produced graphene nanoribbons below 5 nm.

    • Xinran Wang
    •  & Hongjie Dai

  • Article |

    Although fullerenes have been synthesized from graphite for a long time, the exact mechanism is relatively unknown. Now, in situ microscopy and quantum chemical modelling have directly followed the formation of fullerenes from a single graphitic sheet — graphene.

    • Andrey Chuvilin
    • , Ute Kaiser
    •  & Andrei N. Khlobystov

  • Research Highlights |

    Charge transport through electron hopping has been observed between π–π stacked perylene derivatives incorporated into DNA hairpin scaffolds.

    • Anne Pichon

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