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

  • 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 |

    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 |

    Interactions that generate directed movement in response to a chemical stimulus occur in nature but have been difficult to realize in synthetic systems. Now, it has been shown that asymmetric micelle-mediated exchange of haloalkanes can be used to create tunable chasing interactions between chemically distinct microdroplets. Collective interactions lead to the formation of droplet assemblies with emergent self-organization and collective behaviours.

    • Caleb H. Meredith
    • , Pepijn G. Moerman
    •  & Lauren D. Zarzar

  • 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 |

    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

  • 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

  • Perspective |

    The efficient engineering of nanostructures with semiconducting properties is vital to the development of organic electronics. This Perspective discusses a variety of techniques for fabricating such macromolecules, including graphene carving, the stimulus-induced synthesis of conjugated polymers and surface-assisted synthesis, and considers their potential for reproducing chemically and spatially precise molecular arrangements, that is 'molecular blueprints'.

    • Carlos-Andres Palma
    •  & Paolo Samorì

  • 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

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