Research articles

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  • Despite the central role that the solid electrolyte interphase plays on the efficiency of Li-ion batteries, little is known about its formation mechanism. It is now shown that LiF forms on graphite anodes as a result of the electrocatalytic transformation of HF impurities present in the electrolyte.

    • Dusan Strmcnik
    • Ivano E. Castelli
    • Nenad M. Markovic
  • Plasma catalysis holds promise for overcoming the limitations of conventional catalysis. Now, a kinetic model for ammonia synthesis is reported to predict optimal catalysts for use with plasmas. Reactor measurements at near-ambient conditions confirm the predicted catalytic rates, which are similar to those obtained in the Haber–Bosch process.

    • Prateek Mehta
    • Patrick Barboun
    • William F. Schneider
  • Morphological changes in catalyst structure are known to occur during electrocatalysis, and understanding such changes is important to gain insight into the catalytic process. Now, in the case of iridium oxide, these surface changes are probed in atomic-scale detail during the oxygen evolution reaction, and correlated with activity and stability.

    • T. Li
    • O. Kasian
    • K. J. J. Mayrhofer
  • Electrochemical routes for the production of hydrogen peroxide would reduce the waste inherent in the current anthraquinone process, and also make distributed and on-site production more feasible. Here, inexpensive reduced graphene oxide is proven to be a stable and selective catalyst for oxygen reduction at remarkably low overpotentials.

    • Hyo Won Kim
    • Michael B. Ross
    • Bryan D. McCloskey
  • Aminocarboxylic acids are used in a broad range of domestic products and industrial applications. Here, Poelarends and co-workers report a chemoenzymatic route for the asymmetric synthesis of the antibiotic co-drug candidate aspergillomarasmine A and related aminocarboxylic acids by exploiting the broad substrate promiscuity of ethylenediamine-N,N′-disuccinic acid (EDDS) lyase.

    • Haigen Fu
    • Jielin Zhang
    • Gerrit J. Poelarends
  • For practical applications, water-oxidation catalysts should be inexpensive, active and stable. Here, Cronin and co-workers dope molybdenum into the Weakley sandwich-type polyoxometalate, showing that this dramatically lowers the overpotential for the oxygen evolution reaction while maintaining the stability against oxidation.

    • Mercè Martin-Sabi
    • Joaquín Soriano-López
    • Leroy Cronin
  • Selective catalytic reduction is employed at the exhaust of diesel vehicles to abate nitrogen oxide emissions. Now, guided by time-resolved X-ray absorption spectroscopy and transient experiments using Cu-SSZ-13 as the catalyst, the authors unravel important features of the reaction mechanism that allow the performance of the catalyst to be improved.

    • Adrian Marberger
    • Andrey W. Petrov
    • Davide Ferri
  • Single-atom catalysts are of growing importance, but the nature of their structure and reactivity remains under debate. Here, Sykes and co-workers show that single Pt atoms on a well-defined Cu2O surface are capable of performing low-temperature CO oxidation, and provide data on the binding site and electronic structure of the Pt atoms.

    • Andrew J. Therrien
    • Alyssa J. R. Hensley
    • E. Charles H. Sykes
  • Small metal nanoclusters often display high catalytic activity, but also low stability due to aggregation. Here, Xu and co-workers show that subnanometre Pd clusters can be contained within porous organic cages. Not only do the particles retain high catalytic activity, they also show excellent solubility and stability.

    • Xinchun Yang
    • Jian-Ke Sun
    • Qiang Xu
  • The choice of solvent system has important implications regarding the catalytic upgrading of carbohydrate-containing biomass. Here, Dumesic and co-workers study solvation effects in organic solvent/water mixtures and employ the obtained information to control the rate and selectivity of the acid-catalysed dehydration of fructose.

    • Max A. Mellmer
    • Chotitath Sanpitakseree
    • James A. Dumesic
  • While methods for arylation of amines are well established, alkylation is a less well-developed process. Here, Hu and co-workers report amine alkylation using redox-active esters, using a combination of photoredox catalysis to generate the active electrophile and copper catalysis for the cross-coupling.

    • Runze Mao
    • Adrian Frey
    • Xile Hu
  • Zeolite-catalysed alkylations of phenolic compounds offer unique possibilities for the valorization of renewable aromatics into substituted arenes. Now, a mechanistic study reveals that the course of the reaction can be dramatically altered by changing the polarity of the solvent, which affects the nature of surface species and the pathway for the generation of the alkylating electrophile.

    • Yuanshuai Liu
    • Eszter Baráth
    • Johannes A. Lercher
  • Understanding structure sensitivity—how the structural morphology of a surface influences a catalytic reaction—is important for rational catalyst design. Here, the synthesis and in-depth characterization of a range of size-defined nickel clusters shows the structure sensitivity of CO2 hydrogenation, and also identifies two size-dependent reaction pathways.

    • Charlotte Vogt
    • Esther Groeneveld
    • Bert M. Weckhuysen
  • Ammonia synthesis is an energy-intensive process due to the high activation barrier for N2 dissociation. Here, Hosono and co-workers show that the intermetallic compound LaCoSi can lower the energy requirement for N2 activation and shift the rate-determining step of the process to NH x formation under mild conditions.

    • Yutong Gong
    • Jiazhen Wu
    • Hideo Hosono
  • Bifunctional heterogeneous catalysts are usually prepared by dispersion of a metal on an acidic or basic support. Now a method has been developed to post-functionalize a catalyst and introduce tunable acidity by coating an organic acid layer on the support, resulting in improved performance as showcased for selected hydrodeoxygenation reactions.

    • Jing Zhang
    • Lucas D. Ellis
    • J. Will Medlin
  • Electrocatalytic reduction of CO2 to products containing multiple carbon atoms is useful for producing high-value chemicals and fuels. This work uses theory to predict the preferred copper surface for C–C coupling, and subsequent metal ion cycling to produce the desired facets results in a catalyst that is highly selective for C2+ products.

    • Kun Jiang
    • Robert B. Sandberg
    • Haotian Wang
  • Catalysts that can selectively reduce carbon dioxide to C2+ products are attractive for the generation of more complex and useful chemicals. Here, an electro-redeposited copper catalyst is shown to provide excellent selectivity and high current density for ethylene formation. Detailed characterization and theory link the performance to the catalyst morphology.

    • Phil De Luna
    • Rafael Quintero-Bermudez
    • Edward H. Sargent
  • The direct synthesis of hydrogen peroxide via oxygen reduction is an attractive alternative to the anthraquinone process. Here, a general trend linking oxygenation of carbon surfaces with electrocatalytic performance in peroxide synthesis is demonstrated, and computational studies provide further insight into the nature of the active sites.

    • Zhiyi Lu
    • Guangxu Chen
    • Yi Cui
  • Hydrogenation is one of the most common catalytic processes on both laboratory and industrial scales, and typically is carried out with a noble metal catalyst. Here, the authors show that alkaline earth metal amides are capable of hydrogenating imines under mild conditions.

    • Heiko Bauer
    • Mercedes Alonso
    • Sjoerd Harder