Articles

Filter By:

Article Type
  • Lithium–sulfur batteries are promising energy storage devices where catalysis can play an important role, but developing design principles for optimal performance remains a challenge. Now, a series of p-block metal sulfide cathodes are evaluated, revealing a direct correlation between the p electron gain of sulfur in the sulfide material and the apparent activation energy for the sulfur reduction reaction.

    • Wuxing Hua
    • Tongxin Shang
    • Ying Wan
    Article
  • Placing extra-framework aluminium species in the proximity of Brønsted acid sites is one of the most effective ways of tuning the energetics of zeolite-catalysed reactions. Here, using pentane cracking as an example, the authors show that grafting extra-framework silica species instead represents a valuable alternative way to modulate zeolite acitivty.

    • Ruixue Zhao
    • Rachit Khare
    • Johannes A. Lercher
    Article
  • Albicidin is a peptide antibiotic that has shown great promise for inhibiting DNA topoisomerase of fluoroquinolone-resistant Gram-negative pathogens, but its mode of action is not fully clear. Now, cryoelectron microscopy structures of albicidin–gyrase complexes provide detailed insights into the mechanism of this natural product.

    • Elizabeth Michalczyk
    • Kay Hommernick
    • Dmitry Ghilarov
    Article Open Access
  • The overall water splitting performance of semiconductor photocatalysts is often limited by recombination reactions occurring at the surface of metallic co-catalysts. Here, the authors demonstrate how the controlled deposition of aluminium oxide species on a Rh co-catalyst can strongly inhibit this phenomenon and enhance the performance of GaN–ZnO photocatalyst.

    • Zheng Li
    • Rengui Li
    • Can Li
    Article
  • Insights on the mechanistic differences between artificial metalloenzymes (ArMs) with non-native metal centres and the free cofactor or natural enzymes are scarce. Now, a detailed mechanistic analysis of a cyclopropanation reaction catalysed by such an ArM is provided, revealing intriguing differences to the natural system.

    • Brandon J. Bloomer
    • Sean N. Natoli
    • John F. Hartwig
    Article
  • Renilla luciferase is a popular bioluminescent enzyme, but the molecular details of its mechanism of action on luciferins such as coelenterazine remained elusive. Now, protein crystal structures and biochemical analyses provide an atomistic description of its catalytic mechanism.

    • Andrea Schenkmayerova
    • Martin Toul
    • Martin Marek
    Article
  • Biocatalytic methods to access thioesters, such as acyl-coenzyme A, from carboxylic acids are underdeveloped. Now, it is shown that the adenylation domain of a carboxylic acid reductase enzyme can be exploited as a promiscuous thioester synthetase and combination with acyltransferases facilitates the synthesis of amides and peptide labelling.

    • Christian Schnepel
    • Laura Rodríguez Pérez
    • Sabine L. Flitsch
    Article
  • Hydrogenolysis of unactivated C(aryl)–C(alkyl) bonds is a challenging task even in the presence of metal catalysts. Now, an approach using a boron catalyst is described that facilitates the hydrogenolysis of alkylarenes under mild conditions, and its utility is demonstrated by degrading polystyrene waste into benzene and phenylalkanes.

    • Yuliang Xu
    • Yizhou Yang
    • Huadong Wang
    Article
  • Electrocatalytic hydrogenations of organics allow water to be used as the proton source but are limited by low substrate solubility in aqueous media or by low performance in organic electrolytes. Now, a Pickering emulsion system for electrocatalytic hydrogenation is presented to overcome those issues, where the hydrogenation reaction occurs at the interface between the aqueous and organic phases.

    • Chenhui Han
    • Johannes Zenner
    • Walter Leitner
    Article Open Access
  • Activation of inert chemical bonds employing classical photocatalysts usually involves an outer-sphere single electron transfer mechanism. Now, an alternative inner-sphere single electron transfer pathway for the homolytic cleavage of strong C–Cl bonds using gold catalysts is reported.

    • Cheng-Long Ji
    • Jie Han
    • Jin Xie
    Article
  • The Birch reduction is one of the methods of choice to perform the hydrogenation of arenes, although it requires the handling of pyrophoric substances and ammonia at cryogenic temperatures. Here a photocatalytic approach based on boron carbonitride introduces the possibility to hydrogenate (hetero)arenes under mild conditions in water.

    • Tao Yuan
    • Luyang Sun
    • Xinchen Wang
    Article
  • Despite great progress in electrocatalytic CO2 reduction on Cu-based materials, the selectivity for methanol has remained elusive in contrast to thermocatalytic routes. Here, using Cu2NCN with polarized Cu atoms as the cathode, selectivity of up to 70% for methanol is achieved by favouring cleavage of Cu–O over O–C in the crucial Cu–*O–CH3 intermediate.

    • Shuyi Kong
    • Ximeng Lv
    • Fuqiang Huang
    Article
  • While the promise of low metal utilization has brought single-atom catalysts (SACs) into the spotlight, intrinsic limits in reactivity still restrict their application to a small set of reactions. Here, the authors expand the repertoire of SAC transformations with a nitrogen-doped, carbon-supported, Ru single-atom catalyst that exploits the effect of peripheral N species to promote propane dehydrogenation.

    • Yanliang Zhou
    • Fenfei Wei
    • Tao Zhang
    Article
  • Iridium catalysis can be used to achieve the challenging Z-retentive asymmetric allylic substitution reaction by trapping thermodynamically less stable anti-π-allyliridium intermediates. Now the isolation and characterization of these complexes is reported, providing hitherto elusive detailed mechanistic insights into this reaction.

    • Ru Jiang
    • Qing-Ru Zhao
    • Shu-Li You
    Article
  • Carbonyl catalysis is mainly limited to strongly activated primary amines. Now, a chiral bifunctional pyridoxal organocatalyst is developed that enables the activation of the inert α C(sp3)–H bond of NH2-unprotected benzylamines affording chiral β-aminoalcohols with high diastereo- and enantioselectivities.

    • Chengkang Hou
    • Bingfei Peng
    • Baoguo Zhao
    Article