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Volume 5 Issue 7, July 2022

Tracking intermediates

Gaining complete understanding of complex reaction networks is pivotal for process optimization, yet it is a very challenging endeavour. Here, Javier Pérez-Ramírez, Patrick Hemberger, Guido Zichittella and colleagues employ operando photoelectron photoion coincidence spectroscopy to monitor the mechanistic intricacies of the methanol and methyl chloride conversions to hydrocarbons on zeolite catalysts.

See Cesarini et al.

Image credit: Edvin Fako. Cover design: Marina Spence.

Research Highlights

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News & Views

  • General catalytic methods for free radical-mediated asymmetric transformations have long eluded synthetic organic chemists. Now, NAD(P)H-dependent ketoreductases are repurposed and engineered as highly efficient photoenzymes to catalyse asymmetric radical C–C couplings.

    • Rui Guo
    • Heyu Chen
    • Yang Yang
    News & Views
  • Elucidating the reaction mechanism of a catalytic process is very challenging. Now, advanced solid-state nuclear magnetic resonance experiments demonstrate the importance of oxygenates to regulate the conversion of synthesis gas over an oxide–zeolite-based bifunctional catalyst material.

    • Marc Baldus
    • Bert M. Weckhuysen
    News & Views
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Research

  • The conversions of methanol or methyl chloride over zeolite catalysts are promising processes to produce valuable hydrocarbons, but their mechanisms are still not fully understood. Now these are evaluated using operando photoelectron photoion coincidence spectroscopy, which enables the direct observation of elusive intermediates such as methyl radicals or ketene.

    • Alessia Cesarini
    • Sharon Mitchell
    • Javier Pérez-Ramírez
    Article Open Access
  • The deployment of fuel cells demands more efficient electrode–electrolyte interfaces to catalyse the oxygen reduction reaction (ORR). A kinetic ORR descriptor is put forward, which is related to the rate of the *O ↔ *OH transition and includes electrolyte effects via the role of non-specifically adsorbed anions.

    • Mingchuan Luo
    • Marc T. M. Koper
    Article Open Access
  • Alkali metal cations influence electrocatalytic reactions, but their specific role remains elusive. Now, methyl4N+ is established as a vibrational probe for surface-enhanced infrared absorption spectroscopy, revealing that alkali metal cations specifically adsorb on Au during CO2 electroreduction and that their surface coverage depends on their free energy of hydration.

    • Vincent J. Ovalle
    • Yu-Shen Hsu
    • Matthias M. Waegele
    Article
  • Conversion of CO2 to fuels or chemicals via artificial photosynthesis usually requires the assistance of organic additives or electricity. Now, a biohybrid system is reported consisting of a photocatalyst sheet and bacteria producing acetate and O2 from CO2 and H2O using sunlight as the sole energy input.

    • Qian Wang
    • Shafeer Kalathil
    • Erwin Reisner
    Article
  • Allylic amination of unactivated alkenes with aliphatic amines is a long-standing synthetic challenge in organic chemistry. This is now accomplished in an oxidant-free, site-selective process by using a combination of a photocatalyst and cobalt complex for the coupling of olefins and alkyl amines with hydrogen evolution.

    • Shengchun Wang
    • Yiming Gao
    • Aiwen Lei
    Article
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