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Volume 2 Issue 1, January 2019

Mapping bio-based chemicals

Lee and co-workers discuss metabolically engineered microbial cells to produce chemicals of interest from renewable feedstocks. Biological routes in combination with chemical routes are presented in a bio-based chemicals map — serving as a blueprint for the future design of chemical biosynthesis strategies.

See Lee et al.

Image: Sang Yup Lee and Hyun Uk Kim (Korea Advanced Institute of Science and Technology). Cover Design: Karen Moore.

Editorial

  • As we celebrate our first birthday, we thank everyone involved and look back on an exciting 12 months.

    Editorial

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Comment & Opinion

  • Developing catalytic reactions for organic synthesis is the central goal of countless research groups worldwide. High-throughput experimentation is invaluable for this pursuit, with the requisite tools becoming increasingly available to both industrial and academic research labs.

    • C. Liana Allen
    • David C. Leitch
    • Matthew A. Zajac
    Comment
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Research Highlights

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News & Views

  • Optimization of catalytic stereoselectivity for new substrates often requires a time consuming experimental process, and high-accuracy molecular modelling remains intractable for comprehensive virtual screening. Now, highly enantioselective rhodium hydrogenation catalysts have been identified using a rapid computational transition-state analysis protocol and then experimentally verified.

    • Daniel H. Ess
    News & Views
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Reviews

  • Amide bond formation is a hugely important reaction in organic synthesis. This Perspective examines the factors that influence the choice of reaction conditions for this process, comparing widely used stoichiometric reagents with catalysts. The authors draw on both academic and industrial data and focus on the efficiency, scope and sustainability of the various approaches.

    • Marco T. Sabatini
    • Lee. T. Boulton
    • Tom D. Sheppard
    Perspective
  • Production of industrial chemicals from renewable biomass feedstock plays an important role in addressing limited fossil fuel resources, climate change and environmental problems. This Review provides a comprehensive overview of biological and chemical routes for the synthesis of industrial chemicals derived from key precursor metabolites of central carbon metabolic pathways, and visualizes the results in a global bio-based chemicals map.

    • Sang Yup Lee
    • Hyun Uk Kim
    • Yu-Sin Jang
    Review Article
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Research

  • The use of electrochemistry in asymmetric catalysis can prove challenging, not least due to the difficulty of achieving chemo- and stereoselectivity in combination with very reactive electrochemically generated intermediates. Here, catalytic asymmetric electrosynthesis is reported for the synthesis of 1,4-dicarbonyl compounds with high enantiomeric excess, including compounds with all-carbon quaternary stereocentres. The chiral-at-metal catalyst activates the substrate towards anodic oxidation in addition to controlling the enantioselectivity of the process.

    • Xiaoqiang Huang
    • Qi Zhang
    • Eric Meggers
    Article
  • Predicting highly enantioselective ligands for a given asymmetric catalytic reaction is very challenging, but could greatly reduce the need for high-throughput, trial-and-error experimentation. Here, the authors report a freely available, automated tool to identify appropriate chiral ligands for given substrates in asymmetric catalysis.

    • Anthony R. Rosales
    • Jessica Wahlers
    • Per-Ola Norrby
    Article
  • Silicon–hydride materials are attractive candidates for the photoreduction of carbon dioxide into fuels, although they have only worked stoichiometrically so far. Now, Ozin and co-workers show how decorating silicon nanosheets with palladium nanoparticles renders the process catalytic.

    • Chenxi Qian
    • Wei Sun
    • Geoffrey A. Ozin
    Article
  • The electroreduction of carbon dioxide to formate represents a desirable strategy for the production of fuels and commodity chemicals. Now, guided by density functional theory, Cui and colleagues report CuSn3 alloys that exhibit high activity and selectivity for formate production from CO2 electroreduction at potentials as low as −0.5 V versus RHE.

    • Xueli Zheng
    • Yongfei Ji
    • Yi Cui
    Article
  • Reusable catalysts based on earth-abundant metals could offer inexpensive and sustainable routes in organic synthesis. Here a nickel catalyst—formed by pyrolysis of a nickel complex on a γ-Al2O3 support—is shown to be highly active for synthesis of primary amines via reductive amination. The catalyst operates with aqueous ammonia and either aldehydes or ketones, tolerating a wide range of functional groups.

    • G. Hahn
    • P. Kunnas
    • R. Kempe
    Article
  • Catalysts are dynamic species, whose structure can change over the course of a reaction. Here, structural changes are mapped for cobalt–palladium nanoparticles during CO oxidation, showing a reconstruction to CoOx on palladium surfaces. Furthermore, the composition-dependent reconstruction can be correlated with the trend in catalytic activity.

    • Cheng Hao Wu
    • Chang Liu
    • Miquel B. Salmeron
    Article
  • Copper-based catalysts, especially the so-called oxide-derived copper, are capable of producing multicarbon species from electrochemical CO2 reduction. However, little is known about their active sites despite intensive research efforts. Now, Lum and Ager show that oxide-derived copper catalysts have three distinct product-specific sites for the formation of C2+ chemicals, unlike polycrystalline copper or (111)- and (100)-oriented copper films which show no evidence of product specific sites.

    • Yanwei Lum
    • Joel W. Ager
    Article
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