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Volume 2 Issue 3, March 2019

Volume 2 Issue 3

Synthetic lubricants from ethylene

While group 4 catalysts produce high-molecular-mass polyethylenes with spectacular efficiency, these catalysts are ineffective in producing low-molecular-mass highly-branched polyethylenes. Here Lohr, Marks and co-workers report the synthesis of these materials from abundant ethylene. The excellent activity and branch selectivity reflect previously unrecognized aspects of the cationic catalyst–counteranion pairing in nonpolar media. The products are rheologically and tribologically attractive candidates for synthetic lubricants.

See Gao et al.

Image: Yanshan Gao (Northwestern University); LetPub. Cover Design: Alex Wing.

Research Highlights

News & Views

  • News & Views |

    The asymmetric synthesis of chiral γ-lactams is difficult and laborious; typically requiring pre-functionalization of starting materials. Now, a highly efficient alternative approach employing direct C−H amidation via chiral hydrogen-bond-donor catalysts has been developed.

    • Tong-De Tan
    • Long-Wu Ye
  • News & Views |

    The synthesis of highly branched low molecular weight products — potential synthetic lubricants — directly from ethylene is challenging when highly efficient early transition metal catalysts are employed. Now, an alkane soluble co-catalyst permits the synthesis of such polyethylenes using a zirconium catalyst in a saturated hydrocarbon solvent, where competitive solvent coordination at the active site of the catalyst is relatively unimportant.

    • Rhett Kempe
  • News & Views |

    The selective electrochemical conversion of ketones to value-added products still represents a challenge, due to a lack of fundamental understanding. Now, a principle has been revealed that allows the steering of the electroreduction of aliphatic ketones on platinum by carefully controlling the coordination number of the platinum atoms.

    • Ivana Matanović

Reviews

  • Perspective |

    The hydrogenation of CO2 to form methane has been known for over a century. However, given increased interest in small-molecule activation for energy storage, and improved catalysts and understanding of the process, it is worthwhile to look again at the reaction. This Perspective discusses recent work on the fundamentals of the Sabatier reaction and also the potential for large-scale applications.

    • Charlotte Vogt
    • Matteo Monai
    • Bert M. Weckhuysen

Research

  • Article |

    Samarium iodide is a remarkably useful and mild reductant in organic synthesis, but its use can be problematic due to the need for (super)stoichiometric loadings. Now a method that employs samarium iodide as a catalyst—without the need for a stoichiometric co-reductant—is reported. Loadings as low as 5% are shown to catalyse radical cyclization cascades.

    • Huan-Ming Huang
    • Joseph J. W. McDouall
    • David J. Procter
  • Article |

    Chiral γ-lactams are of significant interest being present in numerous pharmaceutical agents; however, their chemical synthesis is complex, requiring pre-functionalized starting materials. Now, Park and Chang report an iridium-based catalyst system for the production of chiral γ-lactams from an abundant feedstock via an intramolecular asymmetric sp3 C−H amidation.

    • Yoonsu Park
    • Sukbok Chang
  • Article |

    Cell viability depends on transcriptional fidelity, but the proofreading mechanism of eukaryotic RNA polymerase II (Pol II) remained elusive. Now, Cheung, Wang, Zhang, Huang and co-workers show that Pol II utilizes the downstream phosphate oxygen of the RNA transcript to activate intrinsic cleavage of misincorporated nucleotides.

    • Carmen Ka Man Tse
    • Jun Xu
    • Xuhui Huang
  • Article |

    Low-molecular-weight, highly branched polyethylenes are attractive candidates for synthetic lubricants, but their efficient production is constrained by a lack of effective catalytic methods. While conventional group IV transition metal catalysts produce diverse polyethylenes on a huge scale, they are unable to produce highly branched polyethylenes. Here a hydrocarbon-soluble organozirconium precatalyst and borate cocatalyst produce the desired polyethylenes with excellent activity and branch selectivity.

    • Yanshan Gao
    • Jiazhen Chen
    • Tobin J. Marks
  • Article |

    The electrocatalytic reduction of carbonyl groups is gaining attention in the context of biorefinery. However, fundamental knowledge on such processes is still limited. Now, the selectivity for the electroreduction of acetone on platinum single crystals is studied, revealing a remarkable structural sensitivity.

    • Christoph J. Bondue
    • Federico Calle-Vallejo
    • Marc T. M. Koper
  • Article |

    The upgrade of carbon monoxide to higher alcohols offers a route to renewable fuels. Now, Sinton, Sargent and co-workers report a highly fragmented, copper-based catalyst with engineered interfaces between the (111) and (100) facets that promote the coupling of C1 and C2 species, leading to enhanced production of n-propanol.

    • Yuanjie Pang
    • Jun Li
    • David Sinton
  • Article |

    Iron single-atom catalysts are among the most promising fuel cell cathode materials in acid electrolyte solution. Now, Shui, Xu and co-workers report concave-shaped Fe–N–C nanoparticles with increased availability of active sites and improved mass transport, meeting the US Department of Energy 2018 target for platinum-group metal-free fuel cell catalysts.

    • Xin Wan
    • Xiaofang Liu
    • Jianglan Shui
  • Article |

    Metal oxides have been identified as a promising class of catalysts for carbon–oxygen bond cleavage in the context of biomass valorization, although the systematic understanding of their reactivity remains elusive. Now, a combination of catalytic screening and first principles calculations provide important insights into this family of catalysts.

    • Konstantinos A. Goulas
    • Alexander V. Mironenko
    • Dionisios G. Vlachos

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