Volume 3 Issue 11, November 2020

Volume 3 Issue 11

Discrete catalytic functions

Analogous with a modern production line, the cover image illustrates how precise placement of different active sites (robotic arms) within a hierarchical pore network enables individual catalyst particles to perform a complex sequence of chemical transformations in a cooperative and predictable process reminiscent of substrate channelling (conveyor belt) in biological systems. Here, the authors illustrate this approach for cascade and antagonistic reactions, namely a two-step deacetalization–Knoevenagel condensation of dimethyl acetals to cyanoates and a base-catalysed triacylglyceride transesterification.

See Isaacs et al.

Image: Ella Maru Studio. Cover Design: Valentina Monaco.

Research Highlights

News & Views

  • News & Views |

    The development of feasible routes for the valorization of waste plastics is an urgent challenge to be solved. Now, a strategy is introduced for the selective production of hydrogen-rich gas and multi-walled carbon nanotubes in a single-step process using an FeAlOx catalyst and microwave irradiation.

    • Gartzen Lopez
    •  & Laura Santamaria
  • News & Views |

    Enhancing the oxygen exchange rate at the surface of oxides through rational design has long been a key goal of researchers pursuing sustainable energy solutions. Now, a simple infiltration method reveals that reaction rates on porous mixed-conducting oxides scale with the acidity of the infiltrate and can be tuned by orders of magnitude.

    • Sossina M. Haile
  • News & Views |

    DNA-based dynamic networks show adaptation to external stimuli toward the generation of the fittest constituent. This selection principle has now been implemented to control the catalytic efficiency of an enzymatic reaction.

    • Lena J. Winat
    •  & Barbara Saccà

Comment & Opinion

  • Comment |

    Considerable research achievements were made to address the plastic crisis using biotechnology, but this is still limited to polyesters. This Comment aims to clarify important aspects related to myths and realities about plastic biodegradation and suggests distinct strategies for a bio-based circular plastic economy in the future.

    • Ren Wei
    • , Till Tiso
    • , Jürgen Bertling
    • , Kevin O’Connor
    • , Lars M. Blank
    •  & Uwe T. Bornscheuer

Reviews

  • Review Article |

    Organochlorides are attractive building blocks for photocatalytic synthesis that have been receiving increasing attention lately, thanks to recent methodological advances that overcome their inertness. In this Review Article, Giedyk and colleagues summarise the developments and strategies for their photocatalytic activation.

    • Martyna Cybularczyk-Cecotka
    • , Joanna Szczepanik
    •  & Maciej Giedyk

Research

  • Article |

    Synthetic methods for the green and atom-economical synthesis of thioesters are scarce. Now, a catalytic protocol utilizing a ruthenium pincer complex provides efficient access to thioesters with hydrogen gas as the sole by-product via dehydrogenative coupling of alcohols with thiols.

    • Jie Luo
    • , Michael Rauch
    • , Liat Avram
    • , Yael Diskin-Posner
    • , Guy Shmul
    • , Yehoshoa Ben-David
    •  & David Milstein
  • Article |

    Achieving plastic deconstruction with high selectivity is crucial for upcycling schemes, but remains challenging. Here, a processive approach for the selective hydrogenolysis of high-density polyethylene into narrow alkane fractions is introduced relying on a Pt/SiO2 catalyst encapsulated in a mesoporous silica shell.

    • Akalanka Tennakoon
    • , Xun Wu
    • , Alexander L. Paterson
    • , Smita Patnaik
    • , Yuchen Pei
    • , Anne M. LaPointe
    • , Salai C. Ammal
    • , Ryan A. Hackler
    • , Andreas Heyden
    • , Igor I. Slowing
    • , Geoffrey W. Coates
    • , Massimiliano Delferro
    • , Baron Peters
    • , Wenyu Huang
    • , Aaron D. Sadow
    •  & Frédéric A. Perras
  • Article |

    The valorisation of plastic waste is highly desirable from an environmental perspective but generally yields low-value products. Now a method is disclosed to deconstruct plastic feedstocks into high-value hydrogen and carbon materials by means of an iron-based catalyst under microwave irradiation.

    • Xiangyu Jie
    • , Weisong Li
    • , Daniel Slocombe
    • , Yige Gao
    • , Ira Banerjee
    • , Sergio Gonzalez-Cortes
    • , Benzhen Yao
    • , Hamid AlMegren
    • , Saeed Alshihri
    • , Jonathan Dilworth
    • , John Thomas
    • , Tiancun Xiao
    •  & Peter Edwards
  • Article |

    Improving the kinetics of O2 reduction on oxide surfaces is critical in many energy and fuel conversion technologies. Now, the authors demonstrate that the acidity of infiltrated surface oxides can serve as a descriptor of the oxygen surface exchange rate on mixed conducting oxides.

    • Clement Nicollet
    • , Cigdem Toparli
    • , George F. Harrington
    • , Thomas Defferriere
    • , Bilge Yildiz
    •  & Harry L. Tuller
  • Article |

    The spatial segregation of distinct catalytic functionalities within the same material holds great promise for cascade or antagonistic reactions, but it remains challenging. Here, the authors report the successful realization of this approach for an efficient hierarchical porous silica catalyst featuring spatially separated sulfated zirconia and magnesium oxide.

    • Mark A. Isaacs
    • , Christopher M. A. Parlett
    • , Neil Robinson
    • , Lee J. Durndell
    • , Jinesh C. Manayil
    • , Simon K. Beaumont
    • , Shan Jiang
    • , Nicole S. Hondow
    • , Alexander C. Lamb
    • , Deshetti Jampaiah
    • , Michael L. Johns
    • , Karen Wilson
    •  & Adam F. Lee
  • Article |

    Despite the efforts to tune their properties, the efficiency of tantalum nitride photoanodes falls short of the theoretical value. Here, a gradient Mg doping strategy is introduced to engineer tantalum nitride’s band structure and control its defects, leading to an applied bias photon-to-current efficiency of 3.25%.

    • Yequan Xiao
    • , Chao Feng
    • , Jie Fu
    • , Faze Wang
    • , Changli Li
    • , Viktoria F. Kunzelmann
    • , Chang-Ming Jiang
    • , Mamiko Nakabayashi
    • , Naoya Shibata
    • , Ian D. Sharp
    • , Kazunari Domen
    •  & Yanbo Li
  • Article |

    Extensive research efforts in systems chemistry are directed to the development of in vitro systems that mimic complex natural networks. Now, stimuli-responsive nucleic acid-based networks conjugated to biocatalysts for the triggered and orthogonal control over biocatalytic cascades are reported.

    • Chen Wang
    • , Liang Yue
    •  & Itamar Willner
  • Article |

    Difunctionalization of alkenes can afford useful building blocks from readily available starting materials, but these reactions often show limitations in olefin scope. This work presents a catalyst-controlled enantioselective 1,1-arylboration of unactivated alkenes that is independent of directing groups.

    • Wang Wang
    • , Chao Ding
    •  & Guoyin Yin

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