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  • Electrochemical methods have great potential to help achieve net-zero emissions. Here, a method to synthesize ethylene carbonate is reported, which is electrochemically initiated and enables the concurrent production of hydrogen, capture of CO2 and subsequent conversion of the captured CO2 during ethylene carbonate synthesis.

    • Jun Ho Jang
    • Changsoo Kim
    • Ki Tae Nam
  • The synthesis, isolation and characterization of palladium complexes featuring one, two and three anionic aluminium ligands are reported, in which the aluminium ligands effectively stabilize the palladium in the zero-oxidation state. The aluminium–palladium bonds are highly polarized and the negatively charged palladium centre readily undergoes activation of B–B and C–N bonds.

    • Chenting Yan
    • Kota Koshino
    • Rei Kinjo
  • The isolation of secondary and primary carbon radical species is challenging, owing to their instability. Now the reduction of an acyclic bis(imino)carbene conjugate acid enables the isolation of a stable pentadienyl-type radical. In silico and in vitro probing of its properties reveal a propensity to act as a secondary carbon radical.

    • Ying Kai Loh
    • Levan Gojiashvili
    • Guy Bertrand
  • Biocatalytic methods for the synthesis of isoindolones, via C–H activation, have remained elusive. Now, an enantiodivergent artificial-metalloenzyme-catalysed method for the synthesis of chiral isoindolones is reported, using a streptavidin–biotin–Rh(III) catalyst system. Crystallographic analysis reveals the key residues that control stereoselectivity in streptavidin.

    • Prasun Mukherjee
    • Anjali Sairaman
    • Debabrata Maiti
  • The in situ generation of reactive (di)gallenes from a gallium–fluorobenzene complex and commercial chiral and achiral bisphosphine ligands is presented. The Ga(I) complex cations can undergo reversible cycloadditions to 1-alkenes and bond insertions into H–Si and H–B bonds.

    • Philipp Dabringhaus
    • Harald Scherer
    • Ingo Krossing
  • Renewable electricity-driven nitrogen oxidation is a green alternative to Haber–Bosch and Ostwald processes, but it is challenging to effectively steer oxygen intermediates towards the nitrogen oxidation reaction pathway. Now, to mitigate competing oxygen evolution and improve nitrogen oxidation efficiency, the use of hydroxyl radicals as the nitrogen oxidant is proposed.

    • Kai Dong
    • Yongchao Yao
    • Bo Tang
  • Atomically thin gold nanosheets are predicted to have interesting properties but their synthesis is challenging. Here the exfoliation of two-dimensional single-atom-thick gold, termed goldene, is achieved through wet-chemically etching Ti3C2 from Ti3AuC2. The synthesized goldene has promising properties as a heterocatalyst.

    • Shun Kashiwaya
    • Yuchen Shi
    • Lars Hultman
    ArticleOpen Access
  • The controlled degradation of larger and potentially harmful molecules into smaller, and preferably valuable, products is a crucial step to close the waste–degradation–synthesis loop envisioned by circular chemistry. Now, a forward-synthesis algorithm is designed to facilitate such degradation-oriented analyses, and proof-of-concept experimental validation is provided.

    • Anna Żądło-Dobrowolska
    • Karol Molga
    • Bartosz A. Grzybowski
  • Palladium-catalysed C(sp3)–H amination reactions of carboxylic acids are challenging due to N-coordination often outcompeting the carboxylic acid directing effect. Now, the development of chlorinated pyridine–pyridone ligands for palladium-catalysed methylene C(sp3)–H lactamization and cycloamination is reported, enabling the synthesis of lactams and cyclic amines.

    • Hau Sun Sam Chan
    • Yilin Lu
    • Jin-Quan Yu
  • Quaternary oxides can be synthesized from a variety of precursors, but there is a poor understanding of how to design efficient synthesis recipes. Here a strategy to navigate high-dimensional phase diagrams in search of the best precursors for quaternary oxide materials is reported and validated experimentally by a robotic laboratory.

    • Jiadong Chen
    • Samuel R. Cross
    • Wenhao Sun
    ArticleOpen Access
  • The making of mirror-image versions of naturally occurring cyclodextrins (CDs) is challenging and constitutes an untouched goal of the CD community. Now a concise approach is developed for the diastereoselective synthesis of three mirror-image CDs in an efficient and scalable manner.

    • Yong Wu
    • Saba Aslani
    • J. Fraser Stoddart
  • Methods for enzymatic C–F bond formation are rare. Now an enzymatic method for enantioselective C(sp3)–F bond formation is reported, through reprogramming non-haem iron enzyme (S)-2-hydroxypropylphosphonate epoxidase. Mechanistic studies reveal that the process proceeds through an iron-mediated radical fluorine transfer process.

    • Qun Zhao
    • Zhenhong Chen
    • Xiongyi Huang
  • Non-canonical amino acids are important building blocks in the synthesis of natural products, peptides and drugs. Now, a one-pot chemoenzymatic approach to synthesize branched azacyclic non-canonical amino acids is reported. This method combines enzymatic transamination of 2,n-diketoacids and stereocontrolled chemical reduction to provide the desired products with high stereoselectivity.

    • Tsung-Han Chao
    • Xiangyu Wu
    • Hans Renata
  • A series of molecular rare-earth telluride clusters incorporating a three-centre, four-electron, tri-tellurido ligand (Te34−) are reported. These atomically precise clusters, possessing ultralow band gaps comparable to those of monocrystalline silicon and gallium arsenide, are potentially applicable as quantum materials and for optoelectronic applications.

    • You-Song Ding
    • Xue-Lian Jiang
    • Zhiping Zheng
  • Spontaneous reactions proceed thermodynamically downhill, limiting transformations to those that are exergonic. Now a chemically fuelled endergonic synthesis is reported in which a Diels–Alder reaction is driven uphill by a ratchet mechanism.

    • Enzo Olivieri
    • James M. Gallagher
    • David A. Leigh
    ArticleOpen Access