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A local electronic manipulation strategy is developed for stabilizing high-valence Ru single sites. The materials are efficient bifunctional catalysts for water electrolysis.
Tailoring of the short-range microenvironment surrounding the active site in ruthenium-based catalyst systems can lead to enhanced overall water splitting.
By systematically exploring a large chemical space using automated experimentation, a high-performing organic photocatalyst for hydrogen evolution is discovered.
Photoinduced C(sp3)–H functionalization reactions, through hydrogen atom transfer (HAT) processes, have become a useful tool in synthesis, but challenges remain. This Perspective showcases the potential of pyridine N-oxides as HAT reagents in photoinduced C(sp3)–H functionalization reactions, highlighting how they can be readily tuned to achieve site-selectivity.
Water electrolysis can produce clean hydrogen, but it is limited by the slow anodic oxygen evolution reaction. Now, a local electronic manipulation strategy for stabilizing high-valence Ru single site catalysts has been developed. The catalyst demonstrates efficient bifunctional activity for water electrolysis.
Control of atoms with single-atom precision is a key challenge in nanoscience. Now an electron beam approach to engineer shielded metal atoms in transition metal dichalcogenides is proposed. This method can create diverse atomic vacancies, leading to interesting magnetic and electronic properties.
An efficient molecular nanojunction photocatalyst for hydrogen evolution is identified from a combinatorial molecular library, assisted by a materials acceleration platform, which is then scaled-up to the litre scale using flow synthesis.
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.
Three closely related proline-based ligands give rise to different catalytic systems in asymmetric dialkylzinc addition reactions. Mechanistic studies reveal that monomeric, dimeric and product–catalyst complexes and aggregates larger than dimers are all catalytically active.
Radical-mediated synthesis of N-glycosides is underdeveloped. Here a glycosyl radical-mediated N-glycosylation reaction using combined copper and photoredox catalysis is reported. This protocol exhibits high chemoselectivity and water tolerance, overcoming challenges associated with cationic glycosylation reactions.
Multicomponent catalytic reactions that generate enantioenriched boronic esters are underdeveloped. Now an N-heterocyclic carbene–nickel catalyst promotes enantioselective alkene 1,2-carboboration to access multifunctional alkylboronates, bearing a tertiary or quaternary β-stereocentre.
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.
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.
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.