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Heterogeneous catalysts are often dynamic under operation. Now, the mechanism of CH4 dry reforming on Ni is studied by in situ microscopy and spectroscopy, revealing the formation of metastable surface nickel–oxygen structures from CO2 dissociation that exhibit different catalytic properties and induce rate oscillations.
The electrochemical deoxygenation of carbonyl groups by hydrogenolysis is challenging as the competing hydrogenation usually prevails. Now the electrochemical Clemmensen reduction is proposed, achieving the selective hydrogenolysis of various carbonyl compounds using Zn as the electrocatalyst in a mildly acidic solution.
Photocatalytic overall water splitting on particulate systems represents a possibility for clean energy storage, yet efficiencies for the process are typically low. Here, highly concentrated saltwater is used to polarize photoexcited N-doped TiO2, resulting in enhanced charge separation and a solar-to-hydrogen efficiency approaching 20%.
Coenzyme Q has several important biological functions, but the understanding of the biosynthesis of coenzyme Q in humans remains incomplete. Now, by constructing the entire COQ metabolon in vitro, the enzymes and reactions underlying coenzyme Q biosynthesis are characterized.
The reconstruction of Cu electrocatalysts during CO2 reduction is an impediment to the stability of this technology, yet a clear picture of the species involved in this process remains elusive. Here, the authors demonstrate the presence of transient solution-based Cu(I) species and theoretically predict complexes with CO and oxalate as the likely candidates.
C–C bond formation involving sp3 centres has typically relied on stoichiometric reagents. Here catalytic Ag electrodes modified with Mg(OAc)2 enable electrocatalytic coupling of an organic halide with an aldehyde for the selective formation of a broad scope of alcohol products.
Using N2 as a N source to nitrogenate compounds is highly desirable but also very challenging. Now a cascade electrosynthesis strategy is proposed to prepare (CF3SO2)2NLi and its analogues from N2 via a looped Li–N2 battery.
Few synthetic CO2-fixation pathways have been tested in vivo. Now, the new-to-nature THETA cycle is designed, realized in vitro and modular implemented in vivo. This cycle involves 17 enzymes, including the two most active carboxylases known so far, to produce the central building block acetyl-CoA using CO2.
Merging photoredox and biocatalysis provides opportunities to address challenges in synthetic chemistry. Now the combination of a ruthenium photocatalyst for oxidative radical formation and ‘ene’-reductases for radical interception enables an enantiodivergent decarboxylative alkylation reaction.
Chiral lactams are important pharmacophores and strategies for their synthesis through direct C–H functionalization are highly sought after. Now, intramolecular C–H amidation of dioxazolones via biocatalytic nitrene transfer enables the synthesis of enantioenriched lactams with various ring sizes.
Low-carbon chemicals generated from CO2 provide a possible path to improve the sustainability of microbial bioproduction of food and chemicals. Now, using a metabolic engineering approach, yeast is engineered to produce glucose, myo-inositol, glucosamine, sucrose and starch from C1–3 molecules.
Fe–N–C catalysts are a promising alternative to precious metals in fuel cell cathodes, but they suffer from durability issues. Now, a preparation method is reported that allows increasing the active site density while also improving durability.
Plasmonic composites have potential for photocatalytic conversions using solar light; however, complex interactions between light and the components are poorly understood. Here, a highly ordered two-dimensional plasmonic bimetallic AuPt supercrystal demonstrates a high rate of H2 generation from formic acid while providing insight into the interaction between plasmonic antenna and catalyst.
Anion-exchange membrane fuel cells are promising devices to produce electricity from green hydrogen, but the development of suitable cathode catalysts is required for their successful deployment. Now, Co(CN)3 microcrystals with cyanide linkages and well-defined coordination structures are shown to exhibit high oxygen reduction reaction performance in alkaline conditions.
Terpenoids are natural products with high value in the chemical industry; however, their expression in different hosts is limited by the availability of cytochrome P450. Here the authors show the engineering of recombinant Escherichia coli that can easily produce terpenoids from different classes and species.
Asymmetric catalytic photoelectrochemical reactions for the construction of complex compounds are underdeveloped. Now, merging photoelectrochemistry with asymmetric catalysis has enabled the dehydrogenative [2 + 2] photocycloaddition between alkyl ketones and alkenes affording enantioenriched cyclobutanes.
Different locations have been proposed for the catalytic centre of particulate methane monooxygenase for methane oxidation to methanol. Now, cryoelectron microscopy structures and electron nuclear double resonance spectroscopic measurements of the enzyme with a product analogue identify CuD as the active site and provide insights into substrate binding.
Enantioconvergent cross-electrophile coupling of non-redox-active alcohol derivatives is challenging. Now, taking advantage of Ni–C bond homolysis, enantioconvergent coupling of non-redox-active propargylic esters with chlorogermanes enables the synthesis of chiral propargyl germylation products.
The development of innovative strategies for the capture and biodegradation of nanoplastics is sought after. Now, artificial hydrolytic active sites are incorporated into non-catalytic membrane nanopores generating pore-based biocatalytic nanoreactors that depolymerize polyethylene terephthalate plastic nanoparticles.
The sluggish conversion of lithium polysulfides in Li–S batteries can be overcome by the use of catalysts, but their design is typically done via trial and error. Now, a binary descriptor is proposed by machine learning to capture electronic and structural effects for the design of Li–S battery cathode catalysts.