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Hydrogen peroxide is an interesting target for artificial photosynthesis, although its actual production via the two-electron oxygen reduction reaction remains limited. Now, a carbon nitride-supported antimony single atom photocatalyst has been developed with a superior performance for this process.
In the face of global plastic pollution, enzymatic degradation of poly(ethylene terephthalate) (PET) has attracted much attention. Now, structural and biochemical studies reveal a minimal mutational strategy to increase the activity of PET-degrading enzymes, with potential evolutionary implications.
Conductive polymers are attractive materials for the construction of photoelectrodes in the context of artificial photosynthesis, although their performance is still limited. Now, an organic semiconductor photoanode for water oxidation is presented, which provides high photocurrent density for over 30 minutes.
The strong metal–support interaction is an important phenomenon for the modulation of a catalyst´s performance but is traditionally restricted to reducible oxide supports. Here, a CO2-induced strong metal–support interaction is reported for gold nanoparticles supported on non-reducible MgO to yield a superior oxidation catalyst.
Nanozymes can provide cost and stability advantages over natural enzymes, but they usually display low catalytic activity and inferior kinetics. Now, a highly active nanozyme is developed that shows comparable kinetics to horseradish peroxidase in the oxidation of a commonly used artificial substrate.
C−H bond functionalization methodologies usually rely on substrate-controlled directing-group chemistries to facilitate regioselective activation. Now, chemobiocatalytic cascades are reported that enable catalyst-controlled regioselective access to aryl nitriles, primary amides and carboxylic acids.
Improving the efficiency of carbon yield in heterotrophic microorganisms is desired for biomanufacturing. Now, a product-independent and energy-efficient CO2 sequestration system that maximizes carbon conversion has been developed, as showcased by the production of chemicals reaching their theoretical yields.
Ammonia lyases are powerful catalysts to access C–N bond formation via hydroamination, but show a narrow synthetic scope. Now, by computational redesign of an aspartase, a C–N lyase is developed that shows cross-compatibility of non-native nucleophiles and electrophiles expanding the synthetic scope.
Nitrous-oxide-mediated oxidation reactions can be effectively promoted by iron-containing zeolites, although structural information on the interaction between oxidant and metal centre is limited. Here, the authors report the characterization of the N2O-ligated Fe(ii) active site in iron-exchanged zeolite beta.
The cleavage of the C(sp2)–OH bond in phenols remains a challenging reaction, despite its relevance for the production of bio-based chemicals. Here, the authors introduce a Al(PO3)3-supported platinum catalyst capable of facilitating such a transformation under mild conditions thanks to the synergy between the metal and support.
The simultaneous achievement of both high ammonia yield and Faradaic efficiency in electrochemical nitrogen reduction is a challenging goal. Now, the diffusion of reactants to the catalyst surface is controlled using a covalent organic framework, which results in high-performance electrochemical ammonia synthesis.
Transformations in organic chemistry are mainly limited to the incorporation of only one equivalent of the greenhouse gas CO2 per substrate. Now, a visible-light photoredox-catalysed dicarboxylation of alkenes, allenes and arenes allows the incorporation of two CO2 molecules into organic compounds.
The standard Mizoroki–Heck reaction of aryl halides usually makes electron-poor alkenes react exclusively on the β-carbon. Now, α-selective intramolecular and intermolecular versions of this reaction with electron-deficient alkenes are reported, giving access to otherwise difficult-to-synthesize products.
Coupled thermal–electrochemical catalysis offers an attractive approach to upgrading CO2 into value-added products. Now, Ir–ceria-based catalysts in a protonic ceramic CO2 electrolyser are shown to selectively produce either CO or CH4 by tuning the Ir–O orbital hybridization.
A major drive in current chemistry research is to develop asymmetric versions of widely used carbon–carbon bond-forming reactions, such as Suzuki-Miyaura cross-couplings. Now, the origins of diastereo- and enantioselectivity in a Rh-catalysed cross-coupling of boronic acid and racemic allyl halides have been established.
The catalytic mechanism of oxygen activation employed by particulate methane monooxygenase for the oxidation of methane has remained elusive. Now, computational simulations suggest an important role of the phenol co-substrate and a catalytic cycle is proposed.
The catalytic hydrogenation of CO2 to methanol is a crucial reaction for the recycling of this greenhouse gas, although the selection and related performance of commercial catalysts is still limited. Now, the authors introduce sulfur vacancy-rich MoS2 nanosheets as a superior catalyst for this process, rivalling the commercial benchmark system.
Integration of biocatalysts into redox films has systematically led to a loss of their intrinsic reversibility. Now, a specially designed redox hydrogel preserves the reversibility of a [FeFe] hydrogenase and the importance of this feature for energy conversion applications is demonstrated.
Common strategies for catalyst design explore ways of fine-tuning continuous structure–property relationships. Here, the abrupt solid–liquid transition of Ga–In and Ga–Sn alloys is shown to have a profound impact on the CO2 electroreduction performance, with the molten alloy achieving a Faradaic efficiency of 95% formate production.
Enzymatic Diels–Alder reactions are of high synthetic interest, but mechanistic insights remain scarce. Now, a structure of the Diels–Alderase CghA in complex with its product is reported, a catalytic mechanism proposed and the enzyme is engineered to form the energetically disfavoured exo adduct.