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Metal utilization is important for the overall efficiency of heterogeneous catalysts, but reducing the amount of precious active phases is challenging due to intrinsic properties such as structure sensitivity. Now Hensen and colleagues engineer the interfaces of supported cobalt catalysts to overcome such structure sensitivity limitations in CO2 hydrogenation.
Carbon dioxide reforming can be used to valorize hydrocarbon-containing CO2 streams without the use of external reductants, but existing methods remain inefficient. Here, an HZSM-5-encapsulated nickel catalyst is introduced that features a remarkable methane dry reforming activity combined with high methane utilization.
Material–microbe hybrids represent a promising strategy for harnessing biochemical reactivity using sunlight, yet little is known about the effect of the interaction on the organism. Here the interface of a CO2- and N2-fixing bacterium to CdTe alters its biochemical pathways, resulting in quantum efficiency close to the theoretical limit.
Artificial enzymes have shown promise for a variety of applications, although their performance is hampered by the limited tunability of current designs. This work introduces a class of artificial enzymes based on metal–organic framework monolayers that feature an amino acid-coordinated metal centre and photoactive cofactors and can be assembled into an efficient artificial photosynthesis system.
Hydroxide exchange membrane fuel cells operating in alkaline electrolyte are more cost-effective than their proton exchange membrane counterparts, but their performance is still considerably lower. Now, a Ni–Mo–Nb metallic glass is put forward as a hydrogen oxidation reaction catalyst with high activity and stability in alkaline electrolyte.
Chiral piperidines are of importance in drug synthesis, but effective and broadly applicable methods for their production remain scarce. Now, a reductive Rh-catalysed method is developed for the introduction of chiral primary amines into reduced pyridinium salts, affording optically active piperidines.
The multihole mechanism of the oxygen evolution reaction on semiconductor electrodes has been hard to elucidate due to a lack of atomic-scale structural characterization of the material interface. Using pulse voltammetry and simulations of α-Fe2O3 photoanodes, this study predicts the chemical origin of the third-order rate dependence on holes.
Platinum is the most active catalyst for the hydrogen evolution reaction, but the specific mechanism and the influence of the alkali metal cations remain elusive in alkaline media. Now, electrical transport spectroscopy, electrochemical impedance spectroscopy and ab initio molecular dynamics simulations are combined to elucidate the role of alkali metal cations for this reaction in alkaline electrolyte.
Immunogenicity concerns preclude the use of bacterial kynureninases for cancer immunotherapy, while the human variant lacks the desired therapeutic effect. A human kynureninase enzyme has now been evolved to reach the activity and substrate specificity of its bacterial counterpart.
Installation of enantioenriched tri- and tetrasubstituted stereogenic centres is important in the synthesis of bioactive compounds. Now, a sterically encumbered chiral N-heterocyclic carbene-Ni(0) catalyst is introduced for the enantioselective carbofunctionalization of substituted alkenes via multicomponent reactions.
Asymmetric synthetic photoelectrochemical transformations are underdeveloped. Now, the combination of a photocatalyst, a chiral copper catalyst and an electrode allows the enantioselective cyanation of benzylic C–H bonds without a chemical oxidant.
A detailed understanding of the catalytic target DNA cleavage mechanism by CRISPR–Cas9 has been lacking. Now the key modulating role of Mg2+ in the conformational activation of Cas9 and the influence of active site residues on the protonation state of catalytic H840 are demonstrated, ultimately unravelling the catalytic mechanism.
Substrate preorganization is a ubiquitous concept in the active sites of natural enzymes and is linked to their intrinsic activity. In this study, a designed cleft in a synthetic supramolecular catalyst is shown to preorganize water, resulting in high water oxidation activity and distinct mechanistic changes.
The hydrogen evolution and oxidation reactions on Pt electrocatalysts exhibit much more favourable kinetics in acidic than in alkaline electrolytes. Now, by combining theoretical simulations and spectroscopic measurements, it is demonstrated that the different connectivity of hydrogen-bond networks in the electric double layer is responsible for such an effect.
An asymmetric C–C coupling (Wood–Ljungdahl) pathway has long been known in biological carbon fixation, whereas its occurrence in inorganic systems has remained unclear. In this study, the coupling of *CO and *CHx intermediates to form multicarbon oxygenates has been experimentally observed on Cu electrodes.
The activation of CO2 for catalytic carboxylation of alkenes is mainly limited to two-electron processes. Now, a visible-light photocatalytic single-electron transfer reduction of CO2 is reported leading to the key intermediate CO2•−, which allows carboxylation of unactivated aliphatic alkenes.
Controlling the enantioselectivity in metallaphotoredox-catalysed radical cross-couplings using cobalt has proven challenging. Now, the identification of a chiral polydentate ligand enables cobalt-catalysed enantioselective couplings with a broad scope of radicals affording chiral heterobiaryl products.
Copper-based catalysts are traditionally very effective for the hydrogenation of CO2 to methanol, although control over the active site has remained elusive. Here, the authors design a Cu1/ZrO2 single-atom catalyst featuring a Cu1–O3 site responsible for a remarkable performance at 180 °C.
Ni–Fe carbon monoxide dehydrogenases (CODHs) are able to oxidize CO with a high rate, but their O2 sensitivity is a major drawback for their industrial application. This work shows that CODHs can be tailored for industrial or gas cleaning processes by engineering the selectivity of their gas channels.
Selective electrocatalytic conversion of nitrogen species requires control over proton and electron transfer. Here, independent optimization of the driving force for proton transfer is realized through the use of MoS2 phases with different pKas, allowing high selectivity for NO, N2O, N2 and NH4+ to be achieved by varying the applied potential.