Nickel–iron and cobalt–iron (oxy)hydroxides are state-of-the-art electrocatalysts for oxygen production in alkaline conditions. Now, the addition of high-valent dopants has been demonstrated to further propel the catalytic rate in these materials by an order of magnitude.

The Fischer–Tropsch product, water, is regularly hypothesized to be the driving force for catalyst deactivation. Cobalt nanoparticles may be oxidized to CoO, form mixed-metal oxides with supports, or sinter to larger particles. This Comment discusses the feasibility of these deactivation pathways, highlighting the importance of in situ characterization.

DNA-based dynamic networks show adaptation to external stimuli toward the generation of the fittest constituent. This selection principle has now been implemented to control the catalytic efficiency of an enzymatic reaction.

Enhancing the oxygen exchange rate at the surface of oxides through rational design has long been a key goal of researchers pursuing sustainable energy solutions. Now, a simple infiltration method reveals that reaction rates on porous mixed-conducting oxides scale with the acidity of the infiltrate and can be tuned by orders of magnitude.

The development of feasible routes for the valorization of waste plastics is an urgent challenge to be solved. Now, a strategy is introduced for the selective production of hydrogen-rich gas and multi-walled carbon nanotubes in a single-step process using an FeAlOx catalyst and microwave irradiation.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

We provide herein an overview of the present issue while introducing two new features that complement our submission and publication process.

Considerable research achievements were made to address the plastic crisis using biotechnology, but this is still limited to polyesters. This Comment aims to clarify important aspects related to myths and realities about plastic biodegradation and suggests distinct strategies for a bio-based circular plastic economy in the future.

Ta3N5 is a promising photoanode material with a theoretical maximum solar conversion efficiency of 15.9% for photoelectrochemical water splitting. However, the highest applied bias photon-to-current efficiency achieved so far is only 2.72%. To bridge the efficiency gap, effective carrier management strategies for Ta3N5 photoanodes should be developed. Here, we propose to use gradient Mg doping for

The ubiquitous challenge of plastic waste has led to the modern descriptor plastisphere to represent the human-made plastic environment and ecosystem. Here we report a straightforward rapid method for the catalytic deconstruction of various plastic feedstocks into hydrogen and high-value carbons. We use microwaves together with abundant and inexpensive iron-based catalysts as microwave susceptors to

The overconsumption of single-use plastics is creating a global waste catastrophe, with widespread environmental, economic and health-related consequences. Here we show that the benefits of processive enzyme-catalysed conversions of biomacromolecules can be leveraged to affect the selective hydrogenolysis of high-density polyethylene into a narrow distribution of diesel and lubricant-range alkanes

The development of robust and reactive chiral catalysts is a fundamental aim in asymmetric catalysis, and crucial for providing efficient methods for synthesizing chiral molecules. Chiral paddle-wheel bimetallic complexes provide a highly tunable chiral environment in rhodium-catalysed asymmetric carbene/nitrene transfer reactions and Lewis acid-catalysed reactions. Chiral paddle-wheel complexes having

Improving the kinetics of O2 reduction on oxide surfaces is critical in many energy and fuel conversion technologies. Here we show that the acidity scale for binary oxides is a powerful descriptor for tuning and predicting oxygen surface exchange kinetics on mixed conducting oxides. By infiltrating a selection of binary oxides from strongly basic (Li2O) to strongly acidic (SiO2) onto the surface of

Thioesters play important roles in chemistry and biology, but their synthesis generally exhibits a poor atom economy and generates copious waste. We report here the dehydrogenative coupling of alcohols and thiols to yield thioesters and evolve H2. This waste-free reaction is catalysed by an acridine-based ruthenium pincer complex in hexamethyldisiloxane as the optimal solvent without any additives

Substantial progress has recently been made in the general understanding of the interfacial CO2 reduction reaction (CO2RR) in electro- and photocatalysis, but the influence of the local chemical environment and its effects on the catalytic interface at the molecular level remains largely elusive. Here, we introduce a classification scheme to group different aspects influencing the interfacial CO2RR

Platinum single sites are highly attractive due to their high atom economy and can be generated on CeO2 by an oxidative high-temperature treatment. However, their location and activity are strongly debated. Furthermore, reaction-driven structural dynamics have not been addressed so far. In this study, we were able to evidence platinum-induced CeO2 surface restructuring, locate platinum single sites

Catalytic carbonyl–olefin metathesis reactions represent powerful synthetic strategies for alkene formation. Successful approaches for carbonyl–olefin ring-closing, ring-opening and cross metathesis have been developed in recent years, but current limitations hamper the generality of these transformations. Stronger, more efficient catalytic systems are needed to further broaden the scope of these transformations

Understanding the mechanism of catalytic hydrogenation at the local environment requires chemical and topographic information involving catalytic sites, active hydrogen species, and their spatial distribution. Here we used tip-enhanced Raman spectroscopy (TERS) to study the catalytic hydrogenation of chloronitrobenzenethiol on a well-defined Pd(submonolayer)/Au(111) bimetallic catalyst (\(p_{\rm{H}_{2}}\) = 1

The activity and the stability of an electrocatalyst are equally important, but the reasons behind deactivation processes still remain unresolved. Achieving a deeper understanding of the process will help to inhibit deactivation and improve revivification protocols.

Peroxygenases are attractive biocatalysts for the selective introduction of oxygen into organic molecules under mild conditions with hydrogen peroxide as the oxygen source. In addition to the identification of primary peroxygenases, different classes of enzymes were shown to display promiscuous peroxygenase activity. Even though enzymes with peroxygenase activity are promising industrial biocatalysts

Industrially, aldehydes are produced annually on a multimillion-tonne scale via the hydroformylation of olefins with syngas (CO/H2 mixture). Nonetheless, this transformation has not found frequent use in the laboratory. Here we report on a simple strategy for the concerted generation of syngas from two accessible and crystalline main element compounds with just water as the primary activator for syngas

The development of low-temperature fuel cells for clean energy production is an appealing alternative to fossil-fuel technologies. CO is a key intermediate in the electro-oxidation of energy carrying fuels and, due to its strong interaction with state-of-the-art Pt electrodes, it is known to act as a poison. Here we demonstrate the ability of Earth-abundant Cu to electro-oxidize CO efficiently in alkaline

Cas9 nucleases recognize and cleave their target DNA through base pairing of a guide RNA with a spacer adjacent to a protospacer adjacent motif (PAM). Streptococcus thermophilus Cas9 (St1Cas9), a smaller Cas9 orthologue than Streptococcus pyogenes Cas9, enables robust genome editing in diverse organisms. Here we report high-resolution structures of St1Cas9 in complex with a single-guide RNA and different

Electrochemical CO2 reduction to value-added chemical feedstocks is of considerable interest for renewable energy storage and renewable source generation while mitigating CO2 emissions from human activity. Copper represents an effective catalyst in reducing CO2 to hydrocarbons or oxygenates, but it is often plagued by a low product selectivity and limited long-term stability. Here we report that copper

The fundamental kinetics of the electrocatalytic sulfur reduction reaction (SRR), a complex 16-electron conversion process in lithium–sulfur batteries, is so far insufficiently explored. Here, by directly profiling the activation energies in the multistep SRR, we reveal that the initial reduction of sulfur to the soluble polysulfides is relatively easy owing to the low activation energy, whereas the

Achieving stable, low-cost electrocatalysts represents a daunting challenge towards practical water oxidation reactions. Here, we report that a degraded electrocatalyst can be revivified under catalytic operating conditions by manipulating reversible phase segregation. Under the oxygen evolution reaction conditions, Fe segregation develops in the Ni–Fe hydroxide host lattice, with the formation of

Platinum dissolution and restructuring due to surface oxidation are primary degradation mechanisms that limit the lifetime of platinum-based electrocatalysts for electrochemical energy conversion. Here, we have studied well-defined Pt(100) and Pt(111) electrode surfaces by in situ high-energy surface X-ray diffraction, online inductively coupled plasma mass spectrometry and density functional theory

Nucleophilic aromatic substitution (SNAr) is routinely used to install 19F– and 18F– in aromatic molecules, but is typically limited to electron-deficient arenes due to kinetic barriers associated with C–F bond formation. Here we demonstrate that a polarity-reversed photoredox-catalysed arene deoxyfluorination that operates via cation-radical-accelerated SNAr enables the fluorination of electron-rich

Suppressing the degradation of polymer electrolyte membrane fuel cells due to anode side-reactions during repetitive cell start-up/shut-down remains a formidable challenge. Now, a phase transition material of WO3 has been explored as a smart catalytic switch to enable highly selective electrocatalysis and improve fuel cell longevity.

Two different types of H2O2 selectivity are reported for the electrochemical synthesis of H2O2: molar fraction selectivity and Faradaic selectivity. Here we revisit their definitions and discuss the best way to report H2O2 selectivity, which can help to avoid misunderstandings or unfair performance comparisons in this growing field.

Axially chiral biaryls are common structural motifs in functional materials, bioactive natural products, pharmaceuticals and chiral catalysts/ligands. As such, efficient preparation of these privileged scaffolds is an important endeavour in organic chemistry. Herein we report a general and modular platform technology for the construction of axial chirality via palladium/chiral norbornene cooperative

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Site-selective deuteration of C–H bonds increases the lifetime and efficacy of drug molecules. Although effective methods to form C(sp2)–D bonds are known, processes for making C(sp3)–D bonds often have low site selectivity, require expensive and unrecoverable D2 gas, or use stoichiometric reagents. Here we report cost-efficient and site-selective reductive deuteration using a tandem electrochemical

The discoveries of new forms of carbon have always opened doors to new science and technology. In 1991, three-dimensional (3D) periodic carbon crystals with negative Gaussian curvatures that consist of six- and eight-membered rings were proposed. To realize these 3D periodic carbon crystals (known as Mackay crystals), methods for creating polyaromatic structures embedding eight-membered rings must

The growing hydrogen economy requires accelerating the hydrogen evolution reaction. The water dissociation step (Volmer step) has been proposed as a main kinetic limitation, but the mechanisms at play in the electrochemical double-layer are poorly understood. This is due to the dual role of water: it acts both as a reactant and as a solvent. Here we propose to confine water inside an organic liquid

Polyketide synthases are multi-domain enzymes that catalyse the construction of many bioactive natural products. Now, some of the inefficiencies and limitations of these systems have been solved by designing an artificial pathway for carbon–carbon bond formation via iterative rounds of non-decarboxylative thio-Claisen reactions.

The organic chemist’s toolbox is vast, with technologies to accelerate the synthesis of novel chemical matter. The field of asymmetric catalysis is one approach to accessing new areas of chemical space and computational power is today sufficient to assist in this exploration. Unfortunately, existing techniques generally require computational expertise and are therefore underutilized in synthetic chemistry

The incorporation of alkynes into organic molecules is one of the most valuable transformations for the formation of C–C bonds and provides a versatile handle for further modifications. The Sonogashira cross-coupling of acetylenes holds a prominent position among the suite of catalytic cross-coupling reactions that are key to modern synthesis. Here we present a method that is complementary to the Sonogashira

Catalytic hydrogenation is one of the backbones of the chemical industry. Controlling the reaction behaviour of the activated hydrogen species over oxide-supported metal catalysts is essential. Aside from the expected addition to substrates, the activated hydrogen species would also destroy the active structures. Here we show that, with the assistance of alkali cations, the atomically dispersed Ru(iii)

Dual photoredox/nickel-catalysed C–N cross-couplings suffer from low yields for electron-rich aryl halides. The formation of catalytically inactive nickel-black is responsible for this limitation and causes severe reproducibility issues. Here, we demonstrate that catalyst deactivation can be avoided by using a carbon nitride photocatalyst. The broad absorption of the heterogeneous photocatalyst enables

Repetitive start-up and shut-down events in polymer electrolyte membrane fuel cells for automotive applications lead to serious corrosion of the cathode due to an instantaneous potential jump that results from unintended air leakage into the anodic flow field followed by a parasitic oxygen reduction reaction (ORR) on the anode. Here we report a solution to the cathode corrosion issue during the start-up/shut-down

Unraveling how reactive facets promote photocatalysis at the molecular level remains a grand challenge, while identification of the reactive facets can provide guidelines for designing highly efficient photocatalysts and unravelling the microscopic mechanisms behind them. Recently, a series of polytriazine imides (PTIs) was reported with highly crystalline structures; all had a relatively low photocatalytic

How life can emerge from inanimate matter is one of the grand questions in science. Self-replicating molecules are necessary for the transition from chemistry to biology, but they need to acquire additional functions for life to emerge. Catalysis is one of the most essential of such functionalities, but mechanisms through which self-replicators can acquire catalytic and, in extension, metabolic properties

Chiral catalyst development is a key to asymmetric catalysis research. The enantioselectivity of a chiral catalyst relies on its ability to distinguish the prochiral centres or faces of substrates, which is difficult when the two groups attached to the centre or face are spatially and electronically similar. For example, dialkyl ketones are difficult to reduce enantioselectively. Here we report a protocol