When 2D materials are supported by substrates, matter trapped at the interface can coalesce to form nano- and microscale bubbles. These bubbles often negatively impact the performance of 2D material devices as they impede charge/photon/phonon transport across the interface. The difficulties created by these bubbles spurred research to understand how they form, whether their formation can be controlled

The ability to forge difficult chemical bonds through catalysis has transformed society on all fronts, from feeding the ever-growing population to increasing life expectancies through the synthesis of new drugs. However, developing new chemical reactions and catalytic systems is a tedious task that requires tremendous discovery and optimization efforts. Over the past decade, advances in machine learning

This review aims to draw attention to two issues of concern when we set out to make machine learning work in the chemical and materials domain, that is, statistical loss function metrics for the validation and benchmarking of data-derived models, and the uncertainty quantification of predictions made by them. They are often overlooked or underappreciated topics as chemists typically only have limited

Machine learning (ML) from large materials datasets enables accelerated materials discovery. Currently, the most accessible way to generate uniform, well-curated, voluminous datasets is by the application of high-throughput first principles computations. Here, we present the guiding principles of using computational data and ML to drive new materials discovery.

Introducing dynamic and exchangeable bonds can breathe life into polymers by imparting self-healing, enhanced toughness, or adaptability to the material. Synergies between the exchangeable bonds and the polymer’s architectural features can facilitate the dynamic exchange pathways and tune the material’s thermal and mechanical properties. In recent years, numerous dynamic chemistries and architectural

Anthropogenic CO2 emissions, primarily from the combustion of fossil fuels, are driving climate change at an alarming rate. Our current dependence on carbon-based fuels has motivated research interest in the capture and catalytic reduction of carbon dioxide back to liquid fuels. Electrochemical reduction of carbon dioxide has been intensely researched over the past decade. Here, some of the important

Chemical data have been created from many different origins. The chemicals themselves tend to be synthesized out of curiosity or as an industry-led need. Their materials characterization and development for functional applications generate cognate data about their structures and properties. Chemical structures and properties may also be computed ahead of their physical creation. The collation of all

Recent literature suggests that the fields of machine learning (ML) and high-throughput experimentation (HTE) have separately received considerable attention from chemists and engineers, leading to the development of powerful reactivity models and platforms capable of rapidly performing thousands of reactions. The merger of ML with HTE presents a wealth of opportunities for the exploration of chemical

While the amide bond is one of the most widespread backbones in natural peptides, pharmaceuticals, and agrochemicals, the atom-economic synthesis of amides remains a major challenge in organic chemistry. In this context, transition-metal-catalyzed hydroaminocarbonylation of cost-effective alkenes and alkynes has emerged as an ideal approach to access amides. However, it is only in recent times that

Ideally, electrochemical synthesis processes should perform value-added chemistries at both electrodes. However, electrochemical reactions are typically studied and optimized one half-reaction at a time and integrating different half-reactions into one cell often poses significant compatibility challenges. Wang et al. employed heterogeneous redox reservoirs to temporarily store charge and sequentially

Recently, DNA-encoded library (DEL) technology has emerged as an innovative screening modality for the rapid discovery of therapeutic candidates in pharmaceutical settings. This platform enables a cost-effective, time-efficient, and large-scale assembly and interrogation of billions of small organic ligands against a biological target in a single experiment. An outstanding challenge in DEL synthesis

The synthetic proficiency of transition metal-catalyzed functionalization of dormant C-H bonds has established it as one of the leading methods for diversifying organic molecules. Palladium-based complexes are reckoned as front-runners for this purpose, primarily due to their low activation barrier during redox state shuffling. Despite the advances, exquisite stereoselective C-H activation remains

The generation and evolutional behavior of the solid-electrolyte interphase (SEI) fatally dictate the performance of working anodes, especially lithium (Li) anodes. In this Opinion, we describe the critical rationale in understanding competitive SEI formation on a working Li metal anode. First, the fundamentals that determine the competitive SEI-forming reactions at the Li/electrolyte interface are

There have been breakthroughs in the mass production of graphene by chemical vapor deposition (CVD) and its practical applications have also been identified. Grain boundaries are typically present in ‘CVD graphene’ and adversely impact its properties. We summarize recent progress in growing large-area single-crystal graphene. Centimeter-scale single-crystal, truly single-layer graphene (SLG) films

Metal halide perovskites have shown rapid development in various fields such as photovoltaics, photodetectors, light-emitting diodes (LEDs), and optically pumped lasers owing to their superior optoelectronic properties. Here, we review the basic optoelectronic properties of halide perovskites from a photophysical perspective. We highlight that halide perovskites are promising in various optoelectronic

Cancer remains a leading cause of death worldwide. Despite breakthrough clinical therapies for the treatment of cancer using platinum and arsenic compounds, metal complexes have received relatively little attention from industrial anticancer drug discovery programs over the last few decades. The chemical diversity and versatility offered by metal complexes, arising from the choice of metal, oxidation

Atomic layer deposition (ALD) has been extensively used in the modification of semiconductor surfaces for scientific and industrial applications. It employs labile organometallic precursors that add to the surface layers of solids in a vacuum that are subsequently activated by surface hydrolysis. In recent applications, it has been used in the preparation of electrodes for molecularly based dye-sensitized

Biological CO2 fixation can inspire critical design elements when developing catalytic processes to convert CO2 into useful chemicals. Two recent studies report molecular catalysts for CO2 reduction to selectively produce formate and methane. The catalyst structures mimic the active sites of two CO dehydrogenase enzymes to uncover novel CO2 activation mechanisms and unprecedented product selectivities

Designing functional molecules with desirable properties is often a challenging, multi-objective optimization. For decades, there have been computational approaches to facilitate this process through the simulation of physical processes, the prediction of molecular properties using structure–property relationships, and the selection or generation of molecular structures. This review provides an overview

Late-metal–ligand multiply bonded complexes are typically highly reactive species and are proposed intermediates in a variety of catalytic bond activations. Using spectroscopic, theoretical, and in situ photocrystallographic tools, Holthausen, Schneider, et al. report the first bona fide metallonitrene complex and illuminate structure-activity relationships critical to catalyst development.

Thermocells (also called thermo-electrochemical cells) are a promising technology for converting low-grade heat (<200°C) into electricity through temperature-dependent redox reactions and/or ion diffusion. Very recently, there have been several breakthroughs in thermocells regarding Seebeck coefficients up to 34 mVK–1 and efficiencies up to 11% by optimizing thermo-electrochemical processes. Proof-of-concept

The cobalamin-dependent radical SAM enzyme CysS performs methylation reactions at an unactivated carbon center using what is predicted to be an unprecedented radical substitution mechanism. Herein, we highlight significant progress made by Wang and Begley in providing support for the enzymatic relevance of this proposal.

A novel strategy to introduce C-isotopes at the carboxylate group has been discovered. Through ‘simple’ CO2 exchange under mild conditions, the C-isotope can be incorporated effectively and has been demonstrated in a variety of biologically important molecules. Also, this methodology is used to install a C–C bond when alternative electrophiles are employed.

In recent years, dynamic covalent chemistry (DCC) has seen the synthesis of increasingly complex cyclooligomers, polymers, and diverse compound libraries. The reversible formation of covalent bonds characteristic of DCC reactions favors thermodynamic product distributions for simple unitopic reactions; however, kinetic effects are increasingly influential in reactions of multitopic precursors. In this

Racemic natural products with complex molecular structures have inspired chemists for decades. Their widespread occurrence raises interesting biosynthetic questions and poses (retro)synthetic challenges. Using some classic examples and representative work from the recent literature, we show how biomimetic synthesis can address some of these questions and challenges, provide insights into the formation

In recent years, solvent-less mechanochemical organic transformations using ball milling have come to the forefront of organic synthesis as cleaner and sustainable synthetic alternatives. Apart from the environmental benefits, mechanochemical approaches potentially enable access to novel chemical space that has reactivities and selectivities different from those of conventional solution-based reactions

Phototherapy, including photodynamic therapy (PDT) and photothermal therapy (PTT), exploits light to activate photoreactions that kill cancer cells. Recent studies show that phototherapy can not only kill irradiated tumor cells, but also elicit a tumor-specific immune response. This phenomenon breaks the limitations of conventional phototherapy and has reinvigorated phototherapy-related research in

N-heterocyclic carbenes (NHCs) are a widely used class of ligands that have enabled an exciting variety of organometallic chemistry and catalysis. As researchers design and customize these ligands for specific applications, various design concepts have emerged. This review covers several of these design concepts and their impact on and promise for organometallic chemistry and catalysis. These concepts

Catalysts development is an evolutionary process. The generation of new single-metal-site catalysts, with isolated metal atoms dispersed on the surface of substrates, offers maximum atom-utilization efficiency, high specific activity, and novel properties. The unique structure of single-site catalysts also enables their potential to bridge the gap between homogeneous and heterogeneous catalysis. This

Photo-therapeutics have attracted increasing attention for the treatment of tumors because of their controllable and tunable nature and low potential for side effects. Photocatalytic materials triggered by targeted wavelengths of light facilitate the generation of reactive oxygen species for tumor DNA damage, allowing for high efficacy at low radiation doses with limited damage of normal tissues. This

Retrospective testing of predictive models does not consider the real-world context in which models are deployed. Prospective validation, however, enables meaningful comparisons between data generation processes by incorporating trained models and considering the subjective decisions that affect reproducibility. Prospective experiments are essential for consistent progress in modeling.

Understanding the role of symmetry in the physical sciences is critical for choosing an appropriate machine-learning method. While invariant models are the most prevalent symmetry-aware models, equivariant models such as Euclidean neural networks more faithfully represent physical interactions and are ready to take on challenges across the physical sciences.

Chemical heuristics have been fundamental to the advancement of chemistry and materials science. These heuristics are typically established by scientists using knowledge and creativity to extract patterns from limited datasets. Machine learning offers opportunities to perfect this approach using computers and larger datasets. Here, we discuss the relationships between traditional heuristics and machine

Indole and isoquinoline nuclei bearing homoallylic amine cores are abundant in several prominent alkaloids, including strychnine. A recent study by Snaddon et al. reports a modular, cooperative catalysis platform to access linear and branched homoallylic amines, thereby streamlining enantioselective access to stereochemically complex Strychnos and Chelidonium alkaloids.

Retinal prostheses with high spatial resolution and sensitivity are desired to restore vision in patients with retinal degenerative diseases. A recent publication by Benfenati et al. demonstrates the use of semiconducting polymer nanoparticles (NPs) as a liquid retinal prosthesis with significant potential to restore high-acuity vision.

The abundance and structural diversity of hydroxide-containing secondary building units (SBUs) in metal–organic frameworks (MOFs) have provided unique opportunities for the development of transition metal (TM) catalysts. This minireview surveys the structures of hydroxide-containing SBUs and summarizes recently developed strategies for the generation of catalytically active metal complexes on these

Quantum mechanical tunneling is a consequence of the wave nature of particles that implies that a particle can penetrate a potential energy barrier even though there is insufficient energy to overcome it. This has serious consequences for chemical reactions, a fact that has, however, not been appreciated fully. Only in the last few years has it become clear how important tunneling is for understanding

Since their discovery a few decades ago, metal–organic frameworks (MOFs) have suffered from poor hydrolytic stability. Since then, significant effort has been devoted to design robust MOFs, including their utilization for water-related applications to overcome relevant societal challenges. This short review provides guidelines on the key parameters that drive the assembly of hydrothermally stable MOFs

C–N bond-forming reactions represent an important synthetic class because amine derivatives play crucial roles in various applications in biology and synthetic chemistry. Recently, electrochemical C–N bonding methods have attracted attention due to several advantages such as their simplicity and possibility of low-cost scale up. Meanwhile, due to severe environmental problems such as global warming

Lithium-sulfur (Li-S) batteries exhibit great promise for next-generation energy storage due to their high theoretical energy density and low cost. However, their practical application is largely hindered by the shuttle effect. Although previous studies on the adsorption of lithium polysulfides (LiPSs) have achieved significant progress, simple adsorption cannot fundamentally eliminate the shuttle

The ability of bismuth to manoeuvre between oxidation states supports several distinct reaction manifolds. Recent advances in the design, synthesis, and application of organobismuth reagents and catalysts illustrate the potential of these redox manifolds as tools complementary to conventional transition-metal-based synthetic strategies.

The development of high-speed, nonvolatile memory devices with low power consumption remains a significant challenge for next-generation computing. A recent study reported molecular switches operating at low voltages in large-area junctions by coupling supramolecular structural changes and counterion migration to bias-dependent redox, culminating in proof-of-concept memory comprising self-assembled

The sluggish kinetics and side reactions of the oxygen reduction reaction have impeded deployment of proton-exchange-membrane fuel cells. A recent article (Xie et al.) introduces an efficient nonprecious metal catalyst (Fe2N6) that enhances the kinetics of 4-electron O2 reduction by more than seven times compared with that of the well-documented single-site FeN4 catalysts.

Harnessing the chemistry of onium ylide intermediates generated from transition metal catalysis is a powerful strategy to convert simple precursors into complex scaffolds. Although the chemistry of onium ylides has been studied for over three decades, transformations of aziridinium ylides have only recently emerged as a versatile way to exploit the strain of these reactive intermediates to furnish

The ever-growing push for sustainable energy has intensified research on catalytic science. Significant developments have been achieved in state-of-the-art catalyst design from the perspective of catalyst materials. Further promotion can be enabled when rethinking and redesigning the catalyst structure with long-range ordering rather than limited to the catalyst material design. Recently, ordered assembled

Lignin is a potential non-fossil resource of diverse functionalized phenolic units. The most important lignin-derived monomers are 4-alkylphenols, 4-hydroxybenzaldehydes, 4-hydroxybenzoic acids, and 4-hydroxycinnamic acids/esters. Efficient transformation of lignin and/or its monomers into valuable aromatics and their derivatives is crucial, not only for a sustainable lignocellulose biorefinery, but

The amide bond represents the most fundamental functional group in numerous areas of chemistry, such as organic synthesis, drug discovery, polymers, and biochemistry. Although typical amides are planar and the amide N–C(O) bond is notoriously difficult to break due to nN→π⁎C=O resonance, over the past 5 years remarkable breakthroughs have been achieved in the activation of amides by complementary mechanisms

Tandem catalysis capable of completing multistep reactions in a single pot or step is an effective strategy to develop cost-effective and environmentally benign chemical processes. A unique challenge in the selectivity control of tandem reactions is the coexistence of reactants, intermediates, and products from all constituent steps in the same reaction medium, causing side reactions. Thus, distinct

Hydrogen peroxide (H2O2) is a valuable chemical with a wide range of applications. A recent trend in H2O2 production focuses on electrochemical reduction of oxygen, which represents an environmentally friendly method for on-site H2O2 generation. To realize highly efficient practical-scale electrosynthesis of H2O2, catalytic materials design and electrochemical reactor engineering play equally important

Macrocycles and related hosts are now being used to reverse the effects of poisonous substances and to alleviate the toxicity of several medicines in vivo. Here, we showcase the emergence of this class of compounds behaving as supramolecular antidotes, some of which outperform ‘gold standards’ in the field.

Over the last decade, pillararenes have shown remarkable potential in a variety of fields by virtue of their symmetrical pillar-shaped structures, flexible functionalization, and unique host–guest interactions. For diverse pillararene-based functional materials and technical applications, the tailored design and construction of pillararene-based supramolecular structures and assemblies are critical

A recent work by Hartwig et al. details an efficient method to borylate strong primary C(sp3)–H bonds via iridium-catalysed C–H activation. The conditions confer counterintuitive selectivity over more labile C–H bonds, while providing an avenue for a gamut of synthetically valuable late-stage functionalisations through versatile borylate intermediates.

CO2-neutral fuels (e-fuels) are considered to be a pragmatic and practical way of decreasing overall CO2 emissions derived from the transportation sector. However, for e-fuels to succeed and have a short-to-medium impact on climate mitigation, they should be fully compatible with existing fuel distribution infrastructure and vehicle technologies, such that they become literally drop-in replacements

Light-emitting diodes (LEDs) based on metal halide perovskite nanocrystals (MHP NCs) have been rapidly developed to reach external quantum efficiencies of up to 22% with their defect-tolerant nature and extremely high color purity (full width half maxima <25 nm) that are superior to traditional inorganic colloidal quantum dots. However, highly dynamic binding of ligands impedes further increase in

This forum article highlights atomic nanoarchitectonics for functional atomic rearrangement and organic nanoarchitectonics for functional unit manipulation. The latter enables organic-synthetic modifications of nano-units from nanotechnological processes. This innovative approach affords creation of new chemical trends, expanding the seemingly endless possibilities of organic synthesis.

The electrochemical reduction of CO2 remains an appealing option for storing renewable energy in a chemical form. In this review, we assess progress in designing catalysts that convert CO2 to high energy density products. We explain how reaction data can be reported to reflect the intrinsic properties of the catalyst. This analysis shows that limited advances have been made in improving the performance

Hydride from sodium hydride acts as a base and not as a nucleophile, due to its small size and high charge density. However, recent research has found that a sodium hydride–sodium iodide composite can be a unique hydride donor in the challenging partial reduction of inert amides to imines.

Sunlight-driven photocatalytic water splitting is one of the most promising approaches to generating renewable hydrogen as an energy source. In recent years, significant progress has been made in the development of photocatalytic water-splitting systems. Among these, the one- and two-step-excitation overall water-splitting processes are most widely investigated. Realization of visible-light-driven

Basic research on the photophysical and photochemical properties of metal triplet emitters has been fueled by their practical applications in diverse areas, including bioimaging, photocatalysis, and organic light-emitting diodes (OLEDs). In addition to the extensively investigated Ru(II), Ir(III), and Pt(II) complexes, a wide range of luminescent Pd(II), Au(III)/Au(I), Re(I), Cu(I), W(VI)/W(0), and

Several hundred million tons of plastics produced worldwide accumulate in nature. The thermoplastic resin polyethylene terephthalate (PET) is highly recalcitrant to degradation. A recent report from Tournier and colleagues provides unprecedented advances towards a circular PET economy by describing an engineered microbial enzyme that efficiently depolymerizes PET.