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Femtosecond spectroscopy of photosynthetic systems reveals long-lived quantum coherences. This Review focuses on efforts to understand the microscopic origins of these signals and discusses how such coherences may be exploited to probe design principles of photosynthetic light harvesting.
Electrosynthesis is a practical and green route to hydrogen peroxide, and could reduce our dependence on less environmentally friendly oxidants. This Review describes catalyst and reactor designs for highly selective hydrogen peroxide electrosynthesis.
Senescence is a state of permanent cell cycle arrest. This Review highlights the chemical characteristics of senescence and how we can use small molecules to target, detect or eliminate senescent cells, as well as to induce or inhibit senescence.
Natural product biosynthetic pathways are rich in novel enzymology, but identifying the enzymes that perform new transformations remains challenging. This Review describes recently characterized examples of remarkable chemistries catalysed by biosynthetic enzymes and explores the extent of enzymatic novelty that awaits discovery.
Light emitting, molecularly tunable organic colour-centers are sp3 quantum defects that create localized two-level systems within the host crystals, providing unique tools to harness electrons, excitons, phonons and spin for novel functionality.
FoF1-ATPase is a vital molecular machine in organisms responsible for the catalytic synthesis of the basic energy unit ATP. In this Review, the development of FoF1-ATPase reconstitution into artificial architectures is discussed ultimately leading to the development of stimuli-responsive ATP synthesis.
The development of C–H functionalization methodology offers a new logic for chemical synthesis. Dirhodium tetracarboxylates have emerged as some of the most effective catalysts for these transformations, enabling site-selective and stereoselective insertion of transient metal carbenes into C–H bonds.
Water oxidation catalysts are key components in water-splitting devices that synthesize fuels by using energy, including that from sunlight. This Perspective presents historical developments in molecular water oxidation catalysis, emphasizing studies of ruthenium complexes that have taught us how to design optimal catalysts.
3D printing technology emerged as a tool for the design and fabrication of prototypes. Chemists are now using this technology to produce chemically reactive materials. In this Review, Hartings and Ahmed discuss different approaches to 3D print chemically reactive objects.
The selective conjugation of two or more molecules is readily achieved using covalent click chemistry or non-covalent click chemistry. The latter approach makes use of complementary molecular recognition partners, and its speed and reversibility are advantageous for many biological applications.
This Review highlights recent conceptual and/or technological advances in photoredox catalysis, organic electrosynthesis, electrostatic chemistry and synthesis in static electric fields, mechanochemistry and synthesis in flow.
Modelling composite systems with components on different length scales is challenging. However, multiscale models based on quantum and classical descriptions can describe these systems and represent the most effective way to explain and predict light-activated events in such complex systems.
Chiral molecules can filter electrons according to their spin. This chiral-induced spin selectivity (CISS) effect can have important applications, such as in spintronics and in enantioseparation. This Review describes the CISS effect, its mechanism and its fascinating applications.
Selective binding of multiple guests within cages could lead to new applications in catalysis and sensing. This Review discusses the design of synthetic cages with the aim of developing and controlling guest–guest chemistry.
Ethanol has emerged as a potential alternative feedstock for the synthesis of middle-distillate transportation fuels. This Review describes the chemistry of ethanol-to-distillate processes and challenges associated with improving current technologies and implementing new ones.
A quasi-liquid layer on the surface of ice makes it slippery even below the bulk melting temperature. The nature of this premelted layer has long been debated, and this Review gathers experimental and theoretical data and discusses opinions and evidence on premelting at ice surfaces.
Over the past 5 years, many novel site-selective protein modification techniques have been reported. Key features of these various strategies as well as prominent examples are discussed in this Review.
The high lithium-ion conductivity and deformability of solid sulfide electrolytes make them key materials in all-solid-state lithium batteries. Liquid-phase reactions are valid and scalable approaches for the preparation of sulfide-based solid electrolytes that overcome the issues of moisture sensitivity and high vapour pressures of sulfur species.
When presented with a light stimulus, heteroaryl azo photoswitches undergo molecular motion that can be harnessed for applications in materials science, catalyst design or drug development, among other fields. This Review describes selected subclasses of these versatile chemical motifs, covering their properties and prominent applications.
SO2 and NO2 are primary causes of air pollution and severe breathing problems worldwide. This Review gives an overview of the recent advances in the use of metal–organic framework materials to capture and remove these toxic gases from air.
Structurally complex natural products can be efficiently accessed through protecting-group-free (PGF) synthesis. This Review describes recent examples of PGF syntheses of terpenes and alkaloids, showcasing the power and elegance of innovative methods and strategies in natural product synthesis.
Super-resolution microscopy (SRM) has already proved to be a powerful lens for investigating biosystems. In this Review, the authors show how SRM can be very powerful in the study of synthetic material both in situ and in operando.
Automation can help in performing routine tasks quickly and consistently. Algorithms facilitate the searching of current knowledge. Combining the two could lead to a chemically intelligent approach to the discovery of not only new molecules but also novel and unpredictable reactivity.
This Perspective introduces energy decomposition analysis as a means of providing a quantum chemically derived bonding model that we can use to rationalize molecular geometries and bonding. The model serves as a bridge between the simple Lewis electron-pair bond and the complicated quantum theoretical nature of the chemical bond.
Lewis’ shared electron-pair model was a stroke of genius, describing the structure and reactivity of molecules purely on the basis of his tremendous knowledge of empirical chemistry without any quantum chemistry. Unprecedented in simplicity, its success unfortunately concealed some misleading interpretations of the physical origin of chemical bonding.
Ion mobility–mass spectrometry (IM-MS) is a gas-phase method for structural characterization — a tool prevalent in biology but only recently finding applications in supramolecular chemistry. This Perspective describes how IM-MS techniques give us information about the structures of molecular self-assemblies, host–guest complexes and metallosupramolecular systems.
Low-valent early transition metals are experiencing a renaissance in synthesis and catalysis, finding applications in unusual C–C bond forming reactions, oxidative group-transfer catalysis, proton-coupled electron transfer, photoredox catalysis and more.
Energy exchange between an excited photosensitizer and an annihilator can result in the upconversion of low-energy to high-energy light. Limiting the oxygen sensitivity of this process is essential for many biological applications. This Review discusses approaches to suppressing or alleviating such sensitivity.
3D printing is becoming a mainstream technology with considerable increase in access to affordable desktop printers. However, specific design principles and material considerations need to be weighed when printing functional devices that integrate catalytic and/or analytical functionalities, as well as when printing common laboratory hardware.
Engineered biocatalysts are increasingly being used for both the identification and manufacture of active pharmaceutical ingredients. Here, the authors review key developments that are expanding the use of biocatalysis in the pharmaceutical industry.
Noyori-type catalysts perform (de)hydrogenation and transfer (de)hydrogenation reactions at a metal centre coordinated to a N–H moiety. Understanding how these metal–ligand bifunctional catalysts operate enables us to design better catalysts for these reactions and for related conversions such as alcohol dehydrogenations, ester or carboxamide hydrogenations and dehydrogenative coupling of primary alcohols with other alcohols or amines.
Large increases in the amount of information produced year on year motivate the development of new storage media. This Review addresses the current status of data storage at the level of single polymer chains: in DNA, proteins and synthetic polymers.
This Perspective describes the physical molecular driving forces that stabilize native lignocellulosic plant biomass structures and govern thermochemical biomass pretreatments. Understanding these driving forces can help us to design efficient methods for deconstructing biomass into biofuels and other bioproducts.
One promising technology for modern energy and chemical conversions is chemical looping, central to which are redox cycles of metal oxides. This Review describes chemical looping schemes and the mechanisms by which metal oxide particles enable these technologies.
The modification of DNA at cytosine and thymine, such as methylation, hydroxylation and formylation, might have epigenetic roles. In this Review, the authors discuss established and newer methods for the detection of these modifications in genomic DNA.
Aqueous media containing homogeneously distributed soft dynamic structures can promote a wide range of synthetic and degradative chemical reactions. This promotion is illustrated by selected examples from academia and industry, as well as from the field of prebiotic chemistry.
Multivariate linear regression methods have become useful predictive tools that can complement potentially computationally expensive and complex transition state calculations. This Review compares these methods, highlights the advantages of each and identifies challenges for the future.
Nitrification and denitrification are responsible for the processing of ammonia fertilizer, ultimately leading to the generation of environmental pollutants that accumulate in waterways and the atmosphere. This Review describes the enzymes involved in these processes, which fascinate with their unusual active sites and the surprising reactions that they catalyse.
Non-viral vehicles for the delivery of nucleic acids have potential applications for the treatment of diseases by, for example, restoring, correcting or silencing the expression of genes. In this Review, the authors discuss the latest developments in synthetic materials used for gene delivery and the challenges that must be overcome to transfer these innovations into the clinic.
Surface plasmons can redistribute photoenergy over different time, space and energy scales and have been exploited in new spectroscopic techniques. This Review reports on how surface plasmons can also drive chemical reactions by localizing photon, electronic and/or thermal energies.
This Perspective describes how reversible catalysis — a hallmark of enzymes — can be reproduced in synthetic catalysts by rationally designing first and second coordination spheres, as well as amino acid-based outer coordination spheres. We describe this in the context of Ni prototypes for efficient H2 oxidation and evolution.
The study of [FeFe]-hydrogenases exemplifies how one can manipulate even sophisticated metal clusters to afford insights into structure–function relationships of biological catalysts. This Perspective describes developments in designing artificial proteins and catalytically active nucleic acids towards minimalistic and robust semi-biological catalysts for chemical synthesis.
Click chemistry enables efficient chemical labelling of small molecules in cells, providing a powerful method to visualize almost any biologically active compound. This versatile methodology can provide valuable information about the mechanisms of action of small molecules in various biological settings.
The discovery of bioactive small molecules is generally driven via iterative design–make–purify–test cycles. Progress has been made towards the automation and integration of adjacent stages within such discovery workflows, which can increase the efficiency and effectiveness of bioactive small-molecule discovery.
Semiconducting quantum dots (QDs) can serve as light-absorbing components in efficient artificial photosynthetic systems for H2 evolution. This Review describes how we can optimize QDs for H2 evolution using sacrificial reductants, before moving on to sustainable strategies for the photolysis of biomass or H2O.
Humans have evolved innate and adaptive immune systems to survive infection. Chemical approaches have enabled modulation of the immune system to activate or dampen it, leading to the development of new treatments for cancer and autoimmunity.
Traditional approaches for studying glycans can lack the precision required to uncover their roles in biomolecular processes. Progress has been made in the use of single molecule techniques for examining individual events in glycobiology — such as the molecular interactions of sugars and their roles in biological processes — within challenging mixtures.