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    Boron-Heteroatom Addition Reactions via Borylative Heterocyclization: Oxyboration, Aminoboration, and Thioboration.
    Acc Chem Res 2017 Sep 21. Epub 2017 Sep 21.
    Department of Chemistry, University of California , Irvine, California 92697-2025, United States.
    Organoboron compounds and heterocycles are powerful building blocks and precursors for organic synthesis, including for drug discovery and agrochemical and material synthesis. The common strategy for the synthesis of borylated heterocycles involves two separate synthetic steps: first, synthesis of the heterocyclic core, and second, borylation of the core through established methods such as transition-metal-catalyzed C-H or C-X activation/borylation or lithiation/borylation. In this Account, we describe our laboratory's development of borylative heterocyclization reactions that access the heterocyclic core and install boron in one synthetic step. Read More

    C- and N-Metalated Nitriles: The Relationship between Structure and Selectivity.
    Acc Chem Res 2017 Sep 20. Epub 2017 Sep 20.
    Department of Chemistry, Drexel University , Philadelphia, Pennsylvania 19104, United States.
    Metalated nitriles are exceptional nucleophiles capable of forging highly hindered stereocenters in cases where enolates are unreactive. The excellent nucleophilicity emanates from the powerful inductive stabilization of adjacent negative charge by the nitrile, which has a miniscule steric demand. Inductive stabilization is the key to understanding the reactivity of metalated nitriles because this permits a continuum of structures that range from N-metalated ketenimines to nitrile anions. Read More

    New Triplet Sensitization Routes for Photon Upconversion: Thermally Activated Delayed Fluorescence Molecules, Inorganic Nanocrystals, and Singlet-to-Triplet Absorption.
    Acc Chem Res 2017 Sep 20. Epub 2017 Sep 20.
    Department of Chemistry and Biochemistry, Graduate School of Engineering, Center for Molecular Systems (CMS), Kyushu University , 744 Moto-oka, Nishi-ku, Fukuoka 819-0395, Japan.
    Photon upconversion based on triplet-triplet annihilation (TTA-UC) has attracted much interest because of its possible applications to renewable energy production and biological fields. In particular, the UC of near-infrared (NIR) light to visible (vis) light is imperative to overcome the Shockley-Queisser limit of single-junction photovoltaic cells, and the efficiency of photocatalytic hydrogen production from water can also be improved with the aid of vis-to-ultraviolet (UV) UC. However, both processes have met limitations in the wavelength range, efficiency, and sensitivity for weak incident light. Read More

    Novel Strategies for the Production of Fuels, Lubricants, and Chemicals from Biomass.
    Acc Chem Res 2017 Sep 20. Epub 2017 Sep 20.
    Energy BioSciences Institute, University of California , 2152 Berkeley Way, Berkeley, California 94720, United States.
    Growing concern with the environmental impact of CO2 emissions produced by combustion of fuels derived from fossil-based carbon resources has stimulated the search for renewable sources of carbon. Much of this focus has been on the development of methods for producing transportation fuels, the major source of CO2 emissions today, and to a lesser extent on the production of lubricants and chemicals. First-generation biofuels such as bioethanol, produced by the fermentation of sugar cane- or corn-based sugars, and biodiesel, produced by the transesterification reaction of triglycerides with alcohols to form a mixture of long-chain fatty esters, can be blended with traditional fuels in limited amounts and also arise in food versus fuel debates. Read More

    Synthesis and Properties of 2D Carbon-Graphdiyne.
    Acc Chem Res 2017 Sep 15. Epub 2017 Sep 15.
    Beijing National Laboratory for Molecular Sciences (BNLMS), CAS Key Laboratory of Organic Solids, Institute of Chemistry, CAS Research/Education Center for Excellence in Molecular Sciences, Chinese Academy of Sciences , Beijing 100190, P. R. China.
    Graphdiyne (GDY) is a flat material comprising sp(2)- and sp-hybridized carbon atoms with high degrees of π conjugation that features uniformly distributed pores. It is interesting not only from a structural point of view but also from the perspective of its electronic, chemical, mechanical, and magnetic properties. We have developed an in situ homocoupling reaction of hexaethynylbenzene on Cu foil for the fabrication of large-area ordered films of graphdiyne. Read More

    The Evolution of DNA-Templated Synthesis as a Tool for Materials Discovery.
    Acc Chem Res 2017 Sep 15. Epub 2017 Sep 15.
    Department of Chemistry, University of Warwick , Coventry CV4 7AL, United Kingdom.
    Precise control over reactivity and molecular structure is a fundamental goal of the chemical sciences. Billions of years of evolution by natural selection have resulted in chemical systems capable of information storage, self-replication, catalysis, capture and production of light, and even cognition. In all these cases, control over molecular structure is required to achieve a particular function: without structural control, function may be impaired, unpredictable, or impossible. Read More

    Design of Donor Polymers with Strong Temperature-Dependent Aggregation Property for Efficient Organic Photovoltaics.
    Acc Chem Res 2017 Sep 15. Epub 2017 Sep 15.
    HKUST-Shenzhen Research Institute , No. 9 Yuexing first Road, Hi-tech Park, Nanshan, Shenzhen 518057, China.
    Bulk heterojunction (BHJ) organic solar cells (OSCs) have attracted intensive research attention over the past two decades owing to their unique advantages including mechanical flexibility, light weight, large area, and low-cost fabrications. To date, OSC devices have achieved power conversion efficiencies (PCEs) exceeding 12%. Much of the progress was enabled by the development of high-performance donor polymers with favorable morphological, electronic, and optical properties. Read More

    Cell-Surface Interactions on Arginine-Rich Cell-Penetrating Peptides Allow for Multiplex Modes of Internalization.
    Acc Chem Res 2017 Sep 14. Epub 2017 Sep 14.
    Nanoscience and Nanotechnology Research Center, Research Organization for the 21st Century, Osaka Prefecture University , Naka-ku, Sakai, Osaka 599-8570, Japan.
    One of the recent hot topics in peptide-related chemical biology research is the potential of cell-penetrating peptides (CPPs). Owing to their ability to deliver exogenous molecules into cells easily and effectively, their flexible design that allows transporters to comprise various chemical structures and functions, and their potential in chemical and cell biology studies and clinical applications, CPPs have been attracting enormous interest among researchers in related fields. Consequently, publications on CPPs have increased significantly. Read More

    High-Purity Semiconducting Single-Walled Carbon Nanotubes: A Key Enabling Material in Emerging Electronics.
    Acc Chem Res 2017 Sep 13. Epub 2017 Sep 13.
    National Research Council of Canada , Ottawa, Ontario, Canada K1A 0R6.
    Semiconducting single-walled carbon nanotubes (sc-SWCNTs) are emerging as a promising material for high-performance, high-density devices as well as low-cost, large-area macroelectronics produced via additive manufacturing methods such as roll-to-roll printing. Proof-of-concept demonstrations have indicated the potential of sc-SWCNTs for digital electronics, radiofrequency circuits, radiation hard memory, improved sensors, and flexible, stretchable, conformable electronics. Advances toward commercial applications bring numerous opportunities in SWCNT materials development and characterization as well as fabrication processes and printing technologies. Read More

    Three Principles of Diversity-Generating Biosynthesis.
    Acc Chem Res 2017 Sep 11. Epub 2017 Sep 11.
    Department of Medicinal Chemistry, University of Utah , Salt Lake City, Utah 84112 United States.
    Natural products are significant therapeutic agents and valuable drug leads. This is likely owing to their three-dimensional structural complexity, which enables them to form complex interactions with biological targets. Enzymes from natural product biosynthetic pathways show great potential to generate natural product-like compounds and libraries. Read More

    CuAAC-Based Click Chemistry in Self-Healing Polymers.
    Acc Chem Res 2017 Sep 11. Epub 2017 Sep 11.
    Chair of Macromolecular Chemistry, Faculty of Natural Science II (Chemistry, Physics and Mathematics), Martin Luther University Halle-Wittenberg , Von-Danckelmann-Platz 4, D-06120 Halle (Saale), Germany.
    Click chemistry has emerged as a significant tool for materials science, organic chemistry, and bioscience. Based on the initial concept of Barry Sharpless in 2001, the copper(I)-catalyzed azide/alkyne cycloaddition (CuAAC) reaction has triggered a plethora of chemical concepts for linking molecules and building blocks under ambient conditions, forming the basis for applications in autonomous cross-linking materials. Self-healing systems on the other hand are often based on mild cross-linking chemistries that are able to react either autonomously or upon an external trigger. Read More

    Oligoprolines as Molecular Entities for Controlling Distance in Biological and Material Sciences.
    Acc Chem Res 2017 Sep 8. Epub 2017 Sep 8.
    ETH Zürich , Laboratory of Organic Chemistry, D-CHAB, Vladimir-Prelog-Weg 3, CH-8093 Zürich, Switzerland.
    Nature utilizes large biomolecules to fulfill tasks that require spatially well-defined arrangements at the molecular level such as electron transfer, ligand-receptor interactions, or catalysis. The creation of synthetic molecules that enable precise control over spacing and functionalization provides opportunities across diverse disciplines. Key requirements of functionalizable oligomeric scaffolds include the specific control of their molecular properties where the correct balance of flexibility and rigidity must be maintained in addition to the prerequisite of defined length. Read More

    Novel in Situ Techniques for Studies of Model Catalysts.
    Acc Chem Res 2017 Sep 7;50(9):2326-2333. Epub 2017 Sep 7.
    Division of Synchrotron Radiation Research, Lund University , Box 118, Lund S-221 00, Sweden.
    Motivated mainly by catalysis, gas-surface interaction between single crystal surfaces and molecules has been studied for decades. Most of these studies have been performed in well-controlled environments and have been instrumental for the present day understanding of catalysis, providing information on surface structures, adsorption sites, and adsorption and desorption energies relevant for catalysis. However, the approach has been criticized for being too far from a catalyst operating under industrial conditions at high temperatures and pressures. Read More

    Bioorthogonal Cycloadditions: Computational Analysis with the Distortion/Interaction Model and Predictions of Reactivities.
    Acc Chem Res 2017 Sep 6;50(9):2297-2308. Epub 2017 Sep 6.
    Department of Chemistry and Biochemistry, University of California , Los Angeles, California 90095, United States.
    Bioorthogonal chemistry has had a major impact on the study of biological processes in vivo. Biomolecules of interest can be tracked by using probes and reporters that do not react with cellular components and do not interfere with metabolic processes in living cells. Much time and effort has been devoted to the screening of potential bioorthogonal reagents experimentally. Read More

    Supramolecular Assembly of Peptide Amphiphiles.
    Acc Chem Res 2017 Sep 6. Epub 2017 Sep 6.
    Simpson Querrey Institute for BioNanotechnology, Northwestern University , Chicago, Illinois 60611, United States.
    Peptide amphiphiles (PAs) are small molecules that contain hydrophobic components covalently conjugated to peptides. In this Account, we describe recent advances involving PAs that consist of a short peptide sequence linked to an aliphatic tail. The peptide sequence can be designed to form β-sheets among the amino acids near the alkyl tail, while the residues farthest from the tail are charged to promote solubility and in some cases contain a bioactive sequence. Read More

    Electron Bifurcation: Thermodynamics and Kinetics of Two-Electron Brokering in Biological Redox Chemistry.
    Acc Chem Res 2017 Sep 6;50(9):2410-2417. Epub 2017 Sep 6.
    Department of Biochemistry, Duke University , Durham, North Carolina 27710, United States.
    How can proteins drive two electrons from a redox active donor onto two acceptors at very different potentials and distances? And how can this transaction be conducted without dissipating very much energy or violating the laws of thermodynamics? Nature appears to have addressed these challenges by coupling thermodynamically uphill and downhill electron transfer reactions, using two-electron donor cofactors that have very different potentials for the removal of the first and second electron. Although electron bifurcation is carried out with near perfection from the standpoint of energy conservation and electron delivery yields, it is a biological energy transduction paradigm that has only come into focus recently. This Account provides an exegesis of the biophysical principles that underpin electron bifurcation. Read More

    The Curious Case of Fluorination of Conjugated Polymers for Solar Cells.
    Acc Chem Res 2017 Sep 5;50(9):2401-2409. Epub 2017 Sep 5.
    Department of Chemistry, University of North Carolina at Chapel Hill , Chapel Hill, North Carolina 27599-3290, United States.
    Organic solar cells (OSCs) have been a rising star in the field of renewable energy since the introduction of the bulk heterojunction (BHJ) in 1992. Recent advances have pushed the efficiencies of OSCs to over 13%, an impressive accomplishment via collaborative efforts in rational materials design and synthesis, careful device engineering, and fundamental understanding of device physics. Throughout these endeavors, several design principles for the conjugated donor polymers used in such solar cells have emerged, including optimizing the conjugated backbone with judicious selection of building blocks, side-chain engineering, and substituents. Read More

    Guest-Responsive Metal-Organic Frameworks as Scaffolds for Separation and Sensing Applications.
    Acc Chem Res 2017 Sep 5. Epub 2017 Sep 5.
    Department of Chemistry, Indian Institute of Science Education and Research (IISER) Pune , Dr. Homi Bhabha Road, Pashan, Pune-411 008, India.
    Metal-organic frameworks (MOFs) have evolved to be next-generation utility materials because of their serviceability in a wide variety of applications. Built from organic ligands with multiple binding sites in conjunction with metal ions/clusters, these materials have found profound advantages over their other congeners in the domain of porous materials. The plethora of applications that these materials encompass has motivated material chemists to develop such novel materials, and the catalogue of MOFs is thus ever-escalating. Read More

    Rare Earth Polyoxometalates.
    Acc Chem Res 2017 Sep 5;50(9):2205-2214. Epub 2017 Sep 5.
    School of Chemistry, University of Melbourne , Parkville, Victoria 3010, Australia.
    Longstanding and important applications make use of the chemical and physical properties of both rare earth metals and polyoxometalates of early transition metals. The catalytic, optical, and magnetic features of rare earth metal ions are well-known, as are the reversible multielectron redox and photoredox capabilities of polyoxomolybdates and polyoxotungstates. The combination of rare earth ions and polyoxometalates in discrete molecules and coordination polymers is of interest for the unique combination of chemical and physical properties that can arise. Read More

    Development of Selective Peptide Catalysts with Secondary Structural Frameworks.
    Acc Chem Res 2017 Sep 5. Epub 2017 Sep 5.
    Institute of Industrial Science, The University of Tokyo , 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan.
    Enzymes are biogenic catalysts that enable the vital activity of organisms. Enzymes promote reactions in a selective manner with a high level of substrate recognition ability. The development of such a sophisticated catalyst has been one of the goals for chemists. Read More

    Silver Clusters in Zeolites: From Self-Assembly to Ground-Breaking Luminescent Properties.
    Acc Chem Res 2017 Sep 1;50(9):2353-2361. Epub 2017 Sep 1.
    Chem&Tech - Molecular Imaging and Photonics, KU Leuven , Celestijnenlaan 200F, B-3001 Leuven, Belgium.
    Interest for functional silver clusters (Ag-CLs) has rapidly grown over years due to large advances in the field of nanoscale fabrication and materials science. The continuous development of strategies to fabricate small-scale silver clusters, together with their interesting physicochemical properties (molecule-like discrete energy levels, for example), make them very attractive for a wide variety of applied research fields, from biotechnology and the environmental sciences to fundamental chemistry and physics. Apart from useful catalytic properties, silver clusters (Agn, n < 10) were recently shown to also exhibit exceptional optical properties. Read More

    Clay, Water, and Salt: Controls on the Permeability of Fine-Grained Sedimentary Rocks.
    Acc Chem Res 2017 Sep 1;50(9):2067-2074. Epub 2017 Sep 1.
    Lawrence Berkeley National Laboratory , Energy Geoscience Division, Berkeley California 94720, United States.
    The ability to predict the permeability of fine-grained soils, sediments, and sedimentary rocks is a fundamental challenge in the geosciences with potentially transformative implications in subsurface hydrology. In particular, fine-grained sedimentary rocks (shale, mudstone) constitute about two-thirds of the sedimentary rock mass and play important roles in three energy technologies: petroleum geology, geologic carbon sequestration, and radioactive waste management. The problem is a challenging one that requires understanding the properties of complex natural porous media on several length scales. Read More

    Anodic Cyclization Reactions and the Mechanistic Strategies That Enable Optimization.
    Acc Chem Res 2017 Sep 31;50(9):2346-2352. Epub 2017 Aug 31.
    Department of Chemistry, Washington University , St. Louis, Missouri 63130, United States.
    Oxidation reactions are powerful tools for synthesis because they allow us to reverse the polarity of electron-rich functional groups, generate highly reactive intermediates, and increase the functionality of molecules. For this reason, oxidation reactions have been and continue to be the subject of intense study. Central to these efforts is the development of mechanism-based strategies that allow us to think about the reactive intermediates that are frequently central to the success of the reactions and the mechanistic pathways that those intermediates trigger. Read More

    Synthesis and Applications of Boronate Affinity Materials: From Class Selectivity to Biomimetic Specificity.
    Acc Chem Res 2017 Sep 29;50(9):2185-2193. Epub 2017 Aug 29.
    State Key Laboratory of Analytical Chemistry for Life Science, School of Chemistry and Chemical Engineering, Nanjing University , Nanjing 210023, China.
    Due to the complexity of biological systems and samples, specific capture and targeting of certain biomolecules is critical in much biological research and many applications. cis-Diol-containing biomolecules, a large family of important compounds including glycoproteins, saccharides, nucleosides, nucleotides, and so on, play essential roles in biological systems. As boronic acids can reversibly bind with cis-diols, boronate affinity materials (BAMs) have gained increasing attention in recent years. Read More

    Chemical Protein Synthesis with the α-Ketoacid-Hydroxylamine Ligation.
    Acc Chem Res 2017 Sep 29;50(9):2104-2115. Epub 2017 Aug 29.
    Laboratorium für Organische Chemie, Department of Chemistry and Applied Biosciences, ETH Zürich , 8093 Zürich, Switzerland.
    The coupling of an α-ketoacid and a hydroxylamine (KAHA ligation) affords amide bonds under aqueous, acidic conditions without the need for protecting groups or coupling agents. Translating this finding into a general approach to chemical protein synthesis required the identification of methods to incorporate the key functional groups into unprotected peptide segments-ideally using well-established Fmoc solid-phase peptide synthesis protocols. A decade of effort has now led to robust, convenient methods for preparing peptides bearing free or masked C-terminal α-ketoacids and N-terminal hydroxylamines. Read More

    Rates of CO2 Mineralization in Geological Carbon Storage.
    Acc Chem Res 2017 Sep 28;50(9):2075-2084. Epub 2017 Aug 28.
    Department of Earth and Planetary Science, UC Berkeley , 307 McCone Hall Berkeley, California 94720-4767, United States.
    Geologic carbon storage (GCS) involves capture and purification of CO2 at industrial emission sources, compression into a supercritical state, and subsequent injection into geologic formations. This process reverses the flow of carbon to the atmosphere with the intention of returning the carbon to long-term geologic storage. Models suggest that most of the injected CO2 will be "trapped" in the subsurface by physical means, but the most risk-free and permanent form of carbon storage is as carbonate minerals (Ca,Mg,Fe)CO3. Read More

    Heading toward Macromolecular and Nanosized Bioresponsive MRI Probes for Successful Functional Imaging.
    Acc Chem Res 2017 Sep 25;50(9):2215-2224. Epub 2017 Aug 25.
    MR Neuroimaging Agents, Max Planck Institute for Biological Cybernetics , D-72076 Tuebingen, Germany.
    The quest for bioresponsive or smart contrast agents (SCAs) in molecular imaging, in particular magnetic resonance imaging (MRI), is progressively increasing since they allow for the monitoring of essential biological processes on molecular and cellular levels in a dynamic fashion. These are offshoot molecules of common contrast agents that are sensitive to biochemical changes in their environment, capable of reporting on such changes by inducing MRI signal alteration. Various mechanistic approaches and different types of SCAs have been developed in order to visualize desired processes, using diverse imaging protocols and methods. Read More

    Metallosupramolecular Architectures Obtained from Poly-N-heterocyclic Carbene Ligands.
    Acc Chem Res 2017 Sep 25;50(9):2167-2184. Epub 2017 Aug 25.
    Institut für Anorganische und Analytische Chemie and NRW Graduate School of Chemistry, Westfälische Wilhelms-Universität Münster , Corrensstraße 30, D-48149 Münster, Germany.
    Over the past two decades, self-assembly of supramolecular architectures has become a field of intensive research due to the wide range of applications for the resulting assemblies in various fields such as molecular encapsulation, supramolecular catalysis, drug delivery, metallopharmaceuticals, chemical and photochemical sensing, and light-emitting materials. For these purposes, a large number of coordination-driven metallacycles and metallacages featuring different sizes and shapes have been prepared and investigated. Almost all of these are Werner-type coordination compounds where metal centers are coordinated by nitrogen and/or oxygen donors of polydentate ligands. Read More

    Designing Pd-N-Heterocyclic Carbene Complexes for High Reactivity and Selectivity for Cross-Coupling Applications.
    Acc Chem Res 2017 Sep 24;50(9):2244-2253. Epub 2017 Aug 24.
    Centre for Catalysis Research and Innovation (CCRI), Department of Chemistry and Biomolecular Sciences, University of Ottawa , 75 Laurier Avenue East, Ottawa, ON K1N 6N5, Canada.
    Over the past decade, the use of Pd-NHC complexes in cross-coupling applications has blossomed, and reactions that were either not previously possible or possible only under very forcing conditions (e.g., > 100 °C, strong base) are now feasible under mild conditions (e. Read More

    Renewable Formate from C-H Bond Formation with CO2: Using Iron Carbonyl Clusters as Electrocatalysts.
    Acc Chem Res 2017 Sep 24;50(9):2362-2370. Epub 2017 Aug 24.
    Department of Chemistry, University of California , Davis, California 95616, United States.
    As a society, we are heavily dependent on nonrenewable petroleum-derived fuels and chemical feedstocks. Rapid depletion of these resources and the increasingly evident negative effects of excess atmospheric CO2 drive our efforts to discover ways of converting excess CO2 into energy dense chemical fuels through selective C-H bond formation and using renewable energy sources to supply electrons. In this way, a carbon-neutral fuel economy might be realized. Read More

    Miniprotein Design: Past, Present, and Prospects.
    Acc Chem Res 2017 Sep 23;50(9):2085-2092. Epub 2017 Aug 23.
    School of Chemistry, University of Bristol , Cantock's Close, Bristol BS8 1TS, U.K.
    The design and study of miniproteins, that is, polypeptide chains <40 amino acids in length that adopt defined and stable 3D structures, is resurgent. Miniproteins offer possibilities for reducing the complexity of larger proteins and so present new routes to studying sequence-to-structure and sequence-to-stability relationships in proteins generally. They also provide modules for protein design by pieces and, with this, prospects for building more-complex or even entirely new protein structures. Read More

    Nanosecond Dynamics at Protein Metal Sites: An Application of Perturbed Angular Correlation (PAC) of γ-Rays Spectroscopy.
    Acc Chem Res 2017 Sep 23;50(9):2225-2232. Epub 2017 Aug 23.
    Department of Chemistry, University of Copenhagen , Universitetsparken 5, DK-2100 København Ø, Denmark.
    Metalloproteins are essential to numerous reactions in nature, and constitute approximately one-third of all known proteins. Molecular dynamics of proteins has been elucidated with great success both by experimental and theoretical methods, revealing atomic level details of function involving the organic constituents on a broad spectrum of time scales. However, the characterization of dynamics at biomolecular metal sites on nanosecond time scales is scarce in the literature. Read More

    Nanometric Assembly of Functional Terpyridyl Complexes on Transparent and Conductive Oxide Substrates: Structure, Properties, and Applications.
    Acc Chem Res 2017 Sep 22;50(9):2128-2138. Epub 2017 Aug 22.
    Applied Physical Chemistry, Heidelberg University , 69120 Heidelberg, Germany.
    Over the last few decades, molecular assemblies on solid substrates have become increasingly popular, challenging the traditional systems and materials in terms of better control over molecular structure and function at the nanoscale. A variety of such assemblies with high complexity and adjustable properties was generated on the basis of organic, inorganic, organometallic, polymeric, and biomolecular building blocks. Particular versatile elements in this context are terpyridyls due to their wide design flexibility, ease of functionalization, and ability to coordinate to a broad variety of transition-metal ions without forming diastereoisomers, which facilitates tuning of their optical and electronic properties. Read More

    Novel Methods for the Chemical Synthesis of Insulin Superfamily Peptides and of Analogues Containing Disulfide Isosteres.
    Acc Chem Res 2017 Sep 22;50(9):2116-2127. Epub 2017 Aug 22.
    The Florey Institute of Neuroscience and Mental Health and School of Chemistry, University of Melbourne , Melbourne, Victoria 3010, Australia.
    The insulin superfamily of peptides is ubiquitous within vertebrates and invertebrates and is characterized by the presence of a set of three disulfide bonds in a unique disposition. With the exception of insulin-like growth factors I and II, which are single chain peptides, the remaining 8 members of the human insulin superfamily are two-chain peptides containing one intramolecular and two intermolecular disulfide bridges. These structural features have long made the chemical synthesis of the peptides a considerable challenge, in particular, including their correct disulfide bond pairing and formation. Read More

    Topological Polymer Chemistry Designing Complex Macromolecular Graph Constructions.
    Acc Chem Res 2017 Aug 22. Epub 2017 Aug 22.
    Department of Organic and Polymeric Materials, Tokyo Institute of Technology , Meguro-ku, Tokyo 152-8552, Japan.
    The precision design of topologically intriguing macromolecular architectures has continuously been an attractive challenge in polymer science and polymer materials engineering. A class of multicyclic polymer topologies, including three subclasses of spiro, bridged, and fused forms, are particularly unique not only from a topological geometry viewpoint but also from their biochemical relevance to programmed folding structures. In this Account, we describe recent progress in constructing this class of macromolecules, in particular by means of an electrostatic self-assembly and covalent fixation (ESA-CF) protocol, in which ion-paired polymer self-assemblies are employed as key intermediates. Read More

    Pyrite-Type Nanomaterials for Advanced Electrocatalysis.
    Acc Chem Res 2017 Sep 21;50(9):2194-2204. Epub 2017 Aug 21.
    Division of Nanomaterials & Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Collaborative Innovation Center of Suzhou Nano Science and Technology, Department of Chemistry, CAS Centre for Excellence in Nanoscience, Hefei Science Centre of CAS, University of Science and Technology of China , Hefei 230026, China.
    Since being proposed by John Bockris in 1970, hydrogen economy has emerged as a very promising alternative to the current hydrocarbon economy. Access to reliable and affordable hydrogen economy, however, requires cost-effective and highly efficient electrocatalytic materials that replace noble metals (e.g. Read More

    Mesoionic Pyrido[1,2-a]pyrimidinone Insecticides: From Discovery to Triflumezopyrim and Dicloromezotiaz.
    Acc Chem Res 2017 Sep 21;50(9):2381-2388. Epub 2017 Aug 21.
    DuPont Crop Protection, Stine-Haskell Research Center, 1090 Elkton Road, Newark, Delaware 19711, United States.
    One of the greatest global challenges is to feed the ever-increasing world population. The agrochemical tools growers currently utilize are also under continuous pressure, due to a number of factors that contribute to the loss of existing products. Mesoionic pyrido[1,2-a]pyrimidinones are an unusual yet very intriguing class of compounds. Read More

    Synthesis of Complex Glycolates by Enantioconvergent Addition Reactions.
    Acc Chem Res 2017 Sep 17;50(9):2284-2296. Epub 2017 Aug 17.
    Department of Chemistry, University of North Carolina at Chapel Hill , Chapel Hill, North Carolina 27599-3290 United States.
    The unique role that stereochemistry plays in molecular recognition events continues to provide a driving force for synthesizing organic compounds in enantioenriched form. The tendency of enantioenriched organic compounds to revert to an entropically favored racemic state in the presence of viable racemization pathways (e.g. Read More

    Cation-Anion Arrangement Patterns in Self-Assembled Pd2L4 and Pd4L8 Coordination Cages.
    Acc Chem Res 2017 Sep 17;50(9):2233-2243. Epub 2017 Aug 17.
    Department of Chemistry and Chemical Biology, TU Dortmund University , Otto-Hahn-Str. 6, 44227 Dortmund, Germany.
    Compounds featuring one-dimensional regular arrangements of stacked metal complexes and alternating [cation-anion]∞ sequences have raised considerable interest owing to their peculiar electronic and optical properties as well as guest inclusion capabilities. While traditional ways to realize these structural motifs rely on crystalline compounds, exclusively existing in the solid state, recent progress in the area of metal-mediated supramolecular self-assembly allows for the rational synthesis of structurally well-defined short stretches of stacked metal complexes and cation-anion arrangements. Therefore, metal cations, counteranions, and suitably designed organic bridges are allowed to self-assemble in solution. Read More

    Effect of Mineral Dissolution/Precipitation and CO2 Exsolution on CO2 transport in Geological Carbon Storage.
    Acc Chem Res 2017 Sep 16;50(9):2056-2066. Epub 2017 Aug 16.
    Key Laboratory for CO2 Utilization and Reduction Technology of Beijing, Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Department of Thermal Engineering, Tsinghua University , Beijing 100084, China.
    Geological carbon sequestration (GCS) in deep saline aquifers is an effective means for storing carbon dioxide to address global climate change. As the time after injection increases, the safety of storage increases as the CO2 transforms from a separate phase to CO2(aq) and HCO3(-) by dissolution and then to carbonates by mineral dissolution. However, subsequent depressurization could lead to dissolved CO2(aq) escaping from the formation water and creating a new separate phase which may reduce the GCS system safety. Read More

    Confined Water: Structure, Dynamics, and Thermodynamics.
    Acc Chem Res 2017 Sep 15;50(9):2139-2146. Epub 2017 Aug 15.
    Centre for Condensed Matter Theory, Department of Physics, Indian Institute of Science , Bangalore-560012, India.
    Understanding the properties of strongly confined water is important for a variety of applications such as fast flow and desalination devices, voltage generation, flow sensing, and nanofluidics. Confined water also plays an important role in many biological processes such as flow through ion channels. Water in the bulk exhibits many unusual properties that arise primarily from the presence of a network of hydrogen bonds. Read More

    Natural Seminal Amyloids as Targets for Development of Synthetic Inhibitors of HIV Transmission.
    Acc Chem Res 2017 Sep 15;50(9):2159-2166. Epub 2017 Aug 15.
    Department of Chemistry and Biochemistry, University of California, San Diego , 9500 Gilman Drive, La Jolla, California 92093-0358, United States.
    Amyloids refer to a class of protein or peptide aggregates that are heterogeneous in size, morphology, and composition, and are implicated to play a central role in many neurodegenerative and systemic diseases. The strong correlation between biological activity and extent of aggregation of amyloidogenic proteins and peptides has led to an explosion of research efforts to target these materials with synthetic molecules or engineered antibodies to try to attenuate their function in disease pathology. Although many of these efforts to attenuate amyloid function have shown great promise in laboratory settings, the vast majority of work has been focused on targeting amyloids associated with neurologic diseases, which has been met with significant additional challenges that preclude clinical evaluation. Read More

    Chelation-Controlled Additions to Chiral α- and β-Silyloxy, α-Halo, and β-Vinyl Carbonyl Compounds.
    Acc Chem Res 2017 Sep 15;50(9):2389-2400. Epub 2017 Aug 15.
    Institute of Advanced Synthesis, School of Chemistry and Molecular Engineering, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University , 30 South Puzhu Road, Nanjing 211816, P. R. China.
    The science and art of preventing and managing disease and prolonging life is dependent on advances in medicine, biology, and biochemistry. Many of these advances will involve interactions of small molecules with biological entities. As such, they will rely on the efficient synthesis of active compounds with very high stereochemical purity. Read More

    Discovery and Biosensing Applications of Diverse RNA-Cleaving DNAzymes.
    Acc Chem Res 2017 Sep 14;50(9):2273-2283. Epub 2017 Aug 14.
    Department of Biochemistry and Biomedical Sciences, Michael G. DeGroote Institute of Infectious Disease Research, McMaster University , 1280 Main Street West, Hamilton, Ontario L8S 4K1, Canada.
    DNA-based enzymes, or DNAzymes, are not known to exist in Nature but can be isolated from random-sequence DNA pools using test tube selection techniques. Since the report of the first DNAzyme in 1994, many catalytic DNA molecules for catalyzing wide-ranging chemical transformations have been isolated and studied. Our laboratory has a keen interest in searching for diverse DNAzymes capable of cleaving RNA-containing substrates, determining their sequence requirements and structural properties, and examining their potential as biosensors. Read More

    Pyrophosphate Recognition and Sensing in Water Using Bis[zinc(II)dipicolylamino]-Functionalized Peptides.
    Acc Chem Res 2017 Sep 14;50(9):2254-2263. Epub 2017 Aug 14.
    School of Chemistry, The University of Sydney , Sydney 2006, NSW, Australia.
    Phosphate oxoanions and phosphorylated biomolecules (such as nucleotides, lipids, and proteins) play key roles in a wide range of biological processes. The ability to selectively detect these ions in the presence of each other has numerous applications in biochemistry and biomedicine. However, receptors and sensors that can discriminate between polyphosphate species with high selectivity and in biologically relevant conditions are rare. Read More

    Deciphering the Fluorine Code-The Many Hats Fluorine Wears in a Protein Environment.
    Acc Chem Res 2017 Sep 12;50(9):2093-2103. Epub 2017 Aug 12.
    Institute of Chemistry and Biochemistry - Organic Chemistry, Freie Universität Berlin , Takustrasse 3, 14195 Berlin, Germany.
    Deciphering the fluorine code is how we describe not only the focus of this Account, but also the systematic approach to studying the impact of fluorine's incorporation on the properties of peptides and proteins used by our groups and others. The introduction of fluorine has been shown to impart favorable, but seldom predictable, properties to peptides and proteins, but up until about two decades ago the outcomes of fluorine modification of peptides and proteins were largely left to chance. Driven by the motivation to extend the application of the unique properties of the element fluorine from medicinal and agro chemistry to peptide and protein engineering we have established extensive research programs that enable the systematic investigation of effects that accompany the introduction of fluorine into this class of biopolymers. Read More

    The Tetraarylpyrrolo[3,2-b]pyrroles-From Serendipitous Discovery to Promising Heterocyclic Optoelectronic Materials.
    Acc Chem Res 2017 Sep 10;50(9):2334-2345. Epub 2017 Aug 10.
    Institute of Organic Chemistry, Polish Academy of Sciences , Kasprzaka 44-52, 01-224 Warsaw, Poland.
    Progress in organic optoelectronics requires compounds possessing a suitable combination of photophysical and electronic properties. Another key constraint encompasses the availability of feasible, and hopefully scalable, synthetic procedures for preparing the molecular scaffolds of interest. A multicomponent reaction of aromatic aldehydes, aromatic amines, and butane-2,3-dione that was discovered in 2013 gives straightforward access to previously unavailable 1,2,4,5-tetraarylpyrrolo[3,2-b]pyrroles. Read More

    Catalytic Enantioselective Carbonyl Allylation and Propargylation via Alcohol-Mediated Hydrogen Transfer: Merging the Chemistry of Grignard and Sabatier.
    Acc Chem Res 2017 Sep 9;50(9):2371-2380. Epub 2017 Aug 9.
    Department of Chemistry, University of Texas at Austin , Welch Hall (A5300), 105 East 24th Street, Austin, Texas 78712, United States.
    Merging the characteristics of transfer hydrogenation and carbonyl addition, we have developed a new class of catalytic enantioselective C-C bond formations. In these processes, hydrogen transfer between alcohols and π-unsaturated reactants generates carbonyl-organometal pairs that combine to deliver products of addition. On the basis of this mechanistic paradigm, lower alcohols are converted directly to higher alcohols in the absence of premetalated reagents or discrete alcohol-to-carbonyl redox reactions. Read More

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