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    Super-Resolution Structured Illumination Microscopy.
    Chem Rev 2017 Nov 10. Epub 2017 Nov 10.
    Biomolecular Photonics, Department of Physics, University of Bielefeld , Universitätsstraße 25, 33615 Bielefeld, Germany.
    Super-resolved structured illumination microscopy (SR-SIM) is among the most rapidly growing fluorescence microscopy techniques that can surpass the optical diffraction limit. The strength of SR-SIM is that it can be readily applied to samples prepared for conventional fluorescence microscopy, requiring no sophisticated sample preparation protocols. As an extension of wide-field fluorescence microscopy, it is inherently capable of multicolor imaging and optical sectioning and, with sufficiently fast implementations, permits live cell imaging. Read More

    Soft X-ray Absorption Spectroscopy of Liquids and Solutions.
    Chem Rev 2017 Nov 10. Epub 2017 Nov 10.
    Department of Chemistry, University of California , Berkeley, California 94720, United States.
    X-ray absorption spectroscopy (XAS) is an electronic absorption technique for which the initial state is a deeply buried core level. The photon energies corresponding to such transitions are governed primarily by the binding energies of the initial state. Because the binding energies of core electrons vary significantly among atomic species, this makes XAS an element-selective spectroscopy. Read More

    O2 Activation by Metal Surfaces: Implications for Bonding and Reactivity on Heterogeneous Catalysts.
    Chem Rev 2017 Nov 8. Epub 2017 Nov 8.
    Department of Chemistry and Chemical Biology, Harvard University , 12 Oxford St, Cambridge, Massachusetts 02138, United States.
    The activation of O2 on metal surfaces is a critical process for heterogeneous catalysis and materials oxidation. Fundamental studies of well-defined metal surfaces using a variety of techniques have given crucial insight into the mechanisms, energetics, and dynamics of O2 adsorption and dissociation. Here, trends in the activation of O2 on transition metal surfaces are discussed, and various O2 adsorption states are described in terms of both electronic structure and geometry. Read More

    Chemical Biology of H2S Signaling through Persulfidation.
    Chem Rev 2017 Nov 7. Epub 2017 Nov 7.
    Department of Biological Chemistry, University of Michigan Medical School , Ann Arbor, Michigan 48109-0600, United States.
    Signaling by H2S is proposed to occur via persulfidation, a posttranslational modification of cysteine residues (RSH) to persulfides (RSSH). Persulfidation provides a framework for understanding the physiological and pharmacological effects of H2S. Due to the inherent instability of persulfides, their chemistry is understudied. Read More

    Aerobic Oxidations of Light Alkanes over Solid Metal Oxide Catalysts.
    Chem Rev 2017 Nov 7. Epub 2017 Nov 7.
    Department of Chemistry, University of Wisconsin-Madison , 1101 University Avenue, Madison, Wisconsin 53706, United States.
    Heterogeneous metal oxide catalysts are widely studied for the aerobic oxidations of C1-C4 alkanes to form olefins and oxygenates. In this review, we outline the properties of supported metal oxides, mixed-metal oxides, and zeolites and detail their most common applications as catalysts for partial oxidations of light alkanes. By doing this we establish similarities between different classes of metal oxides and identify common themes in reaction mechanisms and research strategies for catalyst improvement. Read More

    Transition-Metal-Catalyzed Cross-Couplings through Carbene Migratory Insertion.
    Chem Rev 2017 Nov 1. Epub 2017 Nov 1.
    Beijing National Laboratory of Molecular Sciences (BNLMS), Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education, College of Chemistry, Peking University , Beijing 100871, China.
    Transition-metal-catalyzed cross-coupling reactions have been well-established as indispensable tools in modern organic synthesis. One of the major research goals in cross-coupling area is expanding the scope of the coupling partners. In the past decade, diazo compounds (or their precursors N-tosylhydrazones) have emerged as nucleophilic cross-coupling partners in C-C single bond or C═C double bond formations in transition-metal-catalyzed reactions. Read More

    Theory and Simulation of the Ultrafast Double-Bond Isomerization of Biological Chromophores.
    Chem Rev 2017 Oct 30. Epub 2017 Oct 30.
    Chemistry Department, Bowling Green State University , Overman Hall, Bowling Green, Ohio 43403, United States.
    Ultrafast processes in light-absorbing proteins have been implicated in the primary step in the light-to-energy conversion and the initialization of photoresponsive biological functions. Theory and computations have played an instrumental role in understanding the molecular mechanism of such processes, as they provide a molecular-level insight of structural and electronic changes at ultrafast time scales that often are very difficult or impossible to obtain from experiments alone. Among theoretical strategies, the application of hybrid quantum mechanics and molecular mechanics (QM/MM) models is an important approach that has reached an evident degree of maturity, resulting in several important contributions to the field. Read More

    Electrogenerated Cationic Reactive Intermediates: The Pool Method and Further Advances.
    Chem Rev 2017 Oct 27. Epub 2017 Oct 27.
    Department of Synthetic Chemistry and Biological Chemistry, Graduate School of Engineering, Kyoto University , Nishikyo-ku, Kyoto 615-8510, Japan.
    Electrochemistry serves as a powerful method for generating reactive intermediates, such as organic cations. In general, there are two ways to use reactive intermediates for chemical reactions: (1) generation in the presence of a reaction partner and (2) generation in the absence of a reaction partner with accumulation in solution as a "pool" followed by reaction with a subsequently added reaction partner. The former approach is more popular because reactive intermediates are usually short-lived transient species, but the latter method is more flexible and versatile. Read More

    Photochemistry and Photophysics in Silica-Based Materials: Ultrafast and Single Molecule Spectroscopy Observation.
    Chem Rev 2017 Oct 25. Epub 2017 Oct 25.
    Departamento de Química Física, Facultad de Ciencias Ambientales y Bioquímica, and INAMOL, Universidad de Castilla-La Mancha , Avenida Carlos III, S.N., 45071 Toledo, Spain.
    Silica-based materials (SBMs) are widely used in catalysis, photonics, and drug delivery. Their pores and cavities act as hosts of diverse guests ranging from classical dyes to drugs and quantum dots, allowing changes in the photochemical behavior of the confined guests. The heterogeneity of the guest populations as well as the confinement provided by these hosts affect the behavior of the formed hybrid materials. Read More

    Group 6 Dihapto-Coordinate Dearomatization Agents for Organic Synthesis.
    Chem Rev 2017 Oct 24. Epub 2017 Oct 24.
    Department of Chemistry, University of Virginia , Charlottesville, Virginia 22904, United States.
    This review covers publications ranging from 2005 to 2017 concerning the organic reactions of aromatic ligands η(2)-coordinated to tungsten or molybdenum and the use of these reactions in the synthesis of novel organic substances. An emphasis is placed on C-C bond-forming reactions using conventional building blocks of organic synthesis such as acetals, enolates, Michael acceptors, acylating reagents, and activated aromatics. Substrates activated by the metal include arenes, pyridines, pyrroles, pyrimidines, furans, and thiophenes. Read More

    Catalysis as an Enabling Science for Sustainable Polymers.
    Chem Rev 2017 Oct 19. Epub 2017 Oct 19.
    Department of Chemistry, Stanford University , Stanford, California 94305-5080, United States.
    The replacement of current petroleum-based plastics with sustainable alternatives is a crucial but formidable challenge for the modern society. Catalysis presents an enabling tool to facilitate the development of sustainable polymers. This review provides a system-level analysis of sustainable polymers and outlines key criteria with respect to the feedstocks the polymers are derived from, the manner in which the polymers are generated, and the end-of-use options. Read More

    Nanotechnology for Multimodal Synergistic Cancer Therapy.
    Chem Rev 2017 Oct 19. Epub 2017 Oct 19.
    Laboratory of Molecular Imaging and Nanomedicine, National Institute of Biomedical Imaging and Bioengineering, National Institutes of Health , Bethesda, Maryland 20892, United States.
    The complexity, diversity, and heterogeneity of tumors seriously undermine the therapeutic potential of treatment. Therefore, the current trend in clinical research has gradually shifted from a focus on monotherapy to combination therapy for enhanced treatment efficacy. More importantly, the cooperative enhancement interactions between several types of monotherapy contribute to the naissance of multimodal synergistic therapy, which results in remarkable superadditive (namely "1 + 1 > 2") effects, stronger than any single therapy or their theoretical combination. Read More

    Interactions of Native Cyclodextrins with Metal Ions and Inorganic Nanoparticles: Fertile Landscape for Chemistry and Materials Science.
    Chem Rev 2017 Oct 19. Epub 2017 Oct 19.
    Institute of Physical Chemistry, Polish Academy of Sciences , Kasprzaka 44/52, 01-224 Warsaw, Poland.
    Readily available cyclodextrins (CDs) with an inherent hydrophobic internal cavity and hydrophilic external surface are macrocyclic entities that display a combination of molecular recognition and complexation properties with vital implications for host-guest supramolecular chemistry. While the host-guest chemistry of CDs has been widely recognized and led to their exploitation in a variety of important functions over the last five decades, these naturally occurring macrocyclic systems have emerged only recently as promising macrocyclic molecules to fabricate environmentally benign functional nanomaterials. This review surveys the development in the field paying special attention to the synthesis and emerging uses of various unmodified CD-metal complexes and CD-inorganic nanoparticle systems and identifies possible future directions. Read More

    Structural Engineering in Plasmon Nanolasers.
    Chem Rev 2017 Oct 17. Epub 2017 Oct 17.
    Graduate Program in Applied Physics, ‡Department of Materials Science and Engineering, and §Department of Chemistry, Northwestern University , Evanston, Illinois 60208, United States.
    This review focuses on structural engineering of lasers from the macroscale to the nanoscale, with an emphasis on plasmon nanolasers. Conventional lasers based on Fabry-Pérot cavities are limited in device size. In contrast, plasmon nanolasers can overcome the diffraction limit of light and incorporate unique structural designs to engineer cavity geometries and optical band structure. Read More

    Use of Electrochemistry in the Synthesis of Heterocyclic Structures.
    Chem Rev 2017 Oct 17. Epub 2017 Oct 17.
    Beijing Key Laboratory of Environmental and Viral Oncology, College of Life Science & Bioengineering, Beijing University of Technology , Beijing 100124, China.
    The preparation and transformation of heterocyclic structures have always been of great interest in organic chemistry. Electrochemical technique provides a versatile and powerful approach to the assembly of various heterocyclic structures. In this review, we examine the advance in relation to the electrochemical construction of heterocyclic compounds published since 2000 via intra- and intermolecular cyclization reactions. Read More

    Multifunctional Cytochrome c: Learning New Tricks from an Old Dog.
    Chem Rev 2017 Nov 13;117(21):13382-13460. Epub 2017 Oct 13.
    Departamento de Química Inorgánica, Analítica y Química Física and INQUIMAE (CONICET-UBA), Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria , Pab. 2, piso 1, Buenos Aires C1428EHA, Argentina.
    Cytochrome c (cyt c) is a small soluble heme protein characterized by a relatively flexible structure, particularly in the ferric form, such that it is able to sample a broad conformational space. Depending on the specific conditions, interactions, and cellular localization, different conformations may be stabilized, which differ in structure, redox properties, binding affinities, and enzymatic activity. The primary function is electron shuttling in oxidative phosphorylation, and is exerted by the so-called native cyt c in the intermembrane mitochondrial space of healthy cells. Read More

    Noncoding RNA Surveillance: The Ends Justify the Means.
    Chem Rev 2017 Oct 12. Epub 2017 Oct 12.
    RNA Biology Laboratory, Center for Cancer Research, National Cancer Institute, National Institutes of Health , Frederick, Maryland 21702, United States.
    Numerous surveillance pathways sculpt eukaryotic transcriptomes by degrading unneeded, defective, and potentially harmful noncoding RNAs (ncRNAs). Because aberrant and excess ncRNAs are largely degraded by exoribonucleases, a key characteristic of these RNAs is an accessible, protein-free 5' or 3' end. Most exoribonucleases function with cofactors that recognize ncRNAs with accessible 5' or 3' ends and/or increase the availability of these ends. Read More

    Breaking the Kasha Rule for More Efficient Photochemistry.
    Chem Rev 2017 Nov 9;117(21):13353-13381. Epub 2017 Oct 9.
    Department of Chemistry, National Taiwan University , 1 Roosevelt Road Section 4, Taipei 106, Taiwan.
    This paper provides a systematic review and analysis of different phenomena that violate a basic principle, Kasha's rule, when applied to photochemical reactions. In contrast to the classical route of ultrafast transition to the lowest energy excited state and photochemical reaction starting therein, in some cases, these reactions proceed directly from high-energy excited states. Nowadays, this phenomenon can be observed for a number of major types of excited-state reactions: harvesting product via intersystem crossing; photoisomerizations; bond-breaking; and electron, proton, and energy transfers. Read More

    Functional and Biomimetic Materials for Engineering of the Three-Dimensional Cell Microenvironment.
    Chem Rev 2017 Oct 9;117(20):12764-12850. Epub 2017 Oct 9.
    MOE Key Laboratory of Biomedical Information Engineering, School of Life Science and Technology, Xi'an Jiaotong University , Xi'an 710049, People's Republic of China.
    The cell microenvironment has emerged as a key determinant of cell behavior and function in development, physiology, and pathophysiology. The extracellular matrix (ECM) within the cell microenvironment serves not only as a structural foundation for cells but also as a source of three-dimensional (3D) biochemical and biophysical cues that trigger and regulate cell behaviors. Increasing evidence suggests that the 3D character of the microenvironment is required for development of many critical cell responses observed in vivo, fueling a surge in the development of functional and biomimetic materials for engineering the 3D cell microenvironment. Read More

    Synthetic Organic Electrochemical Methods Since 2000: On the Verge of a Renaissance.
    Chem Rev 2017 Nov 9;117(21):13230-13319. Epub 2017 Oct 9.
    Department of Chemistry, The Scripps Research Institute , La Jolla, California 92037, United States.
    Electrochemistry represents one of the most intimate ways of interacting with molecules. This review discusses advances in synthetic organic electrochemistry since 2000. Enabling methods and synthetic applications are analyzed alongside innate advantages as well as future challenges of electroorganic chemistry. Read More

    Biomimetic Reactivity of Oxygen-Derived Manganese and Iron Porphyrinoid Complexes.
    Chem Rev 2017 Nov 9;117(21):13320-13352. Epub 2017 Oct 9.
    Department of Chemistry, The Johns Hopkins University , 3400 North Charles Street, Baltimore, Maryland 21218, United States.
    Heme proteins utilize the heme cofactor, an iron porphyrin, to perform a diverse range of reactions including dioxygen binding and transport, electron transfer, and oxidation/oxygenations. These reactions share several key metalloporphyrin intermediates, typically derived from dioxygen and its congeners such as hydrogen peroxide. These species are composed of metal-dioxygen, metal-superoxo, metal-peroxo, and metal-oxo adducts. Read More

    Nature-Inspired Structural Materials for Flexible Electronic Devices.
    Chem Rev 2017 Oct 9;117(20):12893-12941. Epub 2017 Oct 9.
    Innovative Centre for Flexible Devices (iFLEX), School of Materials Science and Engineering, Nanyang Technological University , 50 Nanyang Avenue, 639798, Singapore.
    Exciting advancements have been made in the field of flexible electronic devices in the last two decades and will certainly lead to a revolution in peoples' lives in the future. However, because of the poor sustainability of the active materials in complex stress environments, new requirements have been adopted for the construction of flexible devices. Thus, hierarchical architectures in natural materials, which have developed various environment-adapted structures and materials through natural selection, can serve as guides to solve the limitations of materials and engineering techniques. Read More

    Metal-Involving Synthesis and Reactions of Oximes.
    Chem Rev 2017 Nov 9;117(21):13039-13122. Epub 2017 Oct 9.
    Institute of Chemistry, Saint Petersburg State University , Universitetskaya Nab., 7/9, Saint Petersburg, Russian Federation.
    This review classifies and summarizes the past 10-15 years of advancements in the field of metal-involving (i.e., metal-mediated and metal-catalyzed) reactions of oximes. Read More

    Homogeneous Catalysis for Sustainable Hydrogen Storage in Formic Acid and Alcohols.
    Chem Rev 2017 Oct 6. Epub 2017 Oct 6.
    Institute of Chemical Sciences and Engineering , École Polytechnique Fédérale de Lausanne (EPFL), Avenue Forel 2, CH-1015 Lausanne, Switzerland.
    Hydrogen gas is a storable form of chemical energy that could complement intermittent renewable energy conversion. One of the main disadvantages of hydrogen gas arises from its low density, and therefore, efficient handling and storage methods are key factors that need to be addressed to realize a hydrogen-based economy. Storage systems based on liquids, in particular, formic acid and alcohols, are highly attractive hydrogen carriers as they can be made from CO2 or other renewable materials, they can be used in stationary power storage units such as hydrogen filling stations, and they can be used directly as transportation fuels. Read More

    Proton-Transfer-Reaction Mass Spectrometry: Applications in Atmospheric Sciences.
    Chem Rev 2017 Nov 4;117(21):13187-13229. Epub 2017 Oct 4.
    Cooperative Institute for Research in Environmental Sciences, University of Colorado at Boulder , Boulder, Colorado 80309, United States.
    Proton-transfer-reaction mass spectrometry (PTR-MS) has been widely used to study the emissions, distributions, and chemical evolution of volatile organic compounds (VOCs) in the atmosphere. The applications of PTR-MS have greatly promoted understanding of VOC sources and their roles in air-quality issues. In the past two decades, many new mass spectrometric techniques have been applied in PTR-MS instruments, and the performance of PTR-MS has improved significantly. Read More

    Ligand-Promoted Palladium-Catalyzed Aerobic Oxidation Reactions.
    Chem Rev 2017 Oct 4. Epub 2017 Oct 4.
    Department of Chemistry, University of Wisconsin-Madison , 1101 University Avenue, Madison, Wisconsin 53706, United States.
    Palladium-catalyzed aerobic oxidation reactions have been the focus of industrial application and extensive research efforts for nearly 60 years. A significant transition occurred in this field approximately 20 years ago, with the introduction of catalysts supported by ancillary ligands. The ligands play crucial roles in the reactions, including promotion of direct oxidation of palladium(0) by O2, bypassing the typical requirement for Cu salts or related redox cocatalysts to facilitate oxidation of the reduced Pd catalyst; facilitation of key bond-breaking and bond-forming steps during substrate oxidation; and modulation of chemo-, regio-, or stereoselectivity of a reaction. Read More

    Synchrotron X-ray Analytical Techniques for Studying Materials Electrochemistry in Rechargeable Batteries.
    Chem Rev 2017 Nov 29;117(21):13123-13186. Epub 2017 Sep 29.
    Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
    Rechargeable battery technologies have ignited major breakthroughs in contemporary society, including but not limited to revolutions in transportation, electronics, and grid energy storage. The remarkable development of rechargeable batteries is largely attributed to in-depth efforts to improve battery electrode and electrolyte materials. There are, however, still intimidating challenges of lower cost, longer cycle and calendar life, higher energy density, and better safety for large scale energy storage and vehicular applications. Read More

    Active Plasmonics: Principles, Structures, and Applications.
    Chem Rev 2017 Sep 29. Epub 2017 Sep 29.
    Department of Physics, The Chinese University of Hong Kong , Shatin, Hong Kong SAR 852, China.
    Active plasmonics is a burgeoning and challenging subfield of plasmonics. It exploits the active control of surface plasmon resonance. In this review, a first-ever in-depth description of the theoretical relationship between surface plasmon resonance and its affecting factors, which forms the basis for active plasmon control, will be presented. Read More

    Ecological Roles and Biological Activities of Specialized Metabolites from the Genus Nicotiana.
    Chem Rev 2017 Oct 29;117(19):12227-12280. Epub 2017 Sep 29.
    Department of Molecular Ecology, Max Planck Institute for Chemical Ecology , Jena 07745, Germany.
    Species of Nicotiana grow naturally in different parts of the world and have long been used both medicinally and recreationally by human societies. More recently in our history, Nicotiana tabacum has attracted interest as one of the most economically important industrial crops. Nicotiana species are frequently investigated for their bioactive natural products, and the ecological role of their specialized metabolites in responses to abiotic stress or biotic stress factors like pathogens and herbivores. Read More

    Natural Products as Platforms To Overcome Antibiotic Resistance.
    Chem Rev 2017 Oct 27;117(19):12415-12474. Epub 2017 Sep 27.
    Department of Chemistry, Emory University , 1515 Dickey Drive, Atlanta, Georgia 30322, United States.
    Natural products have served as powerful therapeutics against pathogenic bacteria since the golden age of antibiotics of the mid-20th century. However, the increasing frequency of antibiotic-resistant infections clearly demonstrates that new antibiotics are critical for modern medicine. Because combinatorial approaches have not yielded effective drugs, we propose that the development of new antibiotics around proven natural scaffolds is the best short-term solution to the rising crisis of antibiotic resistance. Read More

    (31)P NMR Chemical Shifts of Phosphorus Probes as Reliable and Practical Acidity Scales for Solid and Liquid Catalysts.
    Chem Rev 2017 Oct 27;117(19):12475-12531. Epub 2017 Sep 27.
    State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Key Laboratory of Magnetic Resonance in Biological Systems, Wuhan Institute of Physics and Mathematics, the Chinese Academy of Sciences , Wuhan 430071, China.
    Acid-base catalytic reaction, either in heterogeneous or homogeneous systems, is one of the most important chemical reactions that has provoked a wide variety of industrial catalytic processes for production of chemicals and petrochemicals over the past few decades. In view of the fact that the catalytic performances (e.g. Read More

    Dehydrogenation of Alkanes and Aliphatic Groups by Pincer-Ligated Metal Complexes.
    Chem Rev 2017 Oct 27;117(19):12357-12384. Epub 2017 Sep 27.
    Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey , New Brunswick, New Jersey 08903, United States.
    The alkyl group is the most common component of organic molecules and the most difficult to selectively functionalize. The development of catalysts for dehydrogenation of alkyl groups to give the corresponding olefins could open almost unlimited avenues to functionalization. Homogeneous systems, or more generally systems based on molecular (including solid-supported) catalysts, probably offer the greatest potential for regio- and chemoselective dehydrogenation of alkyl groups and alkanes. Read More

    How Water's Properties Are Encoded in Its Molecular Structure and Energies.
    Chem Rev 2017 Oct 26;117(19):12385-12414. Epub 2017 Sep 26.
    Faculty of Chemistry and Chemical Technology, University of Ljubljana , Večna pot 113, SI-1000 Ljubljana, Slovenia.
    How are water's material properties encoded within the structure of the water molecule? This is pertinent to understanding Earth's living systems, its materials, its geochemistry and geophysics, and a broad spectrum of its industrial chemistry. Water has distinctive liquid and solid properties: It is highly cohesive. It has volumetric anomalies-water's solid (ice) floats on its liquid; pressure can melt the solid rather than freezing the liquid; heating can shrink the liquid. Read More

    Simulating Coherent Multidimensional Spectroscopy of Nonadiabatic Molecular Processes: From the Infrared to the X-ray Regime.
    Chem Rev 2017 Oct 26;117(19):12165-12226. Epub 2017 Sep 26.
    Department of Chemistry and Department of Physics and Astronomy, University of California , Irvine, California 92697-2025, United States.
    Crossings of electronic potential energy surfaces in nuclear configuration space, known as conical intersections, determine the rates and outcomes of a large class of photochemical molecular processes. Much theoretical progress has been made in computing strongly coupled electronic and nuclear motions at different levels, but how to incorporate them in different spectroscopic signals and the approximations involved are less established. This will be the focus of the present review. Read More

    Bio-Optics and Bio-Inspired Optical Materials.
    Chem Rev 2017 Oct 22;117(20):12705-12763. Epub 2017 Sep 22.
    Department of Mechanical Engineering and Materials Science and Institute of Materials Science and Engineering, Washington University in St. Louis , St. Louis, Missouri 63130, United States.
    Through the use of the limited materials palette, optimally designed micro- and nanostructures, and tightly regulated processes, nature demonstrates exquisite control of light-matter interactions at various length scales. In fact, control of light-matter interactions is an important element in the evolutionary arms race and has led to highly engineered optical materials and systems. In this review, we present a detailed summary of various optical effects found in nature with a particular emphasis on the materials and optical design aspects responsible for their optical functionality. Read More

    O2 Reduction in Enzymatic Biofuel Cells.
    Chem Rev 2017 Sep 20. Epub 2017 Sep 20.
    Aix Marseille Univ., CNRS, BIP , 31, chemin Aiguier, 13402 Marseille, France.
    Catalytic four-electron reduction of O2 to water is one of the most extensively studied electrochemical reactions due to O2 exceptional availability and high O2/H2O redox potential, which may in particular allow highly energetic reactions in fuel cells. To circumvent the use of expensive and inefficient Pt catalysts, multicopper oxidases (MCOs) have been envisioned because they provide efficient O2 reduction with almost no overpotential. MCOs have been used to elaborate enzymatic biofuel cells (EBFCs), a subclass of fuel cells in which enzymes replace the conventional catalysts. Read More

    What Can Be Learned from Nuclear Resonance Vibrational Spectroscopy: Vibrational Dynamics and Hemes.
    Chem Rev 2017 Oct 18;117(19):12532-12563. Epub 2017 Sep 18.
    Department of Physics and Center for Interdisciplinary Research on Complex Systems, Northeastern University , 120 Forsyth Street, Boston, Massachusetts 02115, United States.
    Nuclear resonance vibrational spectroscopy (NRVS; also known as nuclear inelastic scattering, NIS) is a synchrotron-based method that reveals the full spectrum of vibrational dynamics for Mössbauer nuclei. Another major advantage, in addition to its completeness (no arbitrary optical selection rules), is the unique selectivity of NRVS. The basics of this recently developed technique are first introduced with descriptions of the experimental requirements and data analysis including the details of mode assignments. Read More

    Flow Electrolysis Cells for the Synthetic Organic Chemistry Laboratory.
    Chem Rev 2017 Sep 18. Epub 2017 Sep 18.
    Chemistry, University of Southampton , Southampton SO17 1BJ, U.K.
    Electrosynthesis has much to offer to the synthetic organic chemist. But in order to be widely accepted as a routine procedure in an organic synthesis laboratory, electrosynthesis needs to be presented in a much more user-friendly way. The literature is largely based on electrolysis in a glass beaker or H-cells that often give poor performance for synthesis with a very slow rate of conversion and, often, low selectivity and reproducibility. Read More

    Recent Advances in the Chemical Synthesis of C-Glycosides.
    Chem Rev 2017 Oct 15;117(19):12281-12356. Epub 2017 Sep 15.
    State Key Laboratory of Bio-organic and Natural Products Chemistry, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences , 345 Lingling Road, Shanghai 200032, China.
    Advances in the chemical synthesis of C-pyranosides/furanosides are summarized, covering the literature from 2000 to 2016. The majority of the methods take advantage of the construction of the glycosidic C-C bond. These C-glycosylation methods are categorized herein in terms of the glycosyl donor precursors, which are commonly used in O-glycoside synthesis and are easily accessible to nonspecialists. Read More

    Acyclic Quaternary Carbon Stereocenters via Enantioselective Transition Metal Catalysis.
    Chem Rev 2017 Oct 14;117(19):12564-12580. Epub 2017 Sep 14.
    Department of Chemistry, Welch Hall (A5300), University of Texas at Austin , 105 East 24th Street, Austin, Texas 78712, United States.
    Whereas numerous asymmetric methods for formation of quaternary carbon stereocenters in cyclic systems have been documented, the construction of acyclic quaternary carbon stereocenters with control of absolute stereochemistry remains a formidable challenge. This Review summarizes enantioselective methods for the construction of acyclic quaternary carbon stereocenters from achiral or chiral racemic reactants via transition metal catalysis. Read More

    Concepts and Methods of Solid-State NMR Spectroscopy Applied to Biomembranes.
    Chem Rev 2017 Oct 14;117(19):12087-12132. Epub 2017 Sep 14.
    Department of Chemistry & Biochemistry and ‡Department of Physics, University of Arizona , Tucson, Arizona 85721, United States.
    Concepts of solid-state NMR spectroscopy and applications to fluid membranes are reviewed in this paper. Membrane lipids with (2)H-labeled acyl chains or polar head groups are studied using (2)H NMR to yield knowledge of their atomistic structures in relation to equilibrium properties. This review demonstrates the principles and applications of solid-state NMR by unifying dipolar and quadrupolar interactions and highlights the unique features offered by solid-state (2)H NMR with experimental illustrations. Read More

    Synthesis, Assembly, and Applications of Hybrid Nanostructures for Biosensing.
    Chem Rev 2017 Oct 13;117(20):12942-13038. Epub 2017 Sep 13.
    School of Materials Science and Engineering, Georgia Institute of Technology , Atlanta, Georgia 30332-0245, United States.
    The robust, sensitive, and selective detection of targeted biomolecules in their native environment by prospective nanostructures holds much promise for real-time, accurate, and high throughput biosensing. However, in order to be competitive, current biosensor nanotechnologies need significant improvements, especially in specificity, integration, throughput rate, and long-term stability in complex bioenvironments. Advancing biosensing nanotechnologies in chemically "noisy" bioenvironments require careful engineering of nanoscale components that are highly sensitive, biorecognition ligands that are capable of exquisite selective binding, and seamless integration at a level current devices have yet to achieve. Read More

    Ligand-Targeted Drug Delivery.
    Chem Rev 2017 Oct 12;117(19):12133-12164. Epub 2017 Sep 12.
    Purdue Institute for Drug Discovery, Purdue University , West Lafayette, Indiana 47907, United States.
    Safety and efficacy constitute the major criteria governing regulatory approval of any new drug. The best method to maximize safety and efficacy is to deliver a proven therapeutic agent with a targeting ligand that exhibits little affinity for healthy cells but high affinity for pathologic cells. The probability of regulatory approval can conceivably be further enhanced by exploiting the same targeting ligand, conjugated to an imaging agent, to select patients whose diseased tissues display sufficient targeted receptors for therapeutic efficacy. Read More

    Applications of Flow Microreactors in Electrosynthetic Processes.
    Chem Rev 2017 Sep 8. Epub 2017 Sep 8.
    Department of Chemistry and Chemical Engineering, Faculty of Engineering, Yamagata University , Jonan 4-3-16, Yonezawa, Yamagata 992-8510, Japan.
    The fundamental advantages and potential benefits of flow microreactor technology include extremely large surface-to-volume ratios, precise control over temperature and residence time, extremely fast molecular diffusion, and increased safety during reactive processes. These advantages and benefits can be applied to a wide range of electrosynthetic techniques, and so the integration of flow microreactors with electrosynthesis has received significant research interest from both academia and industry. This review presents an up-to-date overview of electrosynthetic processes in continuous-flow microreactors. Read More

    Role of Biocatalysis in Sustainable Chemistry.
    Chem Rev 2017 Sep 6. Epub 2017 Sep 6.
    Department of Chemical and Biochemical Engineering, Technical University of Denmark , 2800 Lyngby, Denmark.
    Based on the principles and metrics of green chemistry and sustainable development, biocatalysis is both a green and sustainable technology. This is largely a result of the spectacular advances in molecular biology and biotechnology achieved in the past two decades. Protein engineering has enabled the optimization of existing enzymes and the invention of entirely new biocatalytic reactions that were previously unknown in Nature. Read More

    Recent Progress in Heterogeneous Asymmetric Hydrogenation of C═O and C═C Bonds on Supported Noble Metal Catalysts.
    Chem Rev 2017 Sep 5;117(17):11522-11569. Epub 2017 Sep 5.
    Institute for Chemical and Biochemical Engineering, Department of Chemistry and Applied Biosciences, ETH-Zurich, Hönggerberg, HCI , Vladimir Prelog Weg 1, CH-8093 Zurich, Switzerland.
    The ease of separation, simple regeneration, and the usually high stability of solid catalysts facilitating continuous production processes have stimulated the development of heterogeneous asymmetric hydrogenation catalysis. The simplest and so far most promising strategy to induce enantioselectivity to solid metal catalysts is their modification by chiral organic compounds, as most prominently represented by the cinchona-modified Pt and Pd catalysts for the asymmetric hydrogenation of activated C═O and C═C bonds. In this Review, we provide a systematic account of the research accomplished in the past decade on noble metal-based heterogeneous asymmetric hydrogenation of prochiral C═O and C═C bonds, including all important facets of these catalytic systems. Read More

    Form Follows Function: Nanoparticle Shape and Its Implications for Nanomedicine.
    Chem Rev 2017 Sep 1;117(17):11476-11521. Epub 2017 Sep 1.
    Bio21 Institute & School of Chemistry, University of Melbourne , Parkville 3010, Australia.
    This review is a comprehensive description of the past decade of research into understanding how the geometry and size of nanoparticles affect their interaction with biological systems: from single cells to whole organisms. Recently, there has been a great deal of effort to use both the shape and the size of nanoparticles to target specific cellular uptake mechanisms, biodistribution patterns, and pharmacokinetics. While the successes of spherical lipid-based nanoparticles have heralded marked changes in chemotherapy worldwide, the history of asbestos-induced lung disease casts a long shadow over fibrous materials to date. Read More

    Organometallic Neptunium Chemistry.
    Chem Rev 2017 Sep 30;117(17):11460-11475. Epub 2017 Aug 30.
    European Commission, DG Joint Research Centre, Directorate G-Nuclear Safety and Security, Advanced Nuclear Knowledge-G.I.5, Postfach 2340, D-76125, Karlsruhe, Germany.
    Fifty years have passed since the foundation of organometallic neptunium chemistry, and yet only a handful of complexes have been reported, and even fewer have been fully characterized. Yet, increasingly, combined synthetic/spectroscopic/computational studies are demonstrating how covalently bonding, soft, carbocyclic organometallic ligands provide an excellent platform for advancing the fundamental understanding of the differences in orbital contributions and covalency in f-block metal-ligand bonding. Understanding the subtleties is the key to the safe handling and separations of the highly radioactive nuclei. Read More

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