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    High- k Gate Dielectrics for Emerging Flexible and Stretchable Electronics.
    Chem Rev 2018 May 22. Epub 2018 May 22.
    Department of Chemistry and the Materials Research Center , Northwestern University , 2145 Sheridan Road , Evanston , Illinois 60208 , United States.
    Recent advances in flexible and stretchable electronics (FSE), a technology diverging from the conventional rigid silicon technology, have stimulated fundamental scientific and technological research efforts. FSE aims at enabling disruptive applications such as flexible displays, wearable sensors, printed RFID tags on packaging, electronics on skin/organs, and Internet-of-things as well as possibly reducing the cost of electronic device fabrication. Thus, the key materials components of electronics, the semiconductor, the dielectric, and the conductor as well as the passive (substrate, planarization, passivation, and encapsulation layers) must exhibit electrical performance and mechanical properties compatible with FSE components and products. Read More

    Artificial Plasmonic Molecules and Their Interaction with Real Molecules.
    Chem Rev 2018 May 21. Epub 2018 May 21.
    Schulich Faculty of Chemistry , Technion-Israel Institute of Technology , Haifa 3200008 , Israel.
    Plasmonic molecules are small assemblies of nanosized metal particles. Interactions between the particles modify their optical properties and make them attractive for multiple applications in spectroscopy and sensing. In this review, we focus on basic properties rather than on applications. Read More

    Multiple Architectures and Mechanisms of Latency in Metallopeptidase Zymogens.
    Chem Rev 2018 May 18. Epub 2018 May 18.
    Proteolysis Laboratory, Structural Biology Unit ("María-de-Maeztu" Unit of Excellence) , Molecular Biology Institute of Barcelona, Consejo Superior de Investigaciones Científicas , Barcelona Science Park, c/Baldiri Reixac 15-21 , 08028 Barcelona , Catalonia , Spain.
    Metallopeptidases cleave polypeptides bound in the active-site cleft of catalytic domains through a general base/acid mechanism. This involves a solvent molecule bound to a catalytic zinc and general regulation of the mechanism through zymogen-based latency. Sixty reported structures from 11 metallopeptidase families reveal that prosegments, mostly N-terminal of the catalytic domain, block the cleft regardless of their size. Read More

    Recent Advances and Perspectives on Nonadiabatic Mixed Quantum-Classical Dynamics.
    Chem Rev 2018 May 16. Epub 2018 May 16.
    Aix Marseille Univ, CNRS, ICR , Marseille , France.
    Nonadiabatic mixed quantum-classical (NA-MQC) dynamics methods form a class of computational theoretical approaches in quantum chemistry tailored to investigate the time evolution of nonadiabatic phenomena in molecules and supramolecular assemblies. NA-MQC is characterized by a partition of the molecular system into two subsystems: one to be treated quantum mechanically (usually but not restricted to electrons) and another to be dealt with classically (nuclei). The two subsystems are connected through nonadiabatic couplings terms to enforce self-consistency. Read More

    Small-Pore Zeolites: Synthesis and Catalysis.
    Chem Rev 2018 May 10. Epub 2018 May 10.
    Chemical Engineering , California Institute of Technology , Mail Code 210-41, Pasadena , California 91125 , United States.
    In the past decade or so, small-pore zeolites have received greater attention than large- and medium-pore molecular sieves that have historically dominated the literature. This is primarily due to the commercialization of two major catalytic processes, NOx exhaust removal and methanol conversion to light olefins, that take advantage of the properties of these materials with smaller apertures. Small-pore zeolites possess pores that are constructed of eight tetrahedral atoms (Si and Al), each time linked by a shared oxygen These eight-member ring pores (8MR) provide small molecules access to the intracrystalline void space, e. Read More

    Gas Permeation Properties, Physical Aging, and Its Mitigation in High Free Volume Glassy Polymers.
    Chem Rev 2018 May 8. Epub 2018 May 8.
    Centre for Advanced Separations Engineering and Department of Chemical Engineering , University of Bath , Claverton Down , Bath BA2 7AY , U.K.
    Hundreds of polymers have been evaluated as membrane materials for gas separations, but fewer than 10 have made it into current commercial applications, mainly due to the effects of physical aging and plasticization. Efforts to overcome these two problems are a significant focus in gas separation membrane research, in conjunction with improving membrane separation performance to surpass the Robeson upper bounds of selectivity versus permeability for commercially important gas pairs. While there has been extensive research, ranging from manipulating the chemistry of existing polymers (e. Read More

    First-Row Transition-Metal-Catalyzed Carbonylative Transformations of Carbon Electrophiles.
    Chem Rev 2018 May 3. Epub 2018 May 3.
    Department of Chemistry , Zhejiang Sci-Tech University , Hangzhou , Zhejiang 310018 , People's Republic of China.
    The main contributions in the field of first-row transition-metal-catalyzed (base-metal-catalyzed) carbonylative transformations have been summarized and discussed. The contents have been divided according to the electrophiles applied, followed by the different types of nucleophiles. Their reaction mechanisms and applications have been emphatically discussed. Read More

    Tetramethylpiperidine N-Oxyl (TEMPO), Phthalimide N-Oxyl (PINO), and Related N-Oxyl Species: Electrochemical Properties and Their Use in Electrocatalytic Reactions.
    Chem Rev 2018 May 30;118(9):4834-4885. Epub 2018 Apr 30.
    Department of Chemistry , University of Wisconsin-Madison , 1101 University Avenue , Madison , Wisconsin 53706 , United States.
    N-Oxyl compounds represent a diverse group of reagents that find widespread use as catalysts for the selective oxidation of organic molecules in both laboratory and industrial applications. While turnover of N-oxyl catalysts in oxidation reactions may be accomplished with a variety of stoichiometric oxidants, N-oxyl reagents have also been extensively used as catalysts under electrochemical conditions in the absence of chemical oxidants. Several classes of N-oxyl compounds undergo facile redox reactions at electrode surfaces, enabling them to mediate a wide range of electrosynthetic reactions. Read More

    Cooperativity Principles in Self-Assembled Nanomedicine.
    Chem Rev 2018 Apr 25. Epub 2018 Apr 25.
    Department of Pharmacology, Simmons Comprehensive Cancer Center , UT Southwestern Medical Center , 5323 Harry Hines Boulevard , Dallas , Texas 75390 , United States.
    Nanomedicine is a discipline that applies nanoscience and nanotechnology principles to the prevention, diagnosis, and treatment of human diseases. Self-assembly of molecular components is becoming a common strategy in the design and syntheses of nanomaterials for biomedical applications. In both natural and synthetic self-assembled nanostructures, molecular cooperativity is emerging as an important hallmark. Read More

    Role of Molecular Modeling in the Development of CO-Reactive Ionic Liquids.
    Chem Rev 2018 May 24;118(10):5242-5260. Epub 2018 Apr 24.
    Department of Chemical and Biomolecular Engineering , The University of Notre Dame , Notre Dame , Indiana 46556 , United States.
    Ionic liquids (ILs) have gained considerable attention in recent years as CO-reactive solvents that could be used to improve the economic efficiency of industrial-scale CO separations. Researchers have demonstrated that IL physical and chemical properties can be optimized for a given application through chemical functionalization of both cations and anions. The tunability of ILs presents both a great potential and a significant challenge due to the complex chemistries and the many ways in which ILs can be made to react with CO. Read More

    Stereodivergent Catalysis.
    Chem Rev 2018 May 20;118(10):5080-5200. Epub 2018 Apr 20.
    Departamento de Química Orgánica and Centro de Innovación en Química Avanzada (ORFEO-CINQA) , Universidad de Alicante , Apdo. 99 , E-03080 Alicante , Spain.
    This review covers diastereo- and enantiodivergent catalyzed reactions in acyclic and cyclic systems using metal complexes or organocatalysts. Among them, nucleophilic addition to carbon-carbon and carbon-nitrogen double bonds, α-functionalization of carbonyl compounds, allylic substitutions, and ring opening of oxiranes and aziridines are considered. The diastereodivergent synthesis of alkenes from alkynes is also included. Read More

    Mimicking Natural Photosynthesis: Solar to Renewable H Fuel Synthesis by Z-Scheme Water Splitting Systems.
    Chem Rev 2018 May 20;118(10):5201-5241. Epub 2018 Apr 20.
    Department of Chemical Engineering , University College London , Torrington Place , London WC1E 7JE , U.K.
    Visible light-driven water splitting using cheap and robust photocatalysts is one of the most exciting ways to produce clean and renewable energy for future generations. Cutting edge research within the field focuses on so-called "Z-scheme" systems, which are inspired by the photosystem II-photosystem I (PSII/PSI) coupling from natural photosynthesis. A Z-scheme system comprises two photocatalysts and generates two sets of charge carriers, splitting water into its constituent parts, hydrogen and oxygen, at separate locations. Read More

    Parasites under the Spotlight: Applications of Vibrational Spectroscopy to Malaria Research.
    Chem Rev 2018 Apr 20. Epub 2018 Apr 20.
    Centre for Biospectroscopy, School of Chemistry , Monash University , Clayton , Victoria 3800 , Australia.
    New technologies to diagnose malaria at high sensitivity and specificity are urgently needed in the developing world where the disease continues to pose a huge burden on society. Infrared and Raman spectroscopy-based diagnostic methods have a number of advantages compared with other diagnostic tests currently on the market. These include high sensitivity and specificity for detecting low levels of parasitemia along with ease of use and portability. Read More

    Expanded Theory of H- and J-Molecular Aggregates: The Effects of Vibronic Coupling and Intermolecular Charge Transfer.
    Chem Rev 2018 Apr 17. Epub 2018 Apr 17.
    Department of Chemistry , Temple University , Philadelphia , Pennsylvania 19122 , United States.
    The electronic excited states of molecular aggregates and their photophysical signatures have long fascinated spectroscopists and theoreticians alike since the advent of Frenkel exciton theory almost 90 years ago. The influence of molecular packing on basic optical probes like absorption and photoluminescence was originally worked out by Kasha for aggregates dominated by Coulombic intermolecular interactions, eventually leading to the classification of J- and H-aggregates. This review outlines advances made in understanding the relationship between aggregate structure and photophysics when vibronic coupling and intermolecular charge transfer are incorporated. Read More

    Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles.
    Chem Rev 2018 May 16;118(10):4981-5079. Epub 2018 Apr 16.
    Instituto de Tecnología Química , Universitat Politécnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC) , Avenida de los Naranjos s/n , 46022 Valencia , España.
    Metal species with different size (single atoms, nanoclusters, and nanoparticles) show different catalytic behavior for various heterogeneous catalytic reactions. It has been shown in the literature that many factors including the particle size, shape, chemical composition, metal-support interaction, and metal-reactant/solvent interaction can have significant influences on the catalytic properties of metal catalysts. The recent developments of well-controlled synthesis methodologies and advanced characterization tools allow one to correlate the relationships at the molecular level. Read More

    Biochemistry and Molecular Biology of Flaviviruses.
    Chem Rev 2018 Apr 13;118(8):4448-4482. Epub 2018 Apr 13.
    Department of Biochemistry and Molecular Biology , University of Texas Medical Branch , Galveston , Texas 77555 , United States.
    Flaviviruses, such as dengue, Japanese encephalitis, tick-borne encephalitis, West Nile, yellow fever, and Zika viruses, are critically important human pathogens that sicken a staggeringly high number of humans every year. Most of these pathogens are transmitted by mosquitos, and not surprisingly, as the earth warms and human populations grow and move, their geographic reach is increasing. Flaviviruses are simple RNA-protein machines that carry out protein synthesis, genome replication, and virion packaging in close association with cellular lipid membranes. Read More

    Theoretical Modeling of Singlet Fission.
    Chem Rev 2018 Apr 12. Epub 2018 Apr 12.
    Kimika Fakultatea , Euskal Herriko Unibertsitatea (UPV/EHU) and Donostia International Physics Center (DIPC) , P.K. 1072, 20080 Donostia , Euskadi, Spain.
    Singlet fission is a photophysical reaction in which a singlet excited electronic state splits into two spin-triplet states. Singlet fission was discovered more than 50 years ago, but the interest in this process has gained a lot of momentum in the past decade due to its potential as a way to boost solar cell efficiencies. This review presents and discusses the most recent advances with respect to the theoretical and computational studies on the singlet fission phenomenon. Read More

    Surface-Enhanced Raman Spectroscopy for Bioanalysis: Reliability and Challenges.
    Chem Rev 2018 May 11;118(10):4946-4980. Epub 2018 Apr 11.
    State Key Laboratory of Physical Chemistry of Solid Surfaces, MOE Key Laboratory of Spectrochemical Analysis and Instrumentation, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering , Xiamen University , Xiamen 361005 , China.
    Surface-enhanced Raman spectroscopy (SERS) inherits the rich chemical fingerprint information on Raman spectroscopy and gains sensitivity by plasmon-enhanced excitation and scattering. In particular, most Raman peaks have a narrow width suitable for multiplex analysis, and the measurements can be conveniently made under ambient and aqueous conditions. These merits make SERS a very promising technique for studying complex biological systems, and SERS has attracted increasing interest in biorelated analysis. Read More

    Conducting Polymers in the Fields of Energy, Environmental Remediation, and Chemical-Chiral Sensors.
    Chem Rev 2018 May 9;118(9):4731-4816. Epub 2018 Apr 9.
    Centro Conjunto de Investigación en Química Sustentable , UAEM-UNAM , Km 14.5 Carretera Toluca-Ixtlahuaca , Toluca 50200 , Estado de México Mexico.
    Conducting polymers (CPs), thanks to their unique properties, structures made on-demand, new composite mixtures, and possibility of deposit on a surface by chemical, physical, or electrochemical methodologies, have shown in the last years a renaissance and have been widely used in important fields of chemistry and materials science. Due to the extent of the literature on CPs, this review, after a concise introduction about the interrelationship between electrochemistry and conducting polymers, is focused exclusively on the following applications: energy (energy storage devices and solar cells), use in environmental remediation (anion and cation trapping, electrocatalytic reduction/oxidation of pollutants on CP based electrodes, and adsorption of pollutants) and finally electroanalysis as chemical sensors in solution, gas phase, and chiral molecules. This review is expected to be comprehensive, authoritative, and useful to the chemical community interested in CPs and their applications. Read More

    Quantum Interference, Graphs, Walks, and Polynomials.
    Chem Rev 2018 May 9;118(10):4887-4911. Epub 2018 Apr 9.
    Department of Chemistry and Chemical Biology , Cornell University , Ithaca , New York 14853-1301 , United States.
    In this paper, we explore quantum interference (QI) in molecular conductance from the point of view of graph theory and walks on lattices. By virtue of the Cayley-Hamilton theorem for characteristic polynomials and the Coulson-Rushbrooke pairing theorem for alternant hydrocarbons, it is possible to derive a finite series expansion of the Green's function for electron transmission in terms of the odd powers of the vertex adjacency matrix or Hückel matrix. This means that only odd-length walks on a molecular graph contribute to the conductivity through a molecule. Read More

    Homogeneous Oxygenase Catalysis.
    Chem Rev 2018 May 9;118(10):4912-4945. Epub 2018 Apr 9.
    State Key Laboratory of Natural and Biomimetic Drugs, School of Pharmaceutical Sciences , Peking University , Xue Yuan Road 38 , Beijing 100191 , China.
    Oxygenases-catalyzed reductive activation of molecular oxygen and incorporation of O atoms into an organic molecule is undoubtedly one of the most attractive research areas. Typically, these oxygenation reactions proceed with high selectivity and reactivity, which is seldom found in its "biomimetic" chemocatalytic counterparts. Furthermore, enzymatic oxygenation can avoid undesired overoxidation, which is frequently observed in (industrial) chemical transformation. Read More

    Modern Approaches for Asymmetric Construction of Carbon-Fluorine Quaternary Stereogenic Centers: Synthetic Challenges and Pharmaceutical Needs.
    Chem Rev 2018 Apr 2;118(7):3887-3964. Epub 2018 Apr 2.
    Department of Chemistry , University of California , Berkeley , California 94720 , United States.
    New methods for preparation of tailor-made fluorine-containing compounds are in extremely high demand in nearly every sector of chemical industry. The asymmetric construction of quaternary C-F stereogenic centers is the most synthetically challenging and, consequently, the least developed area of research. As a reflection of this apparent methodological deficit, pharmaceutical drugs featuring C-F stereogenic centers constitute less than 1% of all fluorine-containing medicines currently on the market or in clinical development. Read More

    Electronic Properties of N-Heterocyclic Carbenes and Their Experimental Determination.
    Chem Rev 2018 Mar 30. Epub 2018 Mar 30.
    Department of Chemistry, Faculty of Science , National University of Singapore , 3 Science Drive 3 , Singapore 117543 , Republic of Singapore.
    N-Heterocyclic carbenes (NHCs) have become without doubt one of the most exciting and popular species in chemical science due to the ease of their preparation and modularity in stereoelectronic properties. Numerous types of NHCs have been prepared, and various experimental methodologies have been proposed for the study of their electronic properties in order to rationalize reactivities observed. The objective of this article is to provide a comprehensive overview of the most common and popular ones among them. Read More

    From "Cellular" RNA to "Smart" RNA: Multiple Roles of RNA in Genome Stability and Beyond.
    Chem Rev 2018 Apr 30;118(8):4365-4403. Epub 2018 Mar 30.
    IFOM - The FIRC Institute of Molecular Oncology , Milan , 20139 , Italy.
    Coding for proteins has been considered the main function of RNA since the "central dogma" of biology was proposed. The discovery of noncoding transcripts shed light on additional roles of RNA, ranging from the support of polypeptide synthesis, to the assembly of subnuclear structures, to gene expression modulation. Cellular RNA has therefore been recognized as a central player in often unanticipated biological processes, including genomic stability. Read More

    Substrate Directed Asymmetric Reactions.
    Chem Rev 2018 Apr 23;118(7):3391-3446. Epub 2018 Mar 23.
    Molecular Catalyst Research Center , Chubu University , 1200, Matsumoto-Cho , Kasugai , Aichi 487-8501 , Japan.
    Historically, reagent controlled reactions (mechanism controlled reactions) have played a significant role in the asymmetric synthesis of complex structures. In contrast, today's asymmetric synthesis is greatly dependent on substrate directed approaches. In this approach, a polar functional group, namely, a "directing group", in the vicinity of the reactive site inside the substrate has been documented to preassociate with the chiral catalyst, which exerts stereodirecting influence by directing the reacting partner toward one of the enantiotopic faces of the reaction center. Read More

    Design and Mechanism of GABA Aminotransferase Inactivators. Treatments for Epilepsies and Addictions.
    Chem Rev 2018 Apr 23;118(7):4037-4070. Epub 2018 Mar 23.
    Department of Chemistry, Department of Molecular Biosciences, Chemistry of Life Processes Institute, Center for Molecular Innovation and Drug Discovery, Center for Developmental Therapeutics , Northwestern University , 2145 Sheridan Road , Evanston , Illinois 60208-3113 , United States.
    When the brain concentration of the inhibitory neurotransmitter γ-aminobutyric acid (GABA) diminishes below a threshold level, the excess neuronal excitation can lead to convulsions. This imbalance in neurotransmission can be corrected by inhibition of the enzyme γ-aminobutyric acid aminotransferase (GABA-AT), which catalyzes the conversion of GABA to the excitatory neurotransmitter l-glutamic acid. It also has been found that raising GABA levels can antagonize the rapid elevation and release of dopamine in the nucleus accumbens, which is responsible for the reward response in addiction. Read More

    Flavin-Based Electron Bifurcation, A New Mechanism of Biological Energy Coupling.
    Chem Rev 2018 Apr 21;118(7):3862-3886. Epub 2018 Mar 21.
    Fachbereich Biologie , Philipps-Universität , 35032 Marburg , Germany.
    There are two types of electron bifurcation (EB), either quinone- or flavin-based (QBEB/FBEB), that involve reduction of a quinone or flavin by a two-electron transfer and two reoxidations by a high- and low-potential one-electron acceptor with a reactive semiquinone intermediate. In QBEB, the reduced low-potential acceptor (cytochrome b) is exclusively used to generate ΔμH. In FBEB, the "energy-rich" low-potential reduced ferredoxin or flavodoxin has dual function. Read More

    Spectroscopy in Complex Environments from QM-MM Simulations.
    Chem Rev 2018 Apr 21;118(7):4071-4113. Epub 2018 Mar 21.
    Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE-CONICET, Facultad de Ciencias Exactas y Naturales , Universidad de Buenos Aires , Ciudad Universitaria, Pab. II , C1428EHA Buenos Aires , Argentina.
    The applications of multiscale quantum-classical (QM-MM) approaches have shown an extraordinary expansion and diversification in the last couple of decades. A great proportion of these efforts have been devoted to interpreting and reproducing spectroscopic experiments in a variety of complex environments such as solutions, interfaces, and biological systems. Today, QM-MM-based computational spectroscopy methods constitute accomplished tools with refined predictive power. Read More

    Spin-Vibronic Mechanism for Intersystem Crossing.
    Chem Rev 2018 Mar 20. Epub 2018 Mar 20.
    Institut für Theoretische Chemie, Heinrich-Heine-Universität Düsseldorf , Universitätsstrasse 1 , 40225 Düsseldorf , Germany.
    Intersystem crossing (ISC), formally forbidden within nonrelativistic quantum theory, is the mechanism by which a molecule changes its spin state. It plays an important role in the excited state decay dynamics of many molecular systems and not just those containing heavy elements. In the simplest case, ISC is driven by direct spin-orbit coupling between two states of different multiplicities. Read More

    Oxidative Addition and Reductive Elimination at Main-Group Element Centers.
    Chem Rev 2018 Apr 20;118(7):3608-3680. Epub 2018 Mar 20.
    Department of Chemistry , Brock University , 1812 Sir Isaac Brock Way , St. Catharines , Ontario L2S 3A1 , Canada.
    Oxidative addition and reductive elimination are key steps in a wide variety of catalytic reactions mediated by transition-metal complexes. Historically, this reactivity has been considered to be the exclusive domain of d-block elements. However, this paradigm has changed in recent years with the demonstration of transition-metal-like reactivity by main-group compounds. Read More

    Nonfullerene Acceptor Molecules for Bulk Heterojunction Organic Solar Cells.
    Chem Rev 2018 Apr 20;118(7):3447-3507. Epub 2018 Mar 20.
    Department of Chemistry and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration & Reconstruction , Hong Kong University of Science and Technology (HKUST) , Clear Water Bay , Kowloon, Hong Kong , China.
    The bulk-heterojunction blend of an electron donor and an electron acceptor material is the key component in a solution-processed organic photovoltaic device. In the past decades, a p-type conjugated polymer and an n-type fullerene derivative have been the most commonly used electron donor and electron acceptor, respectively. While most advances of the device performance come from the design of new polymer donors, fullerene derivatives have almost been exclusively used as electron acceptors in organic photovoltaics. Read More

    Mass Spectrometry Approaches to Glycomic and Glycoproteomic Analyses.
    Chem Rev 2018 Mar 19. Epub 2018 Mar 19.
    Department of Chemistry , University of California, Davis , One Shields Avenue , Davis , California 95616 , United States.
    Glycomic and glycoproteomic analyses involve the characterization of oligosaccharides (glycans) conjugated to proteins. Glycans are produced through a complicated nontemplate driven process involving the competition of enzymes that extend the nascent chain. The large diversity of structures, the variations in polarity of the individual saccharide residues, and the poor ionization efficiencies of glycans all conspire to make the analysis arguably much more difficult than any other biopolymer. Read More

    Emerging Two-Dimensional Nanomaterials for Electrocatalysis.
    Chem Rev 2018 Mar 19. Epub 2018 Mar 19.
    School of Chemical Engineering , The University of Adelaide , Adelaide , SA 5005 , Australia.
    Over the past few decades, the design and development of advanced electrocatalysts for efficient energy conversion technologies have been subjects of extensive study. With the discovery of graphene, two-dimensional (2D) nanomaterials have emerged as some of the most promising candidates for heterogeneous electrocatalysts due to their unique physical, chemical, and electronic properties. Here, we review 2D-nanomaterial-based electrocatalysts for selected electrocatalytic processes. Read More

    Designing Smart Polymer Conjugates for Controlled Release of Payloads.
    Chem Rev 2018 Apr 13;118(7):3965-4036. Epub 2018 Mar 13.
    Department of Materials Science and Engineering, School of Molecular Science and Engineering , Vidyasirimedhi Institute of Science and Technology , Rayong 21210 , Thailand.
    Incorporating labile bonds inside polymer backbone and side chains yields interesting polymer materials that are responsive to change of environmental stimuli. Drugs can be conjugated to various polymers through different conjugation linkages and spacers. One of the key factors influencing the release profile of conjugated drugs is the hydrolytic stability of the conjugated linkage. Read More

    Capillary Electrophoresis Separations of Glycans.
    Chem Rev 2018 Mar 12. Epub 2018 Mar 12.
    C. Eugene Bennett Department of Chemistry , West Virginia University , Morgantown , West Virginia 26506 , United States.
    Capillary electrophoresis has emerged as a powerful approach for carbohydrate analyses since 2014. The method provides high resolution capable of separating carbohydrates by charge-to-size ratio. Principle applications are heavily focused on N-glycans, which are highly relevant to biological therapeutics and biomarker research. Read More

    Gas-Phase Reactions of Isoprene and Its Major Oxidation Products.
    Chem Rev 2018 Apr 9;118(7):3337-3390. Epub 2018 Mar 9.
    Isoprene carries approximately half of the flux of non-methane volatile organic carbon emitted to the atmosphere by the biosphere. Accurate representation of its oxidation rate and products is essential for quantifying its influence on the abundance of the hydroxyl radical (OH), nitrogen oxide free radicals (NO ), ozone (O), and, via the formation of highly oxygenated compounds, aerosol. We present a review of recent laboratory and theoretical studies of the oxidation pathways of isoprene initiated by addition of OH, O, the nitrate radical (NO), and the chlorine atom. Read More

    Stability and Reactivity: Positive and Negative Aspects for Nanoparticle Processing.
    Chem Rev 2018 Apr 8;118(7):3209-3250. Epub 2018 Mar 8.
    Division of Nanomaterials and Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, CAS Centre for Excellence in Nanoscience, Collaborative Innovation Center of Suzhou Nano Science and Technology, Hefei Science Centre of CAS, Department of Chemistry , University of Science and Technology of China , Hefei 230026 , China.
    Nanoparticles exist far from the equilibrium state due to their high surface energy. Nanoparticles are therefore extremely unstable and easily change themselves or react with active substances to reach a relatively stable state in some cases. This causes desired changes or undesired changes to nanoparticles and thus makes them exhibit a high reactivity and a poor stability. Read More

    Divergent Strategy in Natural Product Total Synthesis.
    Chem Rev 2018 Apr 8;118(7):3752-3832. Epub 2018 Mar 8.
    State Key Laboratory of Natural and Biomimetic Drugs, School of Pharmaceutical Sciences , Peking University , 38 Xueyuan Road , Beijing 100191 , China.
    The divergent total syntheses of complex natural products from a common intermediate have attracted enormous attention in the chemical community in the past few years because it can improve the efficiency of chemical synthesis. A number of powerful and unified strategies have been developed by emulating the natural biosynthesis or through innovative transformations. This review focuses on the total synthesis of natural products by applying divergent strategies and the literature covering from 2013 to June 2017. Read More

    In Situ, Time-Resolved, and Mechanistic Studies of Metal-Organic Framework Nucleation and Growth.
    Chem Rev 2018 Apr 7;118(7):3681-3721. Epub 2018 Mar 7.
    Theoretical Chemistry Institute and Department of Chemistry , University of Wisconsin-Madison , Madison , Wisconsin 53706 , United States.
    The vast chemical and structural diversity of metal-organic frameworks (MOFs) opens up the exciting possibility of "crystal engineering" MOFs tailored for particular catalytic or separation applications. Yet the process of reaction discovery, optimization, and scale-up of MOF synthesis remains extremely challenging, presenting significant obstacles to the synthetic realization of many otherwise promising MOF structures. Recently, significant new insights into the fundamental processes governing MOF nucleation and growth, as well as the relationship between reaction parameters and synthetic outcome, have been derived using powerful in situ, time-resolved and/or mechanistic studies of MOF crystallization. Read More

    Light-Driven Sodium-Pumping Rhodopsin: A New Concept of Active Transport.
    Chem Rev 2018 Mar 7. Epub 2018 Mar 7.
    PRESTO, Japan Science and Technology Agency , 4-1-8 Honcho , Kawaguchi , Saitama 332-0012 , Japan.
    Ion pumps perform active transport of ions by using energy. The active transport mechanism can be illustrated by the Panama Canal model, which considers two gates and a gain in energy. The Panama Canal model is consistent with the alternating access model that is used to describe active transport, in which the substrate ion is bound, energized, and released. Read More

    Using Physical Organic Chemistry To Shape the Course of Electrochemical Reactions.
    Chem Rev 2018 May 2;118(9):4817-4833. Epub 2018 Mar 2.
    Washington University in St. Louis , St. Louis , Missouri 63130 , United States.
    While organic electrochemistry can look quite different to a chemist not familiar with the technique, the reactions are at their core organic reactions. As such, they are developed and optimized using the same physical organic chemistry principles employed during the development of any other organic reaction. Certainly, the electron transfer that triggers the reactions can require a consideration of new "wrinkles" to those principles, but those considerations are typically minimal relative to the more traditional approaches needed to manipulate the pathways available to the reactive intermediates formed downstream of that electron transfer. Read More

    Chemi- and Bioluminescence of Cyclic Peroxides.
    Chem Rev 2018 Mar 1. Epub 2018 Mar 1.
    Department of Chemistry-Ångström, Uppsala University , P.O. Box 538, SE-751 21 Uppsala, Sweden.
    Bioluminescence is a phenomenon that has fascinated mankind for centuries. Today the phenomenon and its sibling, chemiluminescence, have impacted society with a number of useful applications in fields like analytical chemistry and medicine, just to mention two. In this review, a molecular-orbital perspective is adopted to explain the chemistry behind chemiexcitation in both chemi- and bioluminescence. Read More

    Tandem Hydroaminomethylation Reaction to Synthesize Amines from Alkenes.
    Chem Rev 2018 Apr 1;118(7):3833-3861. Epub 2018 Mar 1.
    Laboratoire de Chimie de Coordination du CNRS UPR 8241 , Composante ENSIACET de l'Institut National Polytechnique de Toulouse, University of Toulouse UPS-INP , 4 allée Emile Monso , 31030 Toulouse Cedex 4 , France.
    In the context of atom economy and low environmental impact, synthesis of amines by an efficient catalytic process is of great importance to produce these building blocks for fine chemical industry. The one-pot hydroaminomethylation of alkenes is a tandem reaction which involves three successive steps under CO/H pressure to perform the catalyzed hydroformylation of the alkene into the corresponding aldehyde followed by its condensation with a N-H function and the catalyzed hydrogenation of the imine/enamine intermediate into the corresponding saturated amine. Rhodium and more recently ruthenium complexes have been designed to combine high conversions of the reactants and chemoselectivity in the expected amines with high regioselectivity in either the linear or the branched amine. Read More

    Perturbations of Native Membrane Protein Structure in Alkyl Phosphocholine Detergents: A Critical Assessment of NMR and Biophysical Studies.
    Chem Rev 2018 Apr 28;118(7):3559-3607. Epub 2018 Feb 28.
    Université Grenoble Alpes, CEA, CNRS, IBS , Grenoble F-38000 , France.
    Membrane proteins perform a host of vital cellular functions. Deciphering the molecular mechanisms whereby they fulfill these functions requires detailed biophysical and structural investigations. Detergents have proven pivotal to extract the protein from its native surroundings. Read More

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