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Chemical Reviews

Quintin R Sheridan, William F Schneider, Edward J Maginn
Ionic liquids (ILs) have gained considerable attention in recent years as CO2 -reactive solvents that could be used to improve the economic efficiency of industrial-scale CO2 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 CO2 ...
April 24, 2018: Chemical Reviews
Irina P Beletskaya, Carmen Nájera, Miguel Yus
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. Finally, stereodivergent intramolecular and intermolecular cycloadditions and other cyclizations are also reported...
April 20, 2018: Chemical Reviews
Yiou Wang, Hajime Suzuki, Jijia Xie, Osamu Tomita, David James Martin, Masanobu Higashi, Dan Kong, Ryu Abe, Junwang Tang
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...
April 20, 2018: Chemical Reviews
David Perez-Guaita, Katarzyna M Marzec, Andrew Hudson, Corey Evans, Tatyana Chernenko, Christian Matthäus, Milos Miljkovic, Max Diem, Philip Heraud, Jack S Richards, Dean Andrew, David A Anderson, Christian Doerig, Jose Garcia-Bustos, Don McNaughton, Bayden R Wood
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. Here, we review the application of vibrational spectroscopic techniques for monitoring and detecting malaria infection...
April 20, 2018: Chemical Reviews
Nicholas J Hestand, Frank C Spano
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...
April 17, 2018: Chemical Reviews
Lichen Liu, Avelino Corma
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...
April 16, 2018: Chemical Reviews
Nicholas J Barrows, Rafael K Campos, Kuo-Chieh Liao, K Reddisiva Prasanth, Ruben Soto-Acosta, Shih-Chia Yeh, Geraldine Schott-Lerner, Julien Pompon, October M Sessions, Shelton S Bradrick, Mariano A Garcia-Blanco
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...
April 13, 2018: Chemical Reviews
David Casanova
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. The work revisits important aspects regarding electronic states involved in the process, the evaluation of fission rates and interstate couplings, the study of the excited state dynamics in singlet fission, and the advances in the design and characterization of singlet fission compounds and materials such as molecular dimers, polymers, or extended structures...
April 12, 2018: Chemical Reviews
Cheng Zong, Mengxi Xu, Li-Jia Xu, Ting Wei, Xin Ma, Xiao-Shan Zheng, Ren Hu, Bin Ren
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. However, there are still great challenges that need to be addressed until it can be widely accepted by the biorelated communities, answer interesting biological questions, and solve fatal clinical problems...
April 11, 2018: Chemical Reviews
Jorge G Ibanez, Marina E Rincón, Silvia Gutierrez-Granados, M'hamed Chahma, Oscar A Jaramillo-Quintero, Bernardo A Frontana-Uribe
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...
April 9, 2018: Chemical Reviews
Yuta Tsuji, Ernesto Estrada, Ramis Movassagh, Roald Hoffmann
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...
April 9, 2018: Chemical Reviews
Yujie Liang, Jialiang Wei, Xu Qiu, Ning Jiao
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. Therefore, it is not surprising that tremendous attention has been paid to enzymatic oxygenation...
April 9, 2018: Chemical Reviews
Christopher T Walsh, Benjamin P Tu, Yi Tang
No abstract text is available yet for this article.
April 5, 2018: Chemical Reviews
Yi Zhu, Jianlin Han, Jiandong Wang, Norio Shibata, Mikiko Sodeoka, Vadim A Soloshonok, Jaime A S Coelho, F Dean Toste
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...
April 2, 2018: Chemical Reviews
Han Vinh Huynh
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...
March 30, 2018: Chemical Reviews
Flavia Michelini, Ameya P Jalihal, Sofia Francia, Chance Meers, Zachary T Neeb, Francesca Rossiello, Ubaldo Gioia, Julio Aguado, Corey Jones-Weinert, Brian Luke, Giuseppe Biamonti, Mariusz Nowacki, Francesca Storici, Piero Carninci, Nils G Walter, Fabrizio d'Adda di Fagagna
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. This ever-expanding list of functions inspired us to think of RNA as a "smart" phone, which has replaced the older obsolete "cellular" phone...
March 30, 2018: Chemical Reviews
Sukalyan Bhadra, Hisashi Yamamoto
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...
March 23, 2018: Chemical Reviews
Richard B Silverman
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...
March 23, 2018: Chemical Reviews
Wolfgang Buckel, Rudolf K Thauer
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. It can give rise to ΔμH+ /Na+ via a ferredoxin:NAD reductase (Rnf) or ferredoxin:proton reductase (Ech) or conducts difficult reductions such as CO2 to CO...
March 21, 2018: Chemical Reviews
Uriel N Morzan, Diego J Alonso de Armiño, Nicolás O Foglia, Francisco Ramírez, Mariano C González Lebrero, Damián A Scherlis, Darío A Estrin
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. The present review summarizes the advances that have been made in QM-MM approaches to UV-visible, Raman, IR, NMR, electron paramagnetic resonance, and Mössbauer spectroscopies, providing in every case an introductory discussion of the corresponding methodological background...
March 21, 2018: Chemical Reviews
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