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Chemical Reviews

Kei Murakami, Shuya Yamada, Takeshi Kaneda, Kenichiro Itami
Azines, which are six-membered aromatic compounds containing one or more nitrogen atoms, serve as ubiquitous structural cores of aromatic species with important applications in biological and materials sciences. Among a variety of synthetic approaches toward azines, C-H functionalization represents the most rapid and atom-economical transformation, and it is advantageous for the late-stage functionalization of azine-containing functional molecules. Since azines have several C-H bonds with different reactivities, the development of new reactions that allow for the functionalization of azines in a regioselective fashion has comprised a central issue...
April 26, 2017: Chemical Reviews
Xiulai Chen, Cong Gao, Liang Guo, Guipeng Hu, Qiuling Luo, Jia Liu, Jens Nielsen, Jian Chen, Liming Liu
Chemical synthesis is a well established route for producing many chemicals on a large scale, but some drawbacks still exist in this process, such as unstable intermediates, multistep reactions, complex process control, etc. Biobased production provides an attractive alternative to these challenges, but how to make cells into efficient factories is challenging. As a key enabling technology to develop efficient cell factories, design-construction-evaluation-optimization (DCEO) biotechnology, which incorporates the concepts and techniques of pathway design, pathway construction, pathway evaluation, and pathway optimization at the systems level, offers a conceptual and technological framework to exploit potential pathways, modify existing pathways and create new pathways for the optimal production of desired chemicals...
April 26, 2017: Chemical Reviews
Akinori Okano, Nicholas A Isley, Dale L Boger
A review of efforts that have provided total syntheses of vancomycin and related glycopeptide antibiotics, their agylcons, and key analogues is provided. It is a tribute to developments in organic chemistry and the field of organic synthesis that not only can molecules of this complexity be prepared today by total synthesis but such efforts can be extended to the preparation of previously inaccessible key analogues that contain deep-seated structural changes. With the increasing prevalence of acquired bacterial resistance to existing classes of antibiotics and with the emergence of vancomycin-resistant pathogens (VRSA and VRE), the studies pave the way for the examination of synthetic analogues rationally designed to not only overcome vancomycin resistance but provide the foundation for the development of even more powerful and durable antibiotics...
April 24, 2017: Chemical Reviews
Jia-Nan Liu, Wenbo Bu, Jianlin Shi
Hypoxia development in tumor is closely associated with its increased aggressiveness and strong resistance to therapy, leading to the poor prognosis in several cancer types. Clinically, invasive oxygen microelectrode and high dosage radiotherapy are often utilized to accurately detect and effectively fight hypoxia. Recently, however, there has been a surge of interdisciplinary research aiming at developing functional molecules and nanomaterials that can be used to noninvasively image and efficiently treat hypoxic tumors...
April 20, 2017: Chemical Reviews
Wei Ma, Liguang Xu, André F de Moura, Xiaoling Wu, Hua Kuang, Chuanlai Xu, Nicholas A Kotov
The field of chiral inorganic nanostructures is rapidly expanding. It started from the observation of strong circular dichroism during the synthesis of simple nanoparticles (NPs) and their assemblies mediated by biomolecules and expanded to sophisticated synthetic protocols involving nanostructures from metals, semiconductors, ceramics, and nanocarbons. Besides the well-established chirality transfer from bioorganic molecules, other methods to impart handedness to nanoscale matter specific to inorganic materials were discovered, including three-dimentional lithography, multiphoton chirality transfer, polarization effects in nanoscale assemblies, and others...
April 20, 2017: Chemical Reviews
Kyle L Dunbar, Daniel H Scharf, Agnieszka Litomska, Christian Hertweck
Sulfur plays a critical role for the development and maintenance of life on earth, which is reflected by the wealth of primary metabolites, macromolecules, and cofactors bearing this element. Whereas a large body of knowledge has existed for sulfur trafficking in primary metabolism, the secondary metabolism involving sulfur has long been neglected. Yet, diverse sulfur functionalities have a major impact on the biological activities of natural products. Recent research at the genetic, biochemical, and chemical levels has unearthed a broad range of enzymes, sulfur shuttles, and chemical mechanisms for generating carbon-sulfur bonds...
April 18, 2017: Chemical Reviews
Samuel E Sherman, Qi Xiao, Virgil Percec
Synthetic vesicles have been assembled and coassembled from phospholipids, their modified versions, and other single amphiphiles into liposomes, and from block copolymers into polymersomes. Their time-consuming synthesis and preparation as stable, monodisperse, and biocompatible liposomes and polymersomes called for the elaboration of new synthetic methodologies. Amphiphilic Janus dendrimers (JDs) and glycodendrimers (JGDs) represent the most recent self-assembling amphiphiles capable of forming monodisperse, stable, and multifunctional unilamellar and multilamellar onion-like vesicles denoted dendrimersomes (DSs) and glycodendrimersomes (GDSs), dendrimercubosomes (DCs), glycodendrimercubosomes (GDCs), and other complex architectures...
April 18, 2017: Chemical Reviews
Lee J Richter, Dean M DeLongchamp, Aram Amassian
Solution-processed organic films are a facile route to high-speed, low cost, large-area deposition of electrically functional components (transistors, solar cells, emitters, etc.) that can enable a diversity of emerging technologies, from Industry 4.0, to the Internet of things, to point-of-use heath care and elder care. The extreme sensitivity of the functional performance of organic films to structure and the general nonequilibrium nature of solution drying result in extreme processing-performance correlations...
April 17, 2017: Chemical Reviews
Antony Lee, Konstantinos Tsekouras, Christopher Calderon, Carlos Bustamante, Steve Pressé
Super-resolution microscopy provides direct insight into fundamental biological processes occurring at length scales smaller than light's diffraction limit. The analysis of data at such scales has brought statistical and machine learning methods into the mainstream. Here we provide a survey of data analysis methods starting from an overview of basic statistical techniques underlying the analysis of super-resolution and, more broadly, imaging data. We subsequently break down the analysis of super-resolution data into four problems: the localization problem, the counting problem, the linking problem, and what we've termed the interpretation problem...
April 17, 2017: Chemical Reviews
Konstantin G Chernov, Taras A Redchuk, Evgeniya S Omelina, Vladislav V Verkhusha
Phytochrome photoreceptors absorb far-red and near-infrared (NIR) light and regulate light responses in plants, fungi, and bacteria. Their multidomain structure and autocatalytic incorporation of linear tetrapyrrole chromophores make phytochromes attractive molecular templates for the development of light-sensing probes. A subclass of bacterial phytochromes (BphPs) utilizes heme-derived biliverdin tetrapyrrole, which is ubiquitous in mammalian tissues, as a chromophore. Because biliverdin possesses the largest electron-conjugated chromophore system among linear tetrapyrroles, BphPs exhibit the most NIR-shifted spectra that reside within the NIR tissue transparency window...
April 12, 2017: Chemical Reviews
Claudia Coughlan, Maria Ibáñez, Oleksandr Dobrozhan, Ajay Singh, Andreu Cabot, Kevin M Ryan
This review captures the synthesis, assembly, properties, and applications of copper chalcogenide NCs, which have achieved significant research interest in the last decade due to their compositional and structural versatility. The outstanding functional properties of these materials stems from the relationship between their band structure and defect concentration, including charge carrier concentration and electronic conductivity character, which consequently affects their optoelectronic, optical, and plasmonic properties...
April 10, 2017: Chemical Reviews
Jiamei Yu, Lin-Hua Xie, Jian-Rong Li, Yuguang Ma, Jorge M Seminario, Perla B Balbuena
This Review focuses on research oriented toward elucidation of the various aspects that determine adsorption of CO2 in metal-organic frameworks and its separation from gas mixtures found in industrial processes. It includes theoretical, experimental, and combined approaches able to characterize the materials, investigate the adsorption/desorption/reaction properties of the adsorbates inside such environments, screen and design new materials, and analyze additional factors such as material regenerability, stability, effects of impurities, and cost among several factors that influence the effectiveness of the separations...
April 10, 2017: Chemical Reviews
Charles T Campbell, Jason R V Sellers
No abstract text is available yet for this article.
April 10, 2017: Chemical Reviews
Adrian T Keatinge-Clay
The enzymology of 135 assembly lines containing primarily cis-acyltransferase modules is comprehensively analyzed, with greater attention paid to less common phenomena. Diverse online transformations, in which the substrate and/or product of the reaction is an acyl chain bound to an acyl carrier protein, are classified so that unusual reactions can be compared and underlying assembly-line logic can emerge. As a complement to the chemistry surrounding the loading, extension, and offloading of assembly lines that construct primarily polyketide products, structural aspects of the assembly-line machinery itself are considered...
April 10, 2017: Chemical Reviews
Gleb Baryshnikov, Boris Minaev, Hans Ågren
Phosphorescence is a phenomenon of delayed luminescence that corresponds to the radiative decay of the molecular triplet state. As a general property of molecules, phosphorescence represents a cornerstone problem of chemical physics due to the spin prohibition of the underlying triplet-singlet emission and because its analysis embraces a deep knowledge of electronic molecular structure. Phosphorescence is the simplest physical process which provides an example of spin-forbidden transformation with a characteristic spin selectivity and magnetic field dependence, being the model also for more complicated chemical reactions and for spin catalysis applications...
April 7, 2017: Chemical Reviews
Franck Le Bideau, Mohammad Kousara, Li Chen, Lai Wei, Françoise Dumas
The structure elucidation, biosynthesis, and biological activity of marine carbotricyclic sesquiterpene compounds are reviewed from the pioneering results to the end of 2015. Their total syntheses with a particular emphasis on the first syntheses, enantiomeric versions, and syntheses that led to the revision of structures or stereochemistries are summarized. Overall, 284 tricyclic compounds are classified into fused, bridged, and miscellaneous structures based on 54 different skeletal types. Tricyclic sesquiterpenes constitute an important group of natural products...
April 5, 2017: Chemical Reviews
Rui Shang, Laurean Ilies, Eiichi Nakamura
Catalytic C-H bond activation, which was an elusive subject of chemical research until the 1990s, has now become a standard synthetic method for the formation of new C-C and C-heteroatom bonds. The synthetic potential of C-H activation was first described for ruthenium catalysis and is now widely exploited by the use of various precious metals. Driven by the increasing interest in chemical utilization of ubiquitous metals that are abundant and nontoxic, iron catalysis has become a rapidly growing area of research, and iron-catalyzed C-H activation has been most actively explored in recent years...
April 5, 2017: Chemical Reviews
Satoshi Nihonyanagi, Shoichi Yamaguchi, Tahei Tahara
We present an overview of studies on the ultrafast dynamics of water at aqueous interfaces carried out by time-resolved vibrational sum frequency generation (VSFG) spectroscopies. This research field has been growing rapidly, stimulated by technical developments achieved recently. In this review, first, the principles and instrumentations are described for conventional VSFG, heterodyne-detected VSFG, and various IR-pump/VSFG-probe techniques, namely, time-resolved conventional VSFG, time-resolved heterodyne-detected VSFG, and their extension to two-dimensional spectroscopy...
April 5, 2017: Chemical Reviews
Abraham J Waldman, Tai L Ng, Peng Wang, Emily P Balskus
Natural products that contain functional groups with heteroatom-heteroatom linkages (X-X, where X = N, O, S, and P) are a small yet intriguing group of metabolites. The reactivity and diversity of these structural motifs has captured the interest of synthetic and biological chemists alike. Functional groups containing X-X bonds are found in all major classes of natural products and often impart significant biological activity. This review presents our current understanding of the biosynthetic logic and enzymatic chemistry involved in the construction of X-X bond containing functional groups within natural products...
April 4, 2017: Chemical Reviews
Yunxiang Qiao, Wenbao Ma, Nils Theyssen, Chen Chen, Zhenshan Hou
Temperature-responsive ionic liquids (ILs), their fundanmental behaviors, and catalytic applications were introduced, especially the concepts of upper critical solution temperature (UCST) and lower critical solution temperature (LCST). It is described that, during a catalytic reaction, they form a homogeneous mixture with the reactants and products at reaction temperature but separate from them afterward at ambient conditions. It is shown that this behavior offers an effective alternative approach to overcome gas/liquid-solid interface mass transfer limitations in many catalytic transformations...
March 30, 2017: Chemical Reviews
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