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Chemical Reviews

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https://www.readbyqxmd.com/read/28525261/methods-utilizing-first-row-transition-metals-in-natural-product-total-synthesis
#1
Joshua E Zweig, Daria E Kim, Timothy R Newhouse
First-row transition-metal-mediated reactions constitute an important and growing area of research due to the low cost, low toxicity, and exceptional synthetic versatility of these metals. Currently, there is considerable effort to replace existing precious-metal-catalyzed reactions with first-row analogs. More importantly, there are a plethora of unique transformations mediated by first-row metals, which have no classical second- or third-row counterpart. Herein, the application of first-row metal-mediated methods to the total synthesis of natural products is discussed...
May 19, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28520419/single-particle-tracking-from-theory-to-biophysical-applications
#2
Hao Shen, Lawrence J Tauzin, Rashad Baiyasi, Wenxiao Wang, Nicholas Moringo, Bo Shuang, Christy F Landes
After three decades of developments, single particle tracking (SPT) has become a powerful tool to interrogate dynamics in a range of materials including live cells and novel catalytic supports because of its ability to reveal dynamics in the structure-function relationships underlying the heterogeneous nature of such systems. In this review, we summarize the algorithms behind, and practical applications of, SPT. We first cover the theoretical background including particle identification, localization, and trajectory reconstruction...
May 18, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28520418/polycyclic-furanobutenolide-derived-cembranoid-and-norcembranoid-natural-products-biosynthetic-connections-and-synthetic-efforts
#3
Robert A Craig, Brian M Stoltz
The polycyclic furanobutenolide-derived cembranoid and norcembranoid natural products are a family of congested, stereochemically complex, and extensively oxygenated polycyclic diterpenes and norditerpenes. Although the elegant architectures and biological activity profiles of these natural products have captured the attention of chemists since the isolation of the first members of the family in the 1990s, the de novo synthesis of only a single polycyclic furanobutenolide-derived cembranoid and norcembranoid has been accomplished...
May 18, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28517929/computational-modeling-and-simulation-of-co2-capture-by-aqueous-amines
#4
Xin Yang, Robert J Rees, William Conway, Graeme Puxty, Qi Yang, David A Winkler
We review the literature on the use of computational methods to study the reactions between carbon dioxide and aqueous organic amines used to capture CO2 prior to storage, reuse, or sequestration. The focus is largely on the use of high level quantum chemical methods to study these reactions, although the review also summarizes research employing hybrid quantum mechanics/molecular mechanics methods and molecular dynamics. We critically review the effects of basis set size, quantum chemical method, solvent models, and other factors on the accuracy of calculations to provide guidance on the most appropriate methods, the expected performance, method limitations, and future needs and trends...
May 18, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28497955/synthetic-and-therapeutic-applications-of-ammonia-lyases-and-aminomutases
#5
Fabio Parmeggiani, Nicholas J Weise, Syed T Ahmed, Nicholas J Turner
Ammonia-lyases and aminomutases are mechanistically and structurally diverse enzymes which catalyze the deamination and/or isomerization of amino acids in nature by cleaving or shifting a C-N bond. Of the many protein families in which these enzyme activities are found, only a subset have been employed in the synthesis of optically pure fine chemicals or in medical applications. This review covers the natural diversity of these enzymes, highlighting particular enzyme classes that are used within industrial and medical biotechnology...
May 12, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28497687/eukaryotic-translesion-dna-synthesis-on-the-leading-and-lagging-strands-unique-detours-around-the-same-obstacle
#6
Mark Hedglin, Stephen J Benkovic
During S-phase, minor DNA damage may be overcome by DNA damage tolerance (DDT) pathways that bypass such obstacles, postponing repair of the offending damage to complete the cell cycle and maintain cell survival. In translesion DNA synthesis (TLS), specialized DNA polymerases replicate the damaged DNA, allowing stringent DNA synthesis by a replicative polymerase to resume beyond the offending damage. Dysregulation of this DDT pathway in human cells leads to increased mutation rates that may contribute to the onset of cancer...
May 12, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28493667/scaffold-diversity-from-n-acyliminium-ions
#7
Peng Wu, Thomas E Nielsen
N-Acyliminium ions are powerful reactive species for the formation of carbon-carbon and carbon-heteroatom bonds. Strategies relying on intramolecular reactions of N-acyliminium intermediates, also referred to as N-acyliminium ion cyclization reactions, have been employed for the construction of structurally diverse scaffolds, ranging from simple bicyclic skeletons to complex polycyclic systems and natural-product-like compounds. This review aims to provide an overview of cyclization reactions of N-acyliminium ions derived from various precursors for the assembly of structurally diverse scaffolds, covering the literature over the past 12 years (from 2004 to 2015)...
May 11, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28488444/targeting-of-high-valent-iron-taml-activators-at-hydrocarbons-and-beyond
#8
Terrence J Collins, Alexander D Ryabov
TAML activators of peroxides are iron(III) complexes. The ligation by four deprotonated amide nitrogens in macrocyclic motifs is the signature of TAMLs where the macrocyclic structures vary considerably. TAML activators are exceptional functional replicas of the peroxidases and cytochrome P450 oxidizing enzymes. In water, they catalyze peroxide oxidation of a broad spectrum of compounds, many of which are micropollutants, compounds that produce undesired effects at low concentrations-as with the enzymes, peroxide is typically activated with near-quantitative efficiency...
May 10, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28488441/multiscale-studies-on-ionic-liquids
#9
Kun Dong, Xiaomin Liu, Haifeng Dong, Xiangping Zhang, Suojiang Zhang
Ionic liquids (ILs) offer a wide range of promising applications because of their much enhanced properties. However, further development of such materials depends on the fundamental understanding of their hierarchical structures and behaviors, which requires multiscale strategies to provide coupling among various length scales. In this review, we first introduce the structures and properties of these typical ILs. Then, we introduce the multiscale modeling methods that have been applied to the ILs, covering from molecular scale (QM/MM), to mesoscale (CG, DPD), to macroscale (CFD for unit scale and thermodynamics COSMO-RS model and environmental assessment GD method for process scale)...
May 10, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28488435/chalcone-a-privileged-structure-in-medicinal-chemistry
#10
Chunlin Zhuang, Wen Zhang, Chunquan Sheng, Wannian Zhang, Chengguo Xing, Zhenyuan Miao
Privileged structures have been widely used as an effective template in medicinal chemistry for drug discovery. Chalcone is a common simple scaffold found in many naturally occurring compounds. Many chalcone derivatives have also been prepared due to their convenient synthesis. These natural products and synthetic compounds have shown numerous interesting biological activities with clinical potentials against various diseases. This review aims to highlight the recent evidence of chalcone as a privileged scaffold in medicinal chemistry...
May 10, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28488433/attosecond-electron-dynamics-in-molecules
#11
Mauro Nisoli, Piero Decleva, Francesca Calegari, Alicia Palacios, Fernando Martín
Advances in attosecond science have led to a wealth of important discoveries in atomic, molecular, and solid-state physics and are progressively directing their footsteps toward problems of chemical interest. Relevant technical achievements in the generation and application of extreme-ultraviolet subfemtosecond pulses, the introduction of experimental techniques able to follow in time the electron dynamics in quantum systems, and the development of sophisticated theoretical methods for the interpretation of the outcomes of such experiments have raised a continuous growing interest in attosecond phenomena, as demonstrated by the vast literature on the subject...
May 10, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28481088/artificial-biocatalytic-linear-cascades-for-preparation-of-organic-molecules
#12
Joerg H Schrittwieser, Stefan Velikogne, Mélanie Hall, Wolfgang Kroutil
The review compiles artificial cascades involving enzymes with a focus on the last 10 years. A cascade is defined as the combination of at least two reaction steps in a single reaction vessel without isolation of the intermediates, whereby at least one step is catalyzed by an enzyme. Additionally, cascades performed in vivo and in vitro are discussed separately, whereby in vivo cascades are defined here as cascades relying on cofactor recycling by the metabolism or on a metabolite from the living organism. The review introduces a systematic classification of the cascades according to the number of enzymes in the linear sequence and differentiates between cascades involving exclusively enzymes and combinations of enzymes with non-natural catalysts or chemical steps...
May 8, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28475312/information-retrieval-and-text-mining-technologies-for-chemistry
#13
Martin Krallinger, Obdulia Rabal, Anália Lourenço, Julen Oyarzabal, Alfonso Valencia
Efficient access to chemical information contained in scientific literature, patents, technical reports, or the web is a pressing need shared by researchers and patent attorneys from different chemical disciplines. Retrieval of important chemical information in most cases starts with finding relevant documents for a particular chemical compound or family. Targeted retrieval of chemical documents is closely connected to the automatic recognition of chemical entities in the text, which commonly involves the extraction of the entire list of chemicals mentioned in a document, including any associated information...
May 5, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28475304/direct-conversion-of-methane-to-value-added-chemicals-over-heterogeneous-catalysts-challenges-and-prospects
#14
Pierre Schwach, Xiulian Pan, Xinhe Bao
The quest for an efficient process to convert methane efficiently to fuels and high value-added chemicals such as olefins and aromatics is motivated by their increasing demands and recently discovered large reserves and resources of methane. Direct conversion to these chemicals can be realized either oxidatively via oxidative coupling of methane (OCM) or nonoxidatively via methane dehydroaromatization (MDA), which have been under intensive investigation for decades. While industrial applications are still limited by their low yield (selectivity) and stability issues, innovations in new catalysts and concepts are needed...
May 5, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28467054/cyclopropanation-strategies-in-recent-total-syntheses
#15
Christian Ebner, Erick M Carreira
Complex molecular architectures containing cyclopropanes present significant challenges for any synthetic chemist. This review aims to highlight the strategic considerations for introduction of the cyclopropane motif in a collection of recent total syntheses. At first, an overview of the most important and widely used cyclopropanation techniques is presented, followed by a discussion of elegant approaches and clever solutions that have been developed to enable the synthesis of various unique cyclopropane natural products or use of cyclopropanes as versatile strategic intermediates...
May 3, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28466644/development-of-halogenase-enzymes-for-use-in-synthesis
#16
Jonathan Latham, Eileen Brandenburger, Sarah A Shepherd, Binuraj R K Menon, Jason Micklefield
Nature has evolved halogenase enzymes to regioselectively halogenate a diverse range of biosynthetic precursors, with the halogens introduced often having a profound effect on the biological activity of the resulting natural products. Synthetic endeavors to create non-natural bioactive small molecules for pharmaceutical and agrochemical applications have also arrived at a similar conclusion: halogens can dramatically improve the properties of organic molecules for selective modulation of biological targets in vivo...
May 3, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28459547/ionic-liquids-in-selective-oxidation-catalysts-and-solvents
#17
Chengna Dai, Jie Zhang, Chongpin Huang, Zhigang Lei
Selective oxidation has an important role in environmental and green chemistry (e.g., oxidative desulfurization of fuels and oxidative removal of mercury) as well as chemicals and intermediates chemistry to obtain high-value-added special products (e.g., organic sulfoxides and sulfones, aldehydes, ketones, carboxylic acids, epoxides, esters, and lactones). Due to their unique physical properties such as the nonvolatility, thermal stability, nonexplosion, high polarity, and temperature-dependent miscibility with water, ionic liquids (ILs) have attracted considerable attention as reaction solvents and media for selective oxidations and are considered as green alternatives to volatile organic solvents...
May 1, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28459540/homogeneous-functionalization-of-methane
#18
Niles Jensen Gunsalus, Anjaneyulu Koppaka, Sae Hume Park, Steven M Bischof, Brian G Hashiguchi, Roy A Periana
One of the remaining "grand challenges" in chemistry is the development of a next generation, less expensive, cleaner process that can allow the vast reserves of methane from natural gas to augment or replace oil as the source of fuels and chemicals. Homogeneous (gas/liquid) systems that convert methane to functionalized products with emphasis on reports after 1995 are reviewed. Gas/solid, bioinorganic, biological, and reaction systems that do not specifically involve methane functionalization are excluded...
May 1, 2017: Chemical Reviews
https://www.readbyqxmd.com/read/28445033/c-h-functionalization-of-azines
#19
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
https://www.readbyqxmd.com/read/28443658/dceo-biotechnology-tools-to-design-construct-evaluate-and-optimize-the-metabolic-pathway-for-biosynthesis-of-chemicals
#20
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
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