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Chemical Reviews

Aditi R Deshpande, Thomas C Pochapsky, Dagmar Ringe
Acireductone dioxygenase (ARD) from the methionine salvage pathway (MSP) is a unique enzyme that exhibits dual chemistry determined solely by the identity of the divalent transition-metal ion (Fe(2+) or Ni(2+)) in the active site. The Fe(2+)-containing isozyme catalyzes the on-pathway reaction using substrates 1,2-dihydroxy-3-keto-5-methylthiopent-1-ene (acireductone) and dioxygen to generate formate and the ketoacid precursor of methionine, 2-keto-4-methylthiobutyrate, whereas the Ni(2+)-containing isozyme catalyzes an off-pathway shunt with the same substrates, generating methylthiopropionate, carbon monoxide, and formate...
July 21, 2017: Chemical Reviews
Mingying Yang, Kegan Sunderland, Chuanbin Mao
Novel affinity agents with high specificity are needed to make progress in disease diagnosis and therapy. Over the last several years, peptides have been considered to have fundamental benefits over other affinity agents, such as antibodies, due to their fast blood clearance, low immunogenicity, rapid tissue penetration, and reproducible chemical synthesis. These features make peptides ideal affinity agents for applications in disease diagnostics and therapeutics for a wide variety of afflictions. Virus-derived peptide techniques provide a rapid, robust, and high-throughput way to identify organism-targeting peptides with high affinity and selectivity...
July 19, 2017: Chemical Reviews
Fabian Schwizer, Yasunori Okamoto, Tillmann Heinisch, Yifan Gu, Michela M Pellizzoni, Vincent Lebrun, Raphael Reuter, Valentin Köhler, Jared C Lewis, Thomas R Ward
The incorporation of a synthetic, catalytically competent metallocofactor into a protein scaffold to generate an artificial metalloenzyme (ArM) has been explored since the late 1970's. Progress in the ensuing years was limited by the tools available for both organometallic synthesis and protein engineering. Advances in both of these areas, combined with increased appreciation of the potential benefits of combining attractive features of both homogeneous catalysis and enzymatic catalysis, led to a resurgence of interest in ArMs starting in the early 2000's...
July 17, 2017: Chemical Reviews
Deborah Fass, Colin Thorpe
Cysteine thiols are among the most reactive functional groups in proteins, and their pairing in disulfide linkages is a common post-translational modification in proteins entering the secretory pathway. This modest amino acid alteration, the mere removal of a pair of hydrogen atoms from juxtaposed cysteine residues, contrasts with the substantial changes that characterize most other post-translational reactions. However, the wide variety of proteins that contain disulfides, the profound impact of cross-linking on the behavior of the protein polymer, the numerous and diverse players in intracellular pathways for disulfide formation, and the distinct biological settings in which disulfide bond formation can take place belie the simplicity of the process...
July 12, 2017: Chemical Reviews
Majed Chergui, Eric Collet
We review the tremendous advances in ultrafast X-ray science, over the past 15 years, making the best use of new ultrashort X-ray sources including table-top or large-scale facilities. Different complementary X-ray-based techniques, including spectroscopy, scattering, and diffraction, are presented. The broad and expanding spectrum of these techniques in the ultrafast time domain is delivering new insight into the dynamics of molecular systems, of solutions, of solids, and of biosystems. Probing the time evolution of the electronic and structural degrees of freedom of these systems on the time scales of femtosecond to picoseconds delivers new insight into our understanding of dynamical matter...
July 10, 2017: Chemical Reviews
Shaojuan Zeng, Xiangping Zhang, Lu Bai, Xiaochun Zhang, Hui Wang, Jianji Wang, Di Bao, Mengdie Li, Xinyan Liu, Suojiang Zhang
The inherent structure tunability, good affinity with CO2, and nonvolatility of ionic liquids (ILs) drive their exploration and exploitation in CO2 separation field, and has attracted remarkable interest from both industries and academia. The aim of this Review is to give a detailed overview on the recent advances on IL-based materials, including pure ILs, IL-based solvents, and IL-based membranes for CO2 capture and separation from the viewpoint of molecule to engineering. The effects of anions, cations and functional groups on CO2 solubility and selectivity of ILs, as well as the studies on degradability of ILs are reviewed, and the recent developments on functionalized ILs, IL-based solvents, and IL-based membranes are also discussed...
July 7, 2017: Chemical Reviews
Carlo Pifferi, Gour Chand Daskhan, Michele Fiore, Tze Chieh Shiao, René Roy, Olivier Renaudet
Among other classes of biomolecules, carbohydrates and glycoconjugates are widely involved in numerous biological functions. In addition to addressing the related synthetic challenges, glycochemists have invested intense efforts in providing access to structures that can be used to study, activate, or inhibit these biological processes. Over the past few decades, aminooxylated carbohydrates have been found to be key building blocks for achieving these goals. This review provides the first in-depth overview covering several aspects related to the syntheses and applications of aminooxylated carbohydrates...
July 6, 2017: Chemical Reviews
Henan Li, Ying Li, Areej Aljarb, Yumeng Shi, Lain-Jong Li
Recently there have been many research breakthroughs in two-dimensional (2D) materials including graphene, boron nitride (h-BN), black phosphors (BPs), and transition-metal dichalcogenides (TMDCs). The unique electrical, optical, and thermal properties in 2D materials are associated with their strictly defined low dimensionalities. These materials provide a wide range of basic building blocks for next-generation electronics. The chemical vapor deposition (CVD) technique has shown great promise to generate high-quality TMDC layers with scalable size, controllable thickness, and excellent electronic properties suitable for both technological applications and fundamental sciences...
July 6, 2017: Chemical Reviews
Mansi S Shah, Michael Tsapatsis, J Ilja Siepmann
Hydrogen sulfide removal is a long-standing economic and environmental challenge faced by the oil and gas industries. H2S separation processes using reactive and non-reactive absorption and adsorption, membranes, and cryogenic distillation are reviewed. A detailed discussion is presented on new developments in adsorbents, such as ionic liquids, metal oxides, metals, metal-organic frameworks, zeolites, carbon-based materials, and composite materials; and membrane technologies for H2S removal. This Review attempts to exhaustively compile the existing literature on sour gas sweetening and to identify promising areas for future developments in the field...
July 5, 2017: Chemical Reviews
Hui Huang, Lei Yang, Antonio Facchetti, Tobin J Marks
Constructing highly planar, extended π-electron systems is an important strategy for achieving high-mobility organic semiconductors. In general, there are two synthetic strategies for achieving π-conjugated systems with high planarity. The conventional strategy connects neighboring aromatic rings through covalent bonds to restrict the rotation about single bonds. However, this usually requires a complex sequence of synthetic steps to achieve this target, which can be costly and labor-intensive. More recently, noncovalent through-space intramolecular interactions, which are defined here as noncovalent conformational locks, have been employed with great success to increase the planarity and rigidity of extended π-electron systems; this has become a well-known and important strategy to design and synthesize highly planar π-conjugated systems for organic electronics...
July 3, 2017: Chemical Reviews
Pedro Molina, Fabiola Zapata, Antonio Caballero
This review highlights the most significant examples of an emerging field in the design of highly selective anion receptors. To date, there has been remarkable progress in the binding and sensing of anions. This has been driven in part by the discovery of ways to construct effective anion binding receptors using the dominant N-H functional groups and neutral and cationic C-H hydrogen bond donors, as well as underexplored strong directional noncovalent interactions such as halogen-bonding and anion-π interactions...
June 30, 2017: Chemical Reviews
Andrea Álvarez, Atul Bansode, Atsushi Urakawa, Anastasiya V Bavykina, Tim A Wezendonk, Michiel Makkee, Jorge Gascon, Freek Kapteijn
The recent advances in the development of heterogeneous catalysts and processes for the direct hydrogenation of CO2 to formate/formic acid, methanol, and dimethyl ether are thoroughly reviewed, with special emphasis on thermodynamics and catalyst design considerations. After introducing the main motivation for the development of such processes, we first summarize the most important aspects of CO2 capture and green routes to produce H2. Once the scene in terms of feedstocks is introduced, we carefully summarize the state of the art in the development of heterogeneous catalysts for these important hydrogenation reactions...
June 28, 2017: Chemical Reviews
Jacek Zielonka, Joy Joseph, Adam Sikora, Micael Hardy, Olivier Ouari, Jeannette Vasquez-Vivar, Gang Cheng, Marcos Lopez, Balaraman Kalyanaraman
Mitochondria are recognized as one of the most important targets for new drug design in cancer, cardiovascular, and neurological diseases. Currently, the most effective way to deliver drugs specifically to mitochondria is by covalent linking a lipophilic cation such as an alkyltriphenylphosphonium moiety to a pharmacophore of interest. Other delocalized lipophilic cations, such as rhodamine, natural and synthetic mitochondria-targeting peptides, and nanoparticle vehicles, have also been used for mitochondrial delivery of small molecules...
June 27, 2017: Chemical Reviews
Harald Oberhofer, Karsten Reuter, Jochen Blumberger
The booming field of molecular electronics has fostered a surge of computational research on electronic properties of organic molecular solids. In particular, with respect to a microscopic understanding of transport and loss mechanisms, theoretical studies assume an ever-increasing role. Owing to the tremendous diversity of organic molecular materials, a great number of computational methods have been put forward to suit every possible charge transport regime, material, and need for accuracy. With this review article we aim at providing a compendium of the available methods, their theoretical foundations, and their ranges of validity...
June 23, 2017: Chemical Reviews
Laure Konnert, Evelina Colacino
The review highlights the hydantoin syntheses presented from the point of view of the preparation methods. Novel synthetic routes to various hydantoin structures, the advances brought to the classical methods in the aim of producing more sustainable and environmentally friendly procedures for the preparation of these biomolecules, and a critical comparison of the different synthetic approaches developed in the last twelve years are also described. The review is composed of 95 schemes, 8 figures and 528 references for the last 12 years and includes the description of the hydantoin-based marketed drugs and clinical candidates...
June 23, 2017: Chemical Reviews
Dominik K Kölmel, Eric T Kool
The formation of oximes and hydrazones is employed in numerous scientific fields as a simple and versatile conjugation strategy. This imine-forming reaction is applied in fields as diverse as polymer chemistry, biomaterials and hydrogels, dynamic combinatorial chemistry, organic synthesis, and chemical biology. Here we outline chemical developments in this field, with special focus on the past ∼10 years of developments. Recent strategies for installing reactive carbonyl groups and α-nucleophiles into biomolecules are described...
June 22, 2017: Chemical Reviews
Bin Mao, Martín Fañanás-Mastral, Ben L Feringa
γ-Butenolides, γ-butyrolactones, and derivatives, especially in enantiomerically pure form, constitute the structural core of numerous natural products which display an impressive range of biological activities which are important for the development of novel physiological and therapeutic agents. Furthermore, optically active γ-butenolides and γ-butyrolactones serve also as a prominent class of chiral building blocks for the synthesis of diverse biological active compounds and complex molecules. Taking into account the varying biological activity profiles and wide-ranging structural diversity of the optically active γ-butenolide or γ-butyrolactone structure, the development of asymmetric synthetic strategies for assembling such challenging scaffolds has attracted major attention from synthetic chemists in the past decade...
June 22, 2017: Chemical Reviews
Hong-Xia Wang, Mingqiang Li, Ciaran M Lee, Syandan Chakraborty, Hae-Won Kim, Gang Bao, Kam W Leong
Genome editing offers promising solutions to genetic disorders by editing DNA sequences or modulating gene expression. The clustered regularly interspaced short palindromic repeats (CRISPR)/associated protein 9 (CRISPR/Cas9) technology can be used to edit single or multiple genes in a wide variety of cell types and organisms in vitro and in vivo. Herein, we review the rapidly developing CRISPR/Cas9-based technologies for disease modeling and gene correction and recent progress toward Cas9/guide RNA (gRNA) delivery based on viral and nonviral vectors...
June 22, 2017: Chemical Reviews
David J Heldebrant, Phillip K Koech, Vassiliki-Alexandra Glezakou, Roger Rousseau, Deepika Malhotra, David C Cantu
This review is designed to foster the discussion regarding the viability of postcombustion CO2 capture by water-lean solvents, by separating fact from fiction for both skeptics and advocates. We highlight the unique physical and thermodynamic properties of notable water-lean solvents, with a discussion of how such properties could translate to efficiency gains compared to aqueous amines. The scope of this review ranges from the purely fundamental molecular-level processes that govern solvent behavior to bench-scale testing, through process engineering and projections of process performance and cost...
June 19, 2017: Chemical Reviews
Max M Gong, David Sinton
Infectious diseases are a major global health issue. Diagnosis is a critical first step in effectively managing their spread. Paper-based microfluidic diagnostics first emerged in 2007 as a low-cost alternative to conventional laboratory testing, with the goal of improving accessibility to medical diagnostics in developing countries. In this review, we examine the advances in paper-based microfluidic diagnostics for medical diagnosis in the context of global health from 2007 to 2016. The theory of fluid transport in paper is first presented...
June 19, 2017: Chemical Reviews
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