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Accounts of Chemical Research

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https://www.readbyqxmd.com/read/28339186/quantum-chemical-strain-analysis-for-mechanochemical-processes
#1
Tim Stauch, Andreas Dreuw
The use of mechanical force to initiate a chemical reaction is an efficient alternative to the conventional sources of activation energy, i.e., heat, light, and electricity. Applications of mechanochemistry in academic and industrial laboratories are diverse, ranging from chemical syntheses in ball mills and ultrasound baths to direct activation of covalent bonds using an atomic force microscope. The vectorial nature of force is advantageous because specific covalent bonds can be preconditioned for rupture by selective stretching...
March 24, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28306247/reversible-hydrogenation-of-carbon-dioxide-to-formic-acid-and-methanol-lewis-acid-enhancement-of-base-metal-catalysts
#2
Wesley H Bernskoetter, Nilay Hazari
New and sustainable energy vectors are required as a consequence of the environmental issues associated with the continued use of fossil fuels. H2 is a potential clean energy source, but as a result of problems associated with its storage and transport as a gas, chemical H2 storage (CHS), which involves the dehydrogenation of small molecules, is an attractive alternative. In principle, formic acid (FA, 4.4 wt % H2) and methanol (MeOH, 12.6 wt % H2) can be obtained renewably and are excellent prospective liquid CHS materials...
March 17, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28306237/the-glycan-microarray-story-from-construction-to-applications
#3
Ji Young Hyun, Jaeyoung Pai, Injae Shin
Not only are glycan-mediated binding processes in cells and organisms essential for a wide range of physiological processes, but they are also implicated in various pathological processes. As a result, elucidation of glycan-associated biomolecular interactions and their consequences is of great importance in basic biological research and biomedical applications. In 2002, we and others were the first to utilize glycan microarrays in efforts aimed at the rapid analysis of glycan-associated recognition events...
March 17, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28301139/designing-hydrogels-for-on-demand-therapy
#4
Nuria Oliva, João Conde, Kui Wang, Natalie Artzi
Systemic administration of therapeutic agents has been the preferred approach to treat most pathological conditions, in particular for cancer therapy. This treatment modality is associated with side effects, off-target accumulation, toxicity, and rapid renal and hepatic clearance. Multiple efforts have focused on incorporating targeting moieties into systemic therapeutic vehicles to enhance retention and minimize clearance and side effects. However, only a small percentage of the nanoparticles administered systemically accumulate at the tumor site, leading to poor therapeutic efficacy...
March 16, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28300397/electrochemical-techniques-for-intercalation-electrode-materials-in-rechargeable-batteries
#5
Yujie Zhu, Tao Gao, Xiulin Fan, Fudong Han, Chunsheng Wang
Understanding of the thermodynamic and kinetic properties of electrode materials is of great importance to develop new materials for high performance rechargeable batteries. Compared with computational understanding of physical and chemical properties of electrode materials, experimental methods provide direct and convenient evaluation of these properties. Often, the information gained from experimental work can not only offer feedback for the computational methods but also provide useful insights for improving the performance of materials...
March 16, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28299927/supramolecular-hydrogels-based-on-dna-self-assembly
#6
Yu Shao, Haoyang Jia, Tianyang Cao, Dongsheng Liu
Extracellular matrix (ECM) provides essential supports three dimensionally to the cells in living organs, including mechanical support and signal, nutrition, oxygen, and waste transportation. Thus, using hydrogels to mimic its function has attracted much attention in recent years, especially in tissue engineering, cell biology, and drug screening. However, a hydrogel system that can merit all parameters of the natural ECM is still a challenge. In the past decade, deoxyribonucleic acid (DNA) has arisen as an outstanding building material for the hydrogels, as it has unique properties compared to most synthetic or natural polymers, such as sequence designability, precise recognition, structural rigidity, and minimal toxicity...
March 16, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28296382/human-%C3%AE-defensin-6-a-small-peptide-that-self-assembles-and-protects-the-host-by-entangling-microbes
#7
Phoom Chairatana, Elizabeth M Nolan
Human α-defensin 6 (HD6) is a 32-residue cysteine-rich peptide that contributes to innate immunity by protecting the host at mucosal sites. This peptide is produced in small intestinal Paneth cells, stored as an 81-residue precursor peptide named proHD6 in granules, and released into the lumen. One unusual feature of HD6 is that it lacks the broad-spectrum antimicrobial activity observed for other human α-defensins, including the Paneth cell peptide human α-defensin 5 (HD5). HD6 exhibits unprecedented self-assembly properties, which confer an unusual host-defense function...
March 15, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28287702/simultaneous-determination-of-concentration-and-enantiomeric-composition-in-fluorescent-sensing
#8
Lin Pu
Fluorescent sensors have found broad applications in determining the concentrations of diverse analytes by measuring specific sensor-analyte fluorescent responses. For a chiral substrate containing varying composition of two enantiomers, both the concentration and enantiomeric composition should greatly influence the fluorescent response of an enantioselective fluorescent sensor. Thus, multiple independent measurements are normally needed to determine both the concentration and enantiomeric composition of a chiral compound...
March 13, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28282117/metal-selenides-as-efficient-counter-electrodes-for-dye-sensitized-solar-cells
#9
Zhitong Jin, Meirong Zhang, Min Wang, Chuanqi Feng, Zhong-Sheng Wang
Solar energy is the most abundant renewable energy available to the earth and can meet the energy needs of humankind, but efficient conversion of solar energy to electricity is an urgent issue of scientific research. As the third-generation photovoltaic technology, dye-sensitized solar cells (DSSCs) have gained great attention since the landmark efficiency of ∼7% reported by O'Regan and Grätzel. The most attractive features of DSSCs include low cost, simple manufacturing processes, medium-purity materials, and theoretically high power conversion efficiencies...
March 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28272872/low-energy-co2-release-from-metal-organic-frameworks-triggered-by-external-stimuli
#10
Haiqing Li, Matthew R Hill
Groundbreaking research over the past 15 years has established metal-organic frameworks (MOFs) as adsorbents capable of unprecedented gas adsorption capacity. This has encouraged the contemplation of their use in applications such as increasing the storage capacity in natural gas fuel tanks, or the capture of carbon dioxide from coal-fired flue gas streams. However, while the gas adsorption capacity of MOFs is large, not all stored gas can be readily released to realize the efficient regeneration of MOF adsorbents...
March 8, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28272871/nanoarchitectonics-with-porphyrin-functionalized-dna
#11
Eugen Stulz
DNA is well-known as bearer of the genetic code. Since its structure elucidation nearly seven decades ago by Watson, Crick, Wilkins, and Franklin, much has been learned about its detailed structure, function, and genetic coding. The development of automated solid-phase synthesis, and with it the availability of synthetic DNA with any desired sequence in lengths of up to hundreds of bases in the best case, has contributed much to the advancement of the field of DNA research. In addition, classic organic synthesis has allowed introduction of a very large number of modifications in the DNA in a sequence specific manner, which have initially been targeted at altering the biological function of DNA...
March 8, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28272869/a-pyridine-alkoxide-chelate-ligand-that-promotes-both-unusually-high-oxidation-states-and-water-oxidation-catalysis
#12
Thoe K Michaelos, Dimitar Y Shopov, Shashi Bhushan Sinha, Liam S Sharninghausen, Katherine J Fisher, Hannah M C Lant, Robert H Crabtree, Gary W Brudvig
Water-oxidation catalysis is a critical bottleneck in the direct generation of solar fuels by artificial photosynthesis. Catalytic oxidation of difficult substrates such as water requires harsh conditions, so the ligand must be designed both to stabilize high oxidation states of the metal center and to strenuously resist ligand degradation. Typical ligand choices either lack sufficient electron donor power or fail to stand up to the oxidizing conditions. Our research on Ir-based water-oxidation catalysts (WOCs) has led us to identify a ligand, 2-(2'-pyridyl)-2-propanoate or "pyalk", that fulfills these requirements...
March 8, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28263559/coordination-driven-syntheses-of-compact-supramolecular-metallacycles-toward-extended-metallo-organic-stacked-supramolecular-assemblies
#13
Christophe Lescop
One important concept associated with supramolecular chemistry is supramolecular self-assembly, which deals with the way discrete individual components interact via intermolecular interactions in order to build, upon their spontaneous association, high order functional assemblies. The accumulation of these very simple and localized noncovalent interactions (such as H-bonding, dipole-dipole, hydrophobic/hydrophilic, van der Waals, π-π, π-CH, etc.) is ubiquitous in the complexity of natural systems (such as DNA, proteins, membranes, micelles, etc...
March 6, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28263544/smart-actuators-and-adhesives-for-reconfigurable-matter
#14
Hyunhyub Ko, Ali Javey
Biological systems found in nature provide excellent stimuli-responsive functions. The camouflage adaptation of cephalopods (octopus, cuttlefish), rapid stiffness change of sea cucumbers, opening of pine cones in response to humidity, and rapid closure of Venus flytraps upon insect touch are some examples of nature's smart systems. Although current technologies are still premature to mimic these sophisticated structures and functions in smart biological systems, recent work on stimuli-responsive programmable matter has shown great progress...
March 6, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28257188/homochiral-evolution-in-self-assembled-chiral-polymers-and-block-copolymers
#15
Tao Wen, Hsiao-Fang Wang, Ming-Chia Li, Rong-Ming Ho
The significance of chirality transfer is not only involved in biological systems, such as the origin of homochiral structures in life but also in man-made chemicals and materials. How the chiral bias transfers from molecular level (molecular chirality) to helical chain (conformational chirality) and then to helical superstructure or phase (hierarchical chirality) from self-assembly is vital for the chemical and biological processes in nature, such as communication, replication, and enzyme catalysis. In this Account, we summarize the methodologies for the examination of homochiral evolution at different length scales based on our recent studies with respect to the self-assembly of chiral polymers and chiral block copolymers (BCPs*)...
March 3, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28252940/design-strategies-of-stimuli-responsive-supramolecular-hydrogels-relying-on-structural-analyses-and-cell-mimicking-approaches
#16
Hajime Shigemitsu, Itaru Hamachi
Stimuli-responsive hydrogels are intriguing biomaterials useful for spatiotemporal controlled release of drugs, cells, and biological cues, cell engineering for various applications, and medical diagnosis. To date, many physical and chemical stimuli-responsive polymer hydrogels have been developed by chemical modification of polymer chains and cross-linking points. In particular, conjugation with biomolecules to polymers produced promising biomolecule-responsive hydrogels. These examples clearly indicate high potentials of stimuli-responsive hydrogels as promising biomaterials...
March 2, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28248487/practical-stereochemistry
#17
Richard M Kellogg
The relationship between fundamental and applied is often uneasy, particularly in modern political climates. A familiar political view, aimed negatively at the scientific community, is that the former is a waste of money whereas the latter gives value for investment. The answer that fundamental is required as the basis for practical suffers from the fact that the timelines between fundamental and practical are often long and the routes contorted and unexpected. This has been my experience. In this Account, examples are given from the research in which I have been involved wherein quite fundamental considerations have led to various applications...
March 1, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28248486/stimuli-responsive-dna-based-hydrogels-from-basic-principles-to-applications
#18
Jason S Kahn, Yuwei Hu, Itamar Willner
The base sequence of nucleic acids encodes structural and functional information into the DNA biopolymer. External stimuli such as metal ions, pH, light, or added nucleic acid fuel strands provide triggers to reversibly switch nucleic acid structures such as metal-ion-bridged duplexes, i-motifs, triplex nucleic acids, G-quadruplexes, or programmed double-stranded hybrids of oligonucleotides (DNA). The signal-triggered oligonucleotide structures have been broadly applied to develop switchable DNA nanostructures and DNA machines, and these stimuli-responsive assemblies provide functional scaffolds for the rapidly developing area of DNA nanotechnology...
March 1, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28248480/toward-the-understanding-of-selective-si-nano-oxidation-by-atomic-scale-simulations
#19
Umedjon Khalilov, Annemie Bogaerts, Erik C Neyts
The continuous miniaturization of nanodevices, such as transistors, solar cells, and optical fibers, requires the controlled synthesis of (ultra)thin gate oxides (<10 nm), including Si gate-oxide (SiO2) with high quality at the atomic scale. Traditional thermal growth of SiO2 on planar Si surfaces, however, does not allow one to obtain such ultrathin oxide due to either the high oxygen diffusivity at high temperature or the very low sticking ability of incident oxygen at low temperature. Two recent techniques, both operative at low (room) temperature, have been put forward to overcome these obstacles: (i) hyperthermal oxidation of planar Si surfaces and (ii) thermal or plasma-assisted oxidation of nonplanar Si surfaces, including Si nanowires (SiNWs)...
March 1, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28240855/solution-based-processing-of-monodisperse-two-dimensional-nanomaterials
#20
Joohoon Kang, Vinod K Sangwan, Joshua D Wood, Mark C Hersam
Exfoliation of single-layer graphene from bulk graphite and the subsequent discovery of exotic physics and emergent phenomena in the atomically thin limit has motivated the isolation of other two-dimensional (2D) layered nanomaterials. Early work on isolated 2D nanomaterial flakes has revealed a broad range of unique physical and chemical properties with potential utility in diverse applications. For example, the electronic and optical properties of 2D nanomaterials depend strongly on atomic-scale variations in thickness, enabling enhanced performance in optoelectronic technologies such as light emitters, photodetectors, and photovoltaics...
February 27, 2017: Accounts of Chemical Research
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