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Accounts of Chemical Research

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https://www.readbyqxmd.com/read/28218831/new-possibilities-for-magnetic-control-of-chemical-and-biochemical-reactions
#1
Anatoly Buchachenko, Ronald G Lawler
Chemistry is controlled by Coulomb energy; magnetic energy is lower by many orders of magnitude and may be confidently ignored in the energy balance of chemical reactions. The situation becomes less clear, however, when reaction rates are considered. In this case, magnetic perturbations of nearly degenerate energy surface crossings may produce observable, and sometimes even dramatic, effects on reactions rates, product yields, and spectroscopic transitions. A case in point that has been studied for nearly five decades is electron spin-selective chemistry via the intermediacy of radical pairs...
February 20, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28207240/interfaces-in-heterogeneous-catalysts-advancing-mechanistic-understanding-through-atomic-scale-measurements
#2
Wenpei Gao, Zachary D Hood, Miaofang Chi
Developing novel catalysts with high efficiency and selectivity is critical for enabling future clean energy conversion technologies. Interfaces in catalyst systems have long been considered the most critical factor in controlling catalytic reaction mechanisms. Interfaces include not only the catalyst surface but also interfaces within catalyst particles and those formed by constructing heterogeneous catalysts. The atomic and electronic structures of catalytic surfaces govern the kinetics of binding and release of reactant molecules from surface atoms...
February 16, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28207235/explorations-of-the-indenofluorenes-and-expanded-quinoidal-analogues
#3
Conerd K Frederickson, Bradley D Rose, Michael M Haley
Highly conjugated hydrocarbons have attracted interest for use as active materials in electronic devices such as organic field effect transistors (OFET) and organic photovoltaics (OPV). In this Account, we review our progress in synthesizing and studying a new class of small molecules for potential use as organic semiconductors. The idea originated from prior research on octadehydrodibenz[12]annulene, as the system can undergo double transannular cyclization to yield the indeno[1,2-b]fluorene skeleton. Subsequent functionalization afforded the first stable, well-characterized indeno[1,2-b]fluorene derivatives, albeit in minute quantities (tens of milligrams)...
February 16, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28205437/surface-and-interface-engineering-of-noble-metal-free-electrocatalysts-for-efficient-energy-conversion-processes
#4
Yun Pei Zhu, Chunxian Guo, Yao Zheng, Shi-Zhang Qiao
Developing cost-effective and high-performance electrocatalysts for renewable energy conversion and storage is motivated by increasing concerns regarding global energy security and creating sustainable technologies dependent on inexpensive and abundant resources. Recent achievements in the design and synthesis of efficient non-precious-metal and even non-metal electrocatalysts make the replacement of noble metal counterparts for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) with earth-abundant elements, for example, C, N, Fe, Mn, and Co, a realistic possibility...
February 16, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28199083/shape-memory-hydrogels-evolution-of-structural-principles-to-enable-shape-switching-of-hydrophilic-polymer-networks
#5
Candy Löwenberg, Maria Balk, Christian Wischke, Marc Behl, Andreas Lendlein
The ability of hydrophilic chain segments in polymer networks to strongly interact with water allows the volumetric expansion of the material and formation of a hydrogel. When polymer chain segments undergo reversible hydration depending on environmental conditions, smart hydrogels can be realized, which are able to shrink/swell and thus alter their volume on demand. In contrast, implementing the capacity of hydrogels to switch their shape rather than volume demands more sophisticated chemical approaches and structural concepts...
February 15, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28191928/self-assembling-multidomain-peptide-nanofibers-for-delivery-of-bioactive-molecules-and-tissue-regeneration
#6
Amanda N Moore, Jeffrey D Hartgerink
Multidomain peptides (MDPs) are a class of self-assembling peptides that are organized in a β-sheet motif, resulting in a nanofibrous architecture. This structure is stabilized by hydrophobic packing in the fiber core and a hydrogen-bonding network down the fiber long axis. Under easily controllable conditions, regulated by electrostatic interactions between the peptides and the pH and salt composition of the solvent, the nanofiber length can be dramatically extended, resulting in fiber entanglement and hydrogel formation...
February 13, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28191927/foldectures-3d-molecular-architectures-from-self-assembly-of-peptide-foldamers
#7
Sung Hyun Yoo, Hee-Seung Lee
The wide range of fascinating supramolecular architectures found in nature, from DNA double helices to giant protein shells, inspires researchers to mimic the diverse shapes and functions of natural systems. Thus, a variety of artificial molecular platforms have been developed by assembling DNA-, peptide-, and protein-based building blocks for medicinal and biological applications. There has also been a significant interest in the research of non-natural oligomers (i.e., foldamers) that fold into well-defined secondary structures analogous to those found in proteins, because the assemblies of foldamers are expected not only to form biomimetic supramolecular architectures that resemble those of nature but also to display unique functions and unprecedented topologies at the same time due to their different folding propensities from those of natural building blocks...
February 13, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28191922/synergistic-integration-of-experimental-and-simulation-approaches-for-the-de-novo-design-of-silk-based-materials
#8
Wenwen Huang, Davoud Ebrahimi, Nina Dinjaski, Anna Tarakanova, Markus J Buehler, Joyce Y Wong, David L Kaplan
Tailored biomaterials with tunable functional properties are crucial for a variety of task-specific applications ranging from healthcare to sustainable, novel bio-nanodevices. To generate polymeric materials with predictive functional outcomes, exploiting designs from nature while morphing them toward non-natural systems offers an important strategy. Silks are Nature's building blocks and are produced by arthropods for a variety of uses that are essential for their survival. Due to the genetic control of encoded protein sequence, mechanical properties, biocompatibility, and biodegradability, silk proteins have been selected as prototype models to emulate for the tunable designs of biomaterial systems...
February 13, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28186727/controlled-synthesis-of-ultralong-carbon-nanotubes-with-perfect-structures-and-extraordinary-properties
#9
Rufan Zhang, Yingying Zhang, Fei Wei
Carbon nanotubes (CNTs) have drawn intensive research interest in the past 25 years due to their excellent properties and wide applications. Ultralong CNTs refers to the horizontally aligned CNT arrays which are usually grown on flat substrates, parallel with each other with large intertube distances. They usually have perfect structures, excellent properties, and lengths up to centimeters, even decimeters. Ultralong CNTs are promising candidates as building blocks for transparent displays, nanoelectronics, superstrong tethers, aeronautics and aerospace materials, etc...
February 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28186723/bioresponsive-dna-hydrogels-beyond-the-conventional-stimuli-responsiveness
#10
Dong Wang, Yue Hu, Peifeng Liu, Dan Luo
Bioresponsive hydrogels can respond to various biological stimuli by a macroscopic change of physical state or by converting biochemical inputs into biological or mechanical outputs. These materials are playing an increasingly important role in a wide variety of applications, especially in the biological and biomedical fields. However, the design and engineering of intriguing bioresponsive materials with adequate biocompatibility and biodegradability have proven to be a great challenge. DNA, on the other hand, possesses many unique and fascinating properties, including its indispensable genetic function, broad biocompatibility, precise molecular recognition capability, tunable multifunctionality, and convenient programmability...
February 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28186717/gating-motions-and-stationary-gating-properties-of-ionotropic-glutamate-receptors-computation-meets-electrophysiology
#11
Huan-Xiang Zhou
Ionotropic glutamate receptors (iGluRs) are tetrameric ligand-gated ion channels essential to all aspects of brain function, including higher order processes such as learning and memory. For decades, electrophysiology was the primary means for characterizing the function of iGluRs and gaining mechanistic insight. Since the turn of the century, structures of isolated water-soluble domains and transmembrane-domain-containing constructs have provided the basis for formulating mechanistic hypotheses. Because these structures only represent sparse, often incomplete snapshots during iGluR activation, significant gaps in knowledge remain regarding structures, energetics, and dynamics of key substates along the functional processes...
February 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28186408/functional-microgels-and-microgel-systems
#12
Felix A Plamper, Walter Richtering
Microgels are macromolecular networks swollen by the solvent in which they are dissolved. They are unique systems that are distinctly different from common colloids, such as, e.g., rigid nanoparticles, flexible macromolecules, micelles, or vesicles. The size of the microgel networks is in the range of several micrometers down to nanometers (then sometimes called "nanogels"). In a collapsed state, they might resemble hard colloids but they can still contain significant amounts of solvent. When swollen, they are soft and have a fuzzy surface with dangling chains...
February 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28186402/next-generation-electrochemical-energy-materials-for-intermediate-temperature-molten-oxide-fuel-cells-and-ion-transport-molten-oxide-membranes
#13
Valery V Belousov
High temperature electrochemical devices such as solid oxide fuel cells (SOFCs) and oxygen separators based on ceramic materials are used for efficient energy conversion. These devices generally operate in the temperature range of 800-1000 °C. The high operating temperatures lead to accelerated degradation of the SOFC and oxygen separator materials. To solve this problem, the operating temperatures of these electrochemical devices must be lowered. However, lowering the temperature is accompanied by decreasing the ionic conductivity of fuel cell electrolyte and oxygen separator membrane...
February 10, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28182404/superatoms-electronic-and-geometric-effects-on-reactivity
#14
Arthur C Reber, Shiv N Khanna
The relative role of electronic and geometric effects on the stability of clusters has been a contentious topic for quite some time, with the focus on electronic structure generally gaining the upper hand. In this Account, we hope to demonstrate that both electronic shell filling and geometric shell filling are necessary concepts for an intuitive understanding of the reactivity of metal clusters. This work will focus on the reactivity of aluminum based clusters, although these concepts may be applied to clusters of different metals and ligand protected clusters...
February 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28182403/forging-the-basis-for-developing-protein-ligand-interaction-scoring-functions
#15
Zhihai Liu, Minyi Su, Li Han, Jie Liu, Qifan Yang, Yan Li, Renxiao Wang
In structure-based drug design, scoring functions are widely used for fast evaluation of protein-ligand interactions. They are often applied in combination with molecular docking and de novo design methods. Since the early 1990s, a whole spectrum of protein-ligand interaction scoring functions have been developed. Regardless of their technical difference, scoring functions all need data sets combining protein-ligand complex structures and binding affinity data for parametrization and validation. However, data sets of this kind used to be rather limited in terms of size and quality...
February 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28181798/shape-morphing-materials-from-stimuli-responsive-hydrogel-hybrids
#16
Seog-Jin Jeon, Adam W Hauser, Ryan C Hayward
The formation of well-defined and functional three-dimensional (3D) structures by buckling of thin sheets subjected to spatially nonuniform stresses is common in biological morphogenesis and has become a subject of great interest in synthetic systems, as such programmable shape-morphing materials hold promise in areas including drug delivery, biomedical devices, soft robotics, and biomimetic systems. Given their ability to undergo large changes in swelling in response to a wide variety of stimuli, hydrogels have naturally emerged as a key type of material in this field...
February 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28181795/water-responsive-shape-recovery-induced-buckling-in-biodegradable-photo-cross-linked-poly-ethylene-glycol-peg-hydrogel
#17
Abhijit Vijay Salvekar, Wei Min Huang, Rui Xiao, Yee Shan Wong, Subbu S Venkatraman, Kiang Hiong Tay, Ze Xiang Shen
The phenomenon of recovering the permanent shape from a severely deformed temporary shape, but only in the presence of the right stimulus, is known as the shape memory effect (SME). Materials with such an interesting effect are known as shape memory materials (SMMs). Typical stimuli to trigger shape recovery include temperature (heating or cooling), chemical (including water/moisture and pH value), and light. As a SMM is able not only to maintain the temporary shape but also to respond to the right stimulus when it is applied, via shape-shifting, a seamless integration of sensing and actuation functions is achieved within one single piece of material...
February 9, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28177217/postsynthetic-tuning-of-metal-organic-frameworks-for-targeted-applications
#18
Timur Islamoglu, Subhadip Goswami, Zhanyong Li, Ashlee J Howarth, Omar K Farha, Joseph T Hupp
Metal-organic frameworks (MOFs) are periodic, hybrid, atomically well-defined porous materials that typically form by self-assembly and consist of inorganic nodes (metal ions or clusters) and multitopic organic linkers. MOFs as a whole offer many intriguing properties, including ultrahigh porosity, tunable chemical functionality, and low density. These properties point to numerous potential applications, including gas storage, chemical separations, catalysis, light harvesting, and chemical sensing, to name a few...
February 8, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28177216/bacterioferritin-structure-dynamics-and-protein-protein-interactions-at-play-in-iron-storage-and-mobilization
#19
Mario Rivera
Despite its essentiality to life, iron presents significant challenges to cells: the exceedingly low solubility of Fe(3+) limits its bioavailability, and the reactivity of Fe(2+) toward H2O2 is a source of the toxic hydroxyl radical (HO(•)). Consequently, cellular levels of free iron are highly regulated to ensure sufficiency while preventing iron-induced toxicity. Relatively little is known about the fate of iron in the bacterial cytosol or how cells balance the need for relatively high cytosolic iron concentrations with the potential toxicity of the nutrient...
February 8, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/28170227/analyte-responsive-hydrogels-intelligent-materials-for-biosensing-and-drug-delivery
#20
Heidi R Culver, John R Clegg, Nicholas A Peppas
Nature has mastered the art of molecular recognition. For example, using synergistic non-covalent interactions, proteins can distinguish between molecules and bind a partner with incredible affinity and specificity. Scientists have developed, and continue to develop, techniques to investigate and better understand molecular recognition. As a consequence, analyte-responsive hydrogels that mimic these recognitive processes have emerged as a class of intelligent materials. These materials are unique not only in the type of analyte to which they respond but also in how molecular recognition is achieved and how the hydrogel responds to the analyte...
February 7, 2017: Accounts of Chemical Research
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