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Accounts of Chemical Research

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https://www.readbyqxmd.com/read/27809479/designing-micro-and-nanoswimmers-for-specific-applications
#1
Jaideep Katuri, Xing Ma, Morgan M Stanton, Samuel Sánchez
Self-propelled colloids have emerged as a new class of active matter over the past decade. These are micrometer sized colloidal objects that transduce free energy from their surroundings and convert it to directed motion. The self-propelled colloids are in many ways, the synthetic analogues of biological self-propelled units such as algae or bacteria. Although they are propelled by very different mechanisms, biological swimmers are typically powered by flagellar motion and synthetic swimmers are driven by local chemical reactions, they share a number of common features with respect to swimming behavior...
November 3, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27797480/cyclobutenes-at-a-crossroad-between-diastereoselective-syntheses-of-dienes-and-unique-palladium-catalyzed-asymmetric-allylic-substitutions
#2
Antonio Misale, Supaporn Niyomchon, Nuno Maulide
The rich chemistry of cyclobutanes is underpinned by a large body of synthetic literature devoted to their synthesis and decoration. This is motivated by the widespread representation of cyclobutane moieties in biologically active natural products and man-made molecules. Surprisingly, this vast array of knowledge finds no parallel in the chemistry of cyclobutenes, their unsaturated analogues. In particular, a dearth of methods to synthesize enantioenriched cyclobutenes is apparent upon cursory investigation of the literature...
October 31, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27786462/advanced-electrochemistry-of-individual-metal-clusters-electrodeposited-atom-by-atom-to-nanometer-by-nanometer
#3
Jiyeon Kim, Jeffrey E Dick, Allen J Bard
Metal clusters are very important as building blocks for nanoparticles (NPs) for electrocatalysis and electroanalysis in both fundamental and applied electrochemistry. Attention has been given to understanding of traditional nucleation and growth of metal clusters and to their catalytic activities for various electrochemical applications in energy harvesting as well as analytical sensing. Importantly, understanding the properties of these clusters, primarily the relationship between catalysis and morphology, is required to optimize catalytic function...
October 27, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27786461/painting-with-rainbows-patterning-light-in-space-time-and-wavelength-for-multiphoton-optogenetic-sensing-and-control
#4
Daan Brinks, Yoav Adam, Simon Kheifets, Adam E Cohen
Photons are a fascinating reagent, flowing and reacting quite differently compared to more massive and less ephemeral particles of matter. The optogenetic palette comprises an ever growing set of light-responsive proteins, which open the possibility of using light to perturb and to measure biological processes with great precision in space and time. Yet there are limits on what light can achieve. Diffraction limits the smallest features, and scattering in tissue limits the largest. Photobleaching, diffusion of photogenerated products, and optical crosstalk between overlapping absorption spectra further muddy the optogenetic picture, particularly when one wants to use multiple optogenetic tools simultaneously...
October 27, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27783504/the-remarkable-character-of-porphobilinogen-synthase
#5
Eileen K Jaffe
Porphobilinogen synthase (PBGS), also known as 5-aminolevulinate dehydratase, is an essential enzyme in the biosynthesis of all tetrapyrroles, which function in respiration, photosynthesis, and methanogenesis. Throughout evolution, PBGS adapted to a diversity of cellular niches and evolved to use an unusual variety of metal ions both for catalytic function and to control protein multimerization. With regard to the active site, some PBGSs require Zn(2+); a subset of those, including human PBGS, contain a constellation of cysteine residues that acts as a sink for the environmental toxin Pb(2+)...
October 26, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27783502/conjugated-polymer-zwitterions-efficient-interlayer-materials-in-organic-electronics
#6
Yao Liu, Volodimyr V Duzhko, Zachariah A Page, Todd Emrick, Thomas P Russell
Conjugated polymer zwitterions (CPZs) are neutral, hydrophilic, polymer semiconductors. The pendent zwitterions, viewed as side chain dipoles, impart solubility in polar solvents for solution processing, and open opportunities as interfacial components of optoelectronic devices, for example, between metal electrodes and organic semiconductor active layers. Such interlayers are crucial for defining the performance of organic electronic devices, e.g., field-effect transistors (OFETs), light-emitting diodes (OLEDs), and photovoltaics (OPVs), all of which consist of multilayer structures...
October 26, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27779846/hybrid-light-matter-states-in-a-molecular-and-material-science-perspective
#7
Thomas W Ebbesen
The notion that light and matter states can be hybridized the way s and p orbitals are mixed is a concept that is not familiar to most chemists and material scientists. Yet it has much potential for molecular and material sciences that is just beginning to be explored. For instance, it has already been demonstrated that the rate and yield of chemical reactions can be modified and that the conductivity of organic semiconductors and nonradiative energy transfer can be enhanced through the hybridization of electronic transitions...
October 25, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27779406/multilevel-investigation-of-charge-transport-in-conjugated-polymers
#8
Huanli Dong, Wenping Hu
Conjugated polymers have attracted the world's attentions since their discovery due to their great promise for optoelectronic devices. However, the fundamental understanding of charge transport in conjugated polymers remains far from clear. The origin of this challenge is the natural disorder of polymers with complex molecular structures in the solid state. Moreover, an effective way to examine the intrinsic properties of conjugated polymers is absent. Optoelectronic devices are always based on spin-coated films...
October 25, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27797179/free-electrons-to-molecular-bonds-and-back-closing-the-energetic-oxygen-reduction-orr-oxygen-evolution-oer-cycle-using-core-shell-nanoelectrocatalysts
#9
Peter Strasser
Nanomaterial science and electrocatalytic science have entered a successful "nanoelectrochemical" symbiosis, in which novel nanomaterials offer new frontiers for studies on electrocatalytic charge transfer, while electrocatalytic processes give meaning and often practical importance to novel nanomaterial concepts. Examples of this fruitful symbiosis are dealloyed core-shell nanoparticle electrocatalysts, which often exhibit enhanced kinetic charge transfer rates at greatly improved atom-efficiency. As such, they represent ideal electrocatalyst architectures for the acidic oxygen reduction reaction to water (ORR) and the acidic oxygen evolution reaction from water (OER) that require scarce Pt- and Ir-based catalysts...
October 24, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27797176/spin-dependent-transport-through-chiral-molecules-studied-by-spin-dependent-electrochemistry
#10
Prakash Chandra Mondal, Claudio Fontanesi, David H Waldeck, Ron Naaman
Molecular spintronics (spin + electronics), which aims to exploit both the spin degree of freedom and the electron charge in molecular devices, has recently received massive attention. Our recent experiments on molecular spintronics employ chiral molecules which have the unexpected property of acting as spin filters, by way of an effect we call "chiral-induced spin selectivity" (CISS). In this Account, we discuss new types of spin-dependent electrochemistry measurements and their use to probe the spin-dependent charge transport properties of nonmagnetic chiral conductive polymers and biomolecules, such as oligopeptides, L/D cysteine, cytochrome c, bacteriorhodopsin (bR), and oligopeptide-CdSe nanoparticles (NPs) hybrid structures...
October 24, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27797171/the-discovery-of-rolling-circle-amplification-and-rolling-circle-transcription
#11
Michael G Mohsen, Eric T Kool
Nucleic acid amplification is a hugely important technology for biology and medicine. While the polymerase chain reaction (PCR) has been highly useful and effective, its reliance on heating and cooling cycles places some constraints on its utility. For example, the heating step of PCR can destroy biological molecules under investigation and heat/cool cycles are not applicable in living systems. Thus, isothermal approaches to DNA and RNA amplification are under widespread study. Perhaps the simplest of these are the rolling circle approaches, including rolling circle amplification (RCA) and rolling circle transcription (RCT)...
October 24, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27768294/understanding-the-magnetic-anisotropy-toward-single-ion-magnets
#12
Yin-Shan Meng, Shang-Da Jiang, Bing-Wu Wang, Song Gao
Single-molecule magnets (SMMs) can retain their magnetization status preferentially after removal of the magnetic field below a certain temperature. The unique property, magnetic bistable status, enables the molecule-scale SMM to become the next-generation high-density information storage medium. SMMs' new applications are also involved in high-speed quantum computation and molecular spintronics. The development of coordination chemistry, especially in transition metal (3d) and lanthanide (4f) complexes, diversifies SMMs by introducing new ones...
October 21, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27759390/mimicking-photosynthesis-with-electrode-supported-lipid-nanoassemblies
#13
Mingming Wang, Wei Zhan
The grand scale, ultimate efficiency, and sustainability of natural photosynthesis have inspired generations of researchers in biomimetic light energy utilization. As an essential and ubiquitous component in all photosynthetic machinery, lipids and their assemblies have long been recognized as powerful molecular scaffolds in building artificial photosynthetic systems. Model lipid bilayers, such as black lipid membranes and liposomes (vesicles), have been extensively used to host natural as well as synthetic photo- and redox-active species, thereby enabling key photosynthetic processes, such as energy transfer and photoinduced electron transfer, to be examined in well-defined, natural-like membrane settings...
October 19, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27754668/predicting-molecular-crystal-properties-from-first-principles-finite-temperature-thermochemistry-to-nmr-crystallography
#14
Gregory J O Beran, Joshua D Hartman, Yonaton N Heit
Molecular crystals occur widely in pharmaceuticals, foods, explosives, organic semiconductors, and many other applications. Thanks to substantial progress in electronic structure modeling of molecular crystals, attention is now shifting from basic crystal structure prediction and lattice energy modeling toward the accurate prediction of experimentally observable properties at finite temperatures and pressures. This Account discusses how fragment-based electronic structure methods can be used to model a variety of experimentally relevant molecular crystal properties...
October 18, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27753496/multicomponent-hetero-4-2-cycloaddition-allylboration-reaction-from-natural-product-synthesis-to-drug-discovery
#15
Dennis G Hall, Taras Rybak, Tristan Verdelet
Multicomponent reactions (MCR), transformations employing three or more simple substrates in a single and highly atom-economical operation, are very attractive in both natural product synthesis and diversity-oriented synthesis of druglike molecules. Several popular multicomponent reactions were designed by combining two well-established individual reactions that utilize mutually compatible substrates. In this regard, it is not surprising that the merging of two reactions deemed as workhorses of stereoselective synthesis, the Diels-Alder cycloaddition and carbonyl allylboration, would produce a powerful and highly versatile tandem MCR process...
October 18, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27753477/from-fullerene-polymer-to-all-polymer-solar-cells-the-importance-of-molecular-packing-orientation-and-morphology-control
#16
Hyunbum Kang, Wonho Lee, Jiho Oh, Taesu Kim, Changyeon Lee, Bumjoon J Kim
All-polymer solar cells (all-PSCs), consisting of conjugated polymers as both electron donor (PD) and acceptor (PA), have recently attracted great attention. Remarkable progress has been achieved during the past few years, with power conversion efficiencies (PCEs) now approaching 8%. In this Account, we first discuss the major advantages of all-PSCs over fullerene-polymer solar cells (fullerene-PSCs): (i) high light absorption and chemical tunability of PA, which affords simultaneous enhancement of both the short-circuit current density (JSC) and the open-circuit voltage (VOC), and (ii) superior long-term stability (in particular, thermal and mechanical stability) of all-PSCs due to entangled long PA chains...
October 18, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27749047/stimulus-responsive-prochelators-for-manipulating-cellular-metals
#17
Qin Wang, Katherine J Franz
Metal ions are essential for a wide range of physiological processes, but they can also be toxic if not appropriately regulated by a complex network of metal trafficking proteins. Intervention in cellular metal distribution with small-molecule or peptide chelating agents has promising therapeutic potential to harness metals to fight disease. Molecular outcomes associated with forming metal-chelate interactions in situ include altering the concentration and subcellular metal distribution, inhibiting metalloenzymes, enhancing the reactivity of a metal species to elicit a favorable biological response, or passivating the reactivity of a metal species to prevent deleterious reactivity...
October 17, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27748122/electrocatalysis-by-mass-selected-ptn-clusters
#18
Alexander von Weber, Scott L Anderson
Mass-selected Ptn(+) ion deposition in ultrahigh vacuum (UHV) was used to prepare a series of size-selected electrodes with Ptn (n ≤ 14) clusters supported on either glassy carbon (GC) or indium tin oxide (ITO). After characterization of the physical properties of the electrodes in UHV, an in situ method was used to study electrocatalytic activity for the oxygen reduction and ethanol oxidation reactions, without significant air exposure. For each reaction studied, there are similarities between the catalytic properties of Ptn-containing electrodes and those of nanoparticulate or bulk Pt electrodes, but there are also important differences that provide mechanistic insights...
October 17, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27739689/palladium-ii-catalyzed-oxidative-difunctionalization-of-alkenes-bond-forming-at-a-high-valent-palladium-center
#19
Guoyin Yin, Xin Mu, Guosheng Liu
Difunctionalization of alkenes to incorporate two functional groups across a double bond has emerged as a powerful transformation to greatly increase molecular complexity in organic synthesis with improved efficiency. Historically, palladium-catalyzed difunctionalization of alkenes has suffered from difficulties with introducing a second functional group through reductive elimination of a Pd(II) intermediate and competing β-hydride elimination reactions. To overcome these challenges, one strategy involves utilizing a steric bulky ligand to promote the reductive elimination steps from the Pd(II) center and impeding the β-hydride elimination reactions, which are beyond the scope of this Account...
October 14, 2016: Accounts of Chemical Research
https://www.readbyqxmd.com/read/27739662/structure-design-and-performance-tuning-of-nanomaterials-for-electrochemical-energy-conversion-and-storage
#20
Tian Sheng, Yue-Feng Xu, Yan-Xia Jiang, Ling Huang, Na Tian, Zhi-You Zhou, Ian Broadwell, Shi-Gang Sun
The performance of nanomaterials in electrochemical energy conversion (fuel cells) and storage (secondary batteries) strongly depends on the nature of their surfaces. Designing the structure of electrode materials is the key approach to achieving better performance. Metal or metal oxide nanocrystals (NCs) with high-energy surfaces and open surface structures have attained significant attention in the past decade since such features possess intrinsically exceptional properties. However, they are thermodynamically metastable, resulting in a huge challenge in their shape-controlled synthesis...
October 14, 2016: Accounts of Chemical Research
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