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Accounts of Chemical Research

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https://www.readbyqxmd.com/read/29327921/the-nature-and-reactivity-of-ferryl-heme-in-compounds-i-and-ii
#1
Peter C E Moody, Emma L Raven
Aerobic organisms have evolved to activate oxygen from the atmosphere, which allows them to catalyze the oxidation of different kinds of substrates. This activation of oxygen is achieved by a metal center (usually iron or copper) buried within a metalloprotein. In the case of iron-containing heme enzymes, the activation of oxygen is achieved by formation of transient iron-oxo (ferryl) intermediates; these intermediates are called Compound I and Compound II. The Compound I and II intermediates were first discovered in the 1930s in horseradish peroxidase, and it is now known that these same species are used across the family of heme enzymes, which include all of the peroxidases, the heme catalases, the P450s, cytochrome c oxidase, and NO synthase...
January 12, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29327579/can-multielectron-intercalation-reactions-be-the-basis-of-next-generation-batteries
#2
M Stanley Whittingham, Carrie Siu, Jia Ding
Intercalation compounds form the basis of essentially all lithium rechargeable batteries. They exhibit a wide range of electronic and crystallographic structures. The former varies from metallic conductors to excellent insulators. The latter often have layer structures or have open tunnel structures that can act as the hosts for the intercalation of a wide range of metal cation and other guest species. They are fascinating materials with almost infinitely variable properties, with the crystal structure controlling the identity and the amount of the guest species that may be intercalated and subsequently removed...
January 12, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29313671/cluster-formation-in-the-superconducting-complex-intermetallic-compound-be21pt5
#3
Alfred Amon, Alim Ormeci, Matej Bobnar, Lev G Akselrud, Maxim Avdeev, Roman Gumeniuk, Ulrich Burkhardt, Yurii Prots, Christoph Hennig, Andreas Leithe-Jasper, Yuri Grin
Materials with the crystal structure of γ-brass type (Cu5Zn8 type) are typical representatives of intermetallic compounds. From the electronic point of view, they are often interpreted using the valence electron concentration approach of Hume-Rothery, developed previously for transition metals. The γ-brass-type phases of the main-group elements are rather rare. The intermetallic compound Be21Pt5, a new member of this family, was synthesized, and its crystal structure, chemical bonding, and physical properties were characterized...
January 9, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29313668/high-thermoelectric-performance-of-in4se3-based-materials-and-the-influencing-factors
#4
Xin Yin, Jing-Yuan Liu, Ling Chen, Li-Ming Wu
Materials that can directly convert electricity into heat, i.e., thermoelectric materials, have attracted renewed attention globally for sustainable energy applications. As one of the state-of-the-art thermoelectric materials, In4Se3 features an interesting crystal structure of quasi-two-dimensional sheets comprising In/Se chains that provide a platform to achieve a Peierls distortion and support a charge density wave instability. Single-crystal In4Se3-δ (δ = 0.65) shows strong anisotropy in its thermoelectric properties with a very high ZT of 1...
January 9, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29309118/proton-coupled-electron-transfer-in-artificial-photosynthetic-systems
#5
S Jimena Mora, Emmanuel Odella, Gary F Moore, Devens Gust, Thomas A Moore, Ana L Moore
Artificial photosynthetic constructs can in principle operate more efficiently than natural photosynthesis because they can be rationally designed to optimize solar energy conversion for meeting human demands rather than the multiple needs of an organism competing for growth and reproduction in a complex ecosystem. The artificial photosynthetic constructs described in this Account consist primarily of covalently linked synthetic chromophores, electron donors and acceptors, and proton donors and acceptors that carry out the light absorption, electron transfer, and proton-coupled electron transfer (PCET) processes characteristic of photosynthetic cells...
January 8, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29308876/organometallic-ruthenium-nanoparticles-synthesis-surface-chemistry-and-insights-into-ligand-coordination
#6
Luis M Martínez-Prieto, Bruno Chaudret
Although there has been for the past 20 years great interest in the synthesis and use of metal nanoparticles, little attention has been paid to the complexity of the surface of these species. In particular, the different aspects concerning the ligands present, their location, their mode of binding, and their dynamics have been little studied. Our group has started in the early 1990s an investigation of the surface coordination chemistry of ruthenium and platinum nanoparticles but at that time with a lack of adequate techniques to fulfill our ambition...
January 8, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29308653/ambiphilic-molecules-from-organometallic-curiosity-to-metal-free-catalysts
#7
Frédéric-Georges Fontaine, Étienne Rochette
Ambiphilic molecules were first used as functional ligands for transition elements, which could enable intriguing organometallic transformations. In the past decade, these intramolecular Lewis pairs, first considered organometallic curiosities, have become staples in organometallic chemistry and catalysis, acting as Z ligands, activating inert molecules using the concept of frustrated Lewis pair (FLP) chemistry, and acting as metal-free catalysts. In this Account, we detail our contribution to this blossoming field of research, focusing on the use of ambiphilic molecules as metal-free catalysts for CO2 reduction and C-H borylation reactions...
January 8, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29303552/correlating-itinerant-magnetism-in-rco2pn2-pnictides-r-la-ce-pr-nd-eu-ca-pn-p-as-to-their-crystal-and-electronic-structures
#8
Xiaoyan Tan, Zachary P Tener, Michael Shatruk
Rare-earth cobalt pnictides, RCo2Pn2 (Pn = P, As), belong to the ThCr2Si2 structure type, which is ubiquitous among intermetallic compounds. The structural and magnetic properties of simple ternary RCo2P2 phosphides, which combine partially delocalized (itinerant) 3d magnetic moments of cobalt and localized 4f magnetic moments of lanthanides, were investigated extensively in 1980-1990s, predominantly by the Jeitschko group. Those studies established that LaCo2P2 shows ferromagnetic (FM) ordering of Co moments, while the other members of the series, with R = Ce, Pr, Nd, or Sm, exhibit antiferromagnetic (AFM) ordering in both R and Co magnetic sublattices...
January 5, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29297680/gold-i-catalyzed-glycosylation-with-glycosyl-o-alkynylbenzoates-as-donors
#9
Biao Yu
Naturally occurring glycans and glycoconjugates have extremely diverse structures and biological functions. Syntheses of these molecules and their artificial mimics, which have attracted the interest of those developing new therapeutic agents, rely on glycosylation methodologies to construct the various glycosidic linkages. In this regard, a wide array of glycosylation methods have been developed, and they mainly involve the substitution of a leaving group on the anomeric carbon of a glycosyl donor with an acceptor (a nucleophile) under the action of a particular promoter (usually a stoichiometric electrophile)...
January 3, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29297671/kinetic-isotope-effect-determination-probes-the-spin-of-the-transition-state-its-stereochemistry-and-its-ligand-sphere-in-hydrogen-abstraction-reactions-of-oxoiron-iv-complexes
#10
Debasish Mandal, Dibyendu Mallick, Sason Shaik
This Account outlines interplay of theory and experiment in the quest to identify the reactive-spin-state in chemical reactions that possess a few spin-dependent routes. Metalloenzymes and synthetic models have forged in recent decades an area of increasing appeal, in which oxometal species bring about functionalization of hydrocarbons under mild conditions and via intriguing mechanisms that provide a glimpse of Nature's designs to harness these reactions. Prominent among these are oxoiron(IV) complexes, which are potent H-abstractors...
January 3, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29297669/in-situ-real-time-mechanical-and-morphological-characterization-of-electrodes-for-electrochemical-energy-storage-and-conversion-by-electrochemical-quartz-crystal-microbalance-with-dissipation-monitoring
#11
Netanel Shpigel, Mikhael D Levi, Sergey Sigalov, Leonid Daikhin, Doron Aurbach
Quartz crystal microbalance with dissipation monitoring (QCM-D) generates surface-acoustic waves in quartz crystal plates that can effectively probe the structure of films, particulate composite electrodes of complex geometry rigidly attached to quartz crystal surface on one side and contacting a gas or liquid phase on the other side. The output QCM-D characteristics consist of the resonance frequency (MHz frequency range) and resonance bandwidth measured with extra-ordinary precision of a few tenths of Hz...
January 3, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29293316/nanoscale-protection-layers-to-mitigate-degradation-in-high-energy-electrochemical-energy-storage-systems
#12
Chuan-Fu Lin, Yue Qi, Keith Gregorczyk, Sang Bok Lee, Gary W Rubloff
In the pursuit of energy storage devices with higher energy and power, new ion storage materials and high-voltage battery chemistries are of paramount importance. However, they invite-and often enhance-degradation mechanisms, which are reflected in capacity loss with charge/discharge cycling and sometimes in safety problems. Degradation mechanisms are often driven by fundamentals such as chemical and electrochemical reactions at electrode-electrolyte interfaces, volume expansion and stress associated with ion insertion and extraction, and profound inhomogeneity of electrochemical behavior...
January 2, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29292988/correction-to-postsynthetic-tuning-of-metal-organic-frameworks-for-targeted-applications
#13
Timur Islamoglu, Subhadip Goswami, Zhanyong Li, Ashlee J Howarth, Omar K Farha, Joseph T Hupp
No abstract text is available yet for this article.
January 2, 2018: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29286636/topology-of-intermetallic-structures-from-statistics-to-rational-design
#14
Tatiana G Akhmetshina, Vladislav A Blatov, Davide M Proserpio, Alexander P Shevchenko
More than 38 000 substances made only of metal atoms are collected in modern structural databases; we may call them intermetallic compounds. They have important industrial applications, and yet they are terra incognita for most of our undergraduate students. Their structural complexity and synthesis are not easily adaptable to first years laboratories, keeping them away from the standard curricula. They have been described over the years following alternative and complementary views such as coordination polyhedra, atomic layers, and polyatomic clusters...
December 29, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29281244/high-density-lipoprotein-nanobiologics-for-precision-medicine
#15
Willem J M Mulder, Mandy M T van Leent, Marnix Lameijer, Edward A Fisher, Zahi A Fayad, Carlos Pérez-Medina
Nature is an inspirational source for biomedical engineering developments. Particularly, numerous nanotechnological approaches have been derived from biological concepts. For example, among many different biological nanosized materials, viruses have been extensively studied and utilized, while exosome research has gained much traction in the 21st century. In our body, fat is transported by lipoproteins, intriguing supramolecular nanostructures that have important roles in cell function, lipid metabolism, and disease...
December 27, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29272106/electronic-and-steric-tuning-of-a-prototypical-piano-stool-complex-rh-iii-catalysis-for-c-h-functionalization
#16
Tiffany Piou, Tomislav Rovis
The history of transition metal catalysis is heavily steeped in ligand design, clearly demonstrating the importance of this approach. The intimate relationship between metal and ligand can profoundly affect the outcome of a reaction, often impacting selectivity, physical properties, and the lifetime of a catalyst. Importantly, this metal-ligand relationship can provide near limitless opportunities for reaction discovery. Over the past several years, transition-metal-catalyzed C-H bond functionalization reactions have been established as a critical foundation in organic chemistry that provides new bond forming strategies...
December 22, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29265804/coordination-compounds-with-photochromic-ligands-ready-tunability-and-visible-light-sensitized-photochromism
#17
Chi-Chiu Ko, Vivian Wing-Wah Yam
Photochromic compounds are well-known for their promising applications in many areas. In this context, many different photochromic families have been developed. As the early study of these photochromic compounds was mainly focused on the organic system, their photochromic reactivity was mainly derived from the singlet excited state. We hypothesized that the incorporation of the photochromic ligand to the transition metal complex and coordination complex systems would not only render the triplet state of the organic photochromic system more readily accessible due to the large spin-orbit coupling of the heavy metal center but also would lead to ready extension of the excitation wavelength to less destructive longer wavelength low-energy excitation...
December 21, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29260852/targeting-the-prion-like-aggregation-of-mutant-p53-to-combat-cancer
#18
Jerson L Silva, Elio A Cino, Iaci N Soares, Vitor F Ferreira, Guilherme A P de Oliveira
Prion-like behavior of several amyloidogenic proteins has been demonstrated in recent years. Despite having functional roles in some cases, irregular aggregation can have devastating consequences. The most commonly known amyloid diseases are Alzheimer's, Parkinson's, and Transmissible Spongiform Encephalopathies (TSEs). The pathophysiology of prion-like diseases involves the structural transformation of wild-type (wt) proteins to transmissible forms that can convert healthy proteins, generating aggregates. The mutant form of tumor suppressor protein, p53, has recently been shown to exhibit prion-like properties...
December 20, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29260851/structure-property-relations-in-giant-semiconductor-nanocrystals-opportunities-in-photonics-and-electronics
#19
Fabiola Navarro-Pardo, Haiguang Zhao, Zhiming M Wang, Federico Rosei
Semiconductor nanocrystals exhibit size-tunable absorption and emission ranging from the ultraviolet (UV) to the near-infrared (NIR) spectral range, high absorption coefficient, and high photoluminescence quantum yield. Effective surface passivation of these so-called quantum dots (QDs) may be achieved by growing a shell of another semiconductor material. The resulting core/shell QDs can be considered as a model system to study and optimize structure/property relations. A special case consists in growing thick shells (1...
December 20, 2017: Accounts of Chemical Research
https://www.readbyqxmd.com/read/29260848/transition-metal-complexes-featuring-dianionic-heavy-group-14-element-aromatic-ligands
#20
Masaichi Saito
The synthesis of dilithio-stannoles and -plumboles, dianionic aromatic compounds containing tin and lead atoms in their π-skeletons, opened a new field of transition-metal chemistry. Since the discovery of ferrocene (Cp2Fe), which is composed of anionic aromatic ligands (Cp: cyclopentadienyl) and Fe(II), ferrocene-type sandwich complexes have long played important roles in many fields of chemistry. During the last few decades, the electronic and structural properties of the Cp ligand have been modified by introducing electron-donating, electron-withdrawing, and sterically encumbered substituents on the skeletal carbon atoms to obtain desirable properties of the resulting sandwich complexes...
December 20, 2017: Accounts of Chemical Research
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