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  • Size dependency of gold nanoparticles interacting with model membranes
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-17
    Claudia Contini; James W. Hindley; Thomas J. Macdonald; Joseph D. Barritt; Oscar Ces; Nick Quirke

    The rapid development of nanotechnology has led to an increase in the number and variety of engineered nanomaterials in the environment. Gold nanoparticles (AuNPs) are an example of a commonly studied nanomaterial whose highly tailorable properties have generated significant interest through a wide range of research fields. In the present work, we characterise the AuNP-lipid membrane interaction by

    更新日期:2020-09-18
  • Towards the catalytic activation of inert small molecules by main-group ambiphiles
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-16
    Rian D. Dewhurst; Marc-André Légaré; Holger Braunschweig

    The activation of very inert small molecules generally requires highly reactive activating species, but the high energy of these species makes their regeneration, and thus also catalytic turnover of the reaction, difficult to achieve. Here, the authors highlight the formidable challenge of overcoming the tradeoff between activating power and catalytic turnover in the context of main-group ambiphiles

    更新日期:2020-09-16
  • Zeolite-supported ultra-small nickel as catalyst for selective oxidation of methane to syngas
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-16
    Shuhei Yasuda; Ryota Osuga; Yusuke Kunitake; Kazuya Kato; Atsushi Fukuoka; Hirokazu Kobayashi; Min Gao; Jun-ya Hasegawa; Ryo Manabe; Hisashi Shima; Susumu Tsutsuminai; Toshiyuki Yokoi

    The development of simple catalysts with high performance in the selective oxidation of methane to syngas at low temperature has attracted much attention. Here we report a nickel-based solid catalyst for the oxidation of methane, synthesised by a facile impregnation method. Highly dispersed ultra-small NiO particles of 1.6 nm in size are successfully formed on the MOR-type zeolite. The zeolite–supported

    更新日期:2020-09-16
  • Silylium ion mediated 2+2 cycloaddition leads to 4+2 Diels-Alder reaction products
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-11
    Heng-Ding Wang; Hong-Jun Fan

    The mechanism of silver(I) and copper(I) catalyzed cycloaddition between 1,2-diazines and siloxy alkynes remains controversial. Here we explore the mechanism of this reaction with density functional theory. Our calculations show that the reaction takes place through a metal (Ag+, Cu+) catalyzed [2+2] cycloaddition pathway and the migration of a silylium ion [triisopropylsilyl ion (TIPS+)] further controls

    更新日期:2020-09-11
  • Unforeseen crystal forms of the natural osmolyte floridoside
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-11
    Andrew J. Maneffa; Adrian C. Whitwood; A. Steve Whitehouse; Hugh Powell; James H. Clark; Avtar S. Matharu

    Floridoside (2-α-O-D-galactopyranosyl glycerol) is a glycerol glycoside that is biosynthesised by most species of red algae and has been implicated as an intracellular regulator of various homeostatic functions. Here, we report the identification of two unforeseen crystal forms of the ubiquitous natural osmolyte floridoside including a seemingly unheralded second anhydrous conformational polymorph

    更新日期:2020-09-11
  • Navigating the DNA encoded libraries chemical space
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-11
    Alfredo Martín; Christos A. Nicolaou; Miguel A. Toledo

    DNA-encoded library (DEL) technology is a novel ligand identification strategy that allows the synthesis and screening of unprecedented chemical diversity more efficiently than conventional methods. However, no reports have been published to systematically study how to increase the diversity and improve the molecular property space that can be covered with DEL. This report describes the development

    更新日期:2020-09-11
  • Quantification of amyloid fibril polymorphism by nano-morphometry reveals the individuality of filament assembly
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-11
    Liam D. Aubrey; Ben J. F. Blakeman; Liisa Lutter; Christopher J. Serpell; Mick F. Tuite; Louise C. Serpell; Wei-Feng Xue

    Amyloid fibrils are highly polymorphic structures formed by many different proteins. They provide biological function but also abnormally accumulate in numerous human diseases. The physicochemical principles of amyloid polymorphism are not understood due to lack of structural insights at the single-fibril level. To identify and classify different fibril polymorphs and to quantify the level of heterogeneity

    更新日期:2020-09-11
  • Structure of an anti-PEG antibody reveals an open ring that captures highly flexible PEG polymers
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-08
    Justin T. Huckaby; Tim M. Jacobs; Zhongbo Li; Robert J. Perna; Anting Wang; Nathan I. Nicely; Samuel K. Lai

    Polyethylene glycol (PEG) is a polymer routinely used to modify biologics and nanoparticles to prolong blood circulation and reduce immunogenicity of the underlying therapeutic. However, several PEGylated therapeutics induce the development of anti-PEG antibodies (APA), leading to reduced efficacy and increased adverse events. Given the highly flexible structure of PEG, how APA specifically bind PEG

    更新日期:2020-09-08
  • Phosphorylation regulates the binding of intrinsically disordered proteins via a flexible conformation selection mechanism
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-07
    Na Liu; Yue Guo; Shangbo Ning; Mojie Duan

    Phosphorylation is one of the most common post-translational modifications. The phosphorylation of the kinase-inducible domain (KID), which is an intrinsically disordered protein (IDP), promotes the folding of KID and binding with the KID-interacting domain (KIX). However, the regulation mechanism of the phosphorylation on KID is still elusive. In this study, the structural ensembles and binding process

    更新日期:2020-09-08
  • Enzymatic kinetic resolution of desmethylphosphinothricin indicates that phosphinic group is a bioisostere of carboxyl group
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-02
    Daniela De Biase; Francesca Cappadocio; Eugenia Pennacchietti; Fabio Giovannercole; Antonio Coluccia; Jouko Vepsäläinen; Alex Khomutov

    Escherichia coli glutamate decarboxylase (EcGadB), a pyridoxal 5’-phosphate (PLP)-dependent enzyme, is highly specific for L-glutamate and was demonstrated to be effectively immobilised for the production of γ-aminobutyric acid (GABA), its decarboxylation product. Herein we show that EcGadB quantitatively decarboxylates the L-isomer of D,L-2-amino-4-(hydroxyphosphinyl)butyric acid (D,L-Glu-γ-PH), a

    更新日期:2020-09-02
  • Rapid optimisation of fragments and hits to lead compounds from screening of crude reaction mixtures
    Commun. Chem. (IF 4.253) Pub Date : 2020-09-02
    Lisa M. Baker; Anthony Aimon; James B. Murray; Allan E. Surgenor; Natalia Matassova; Stephen D. Roughley; Patrick M. Collins; Tobias Krojer; Frank von Delft; Roderick E. Hubbard

    Fragment based methods are now widely used to identify starting points in drug discovery and generation of tools for chemical biology. A significant challenge is optimization of these weak binding fragments to hit and lead compounds. We have developed an approach where individual reaction mixtures of analogues of hits can be evaluated without purification of the product. Here, we describe experiments

    更新日期:2020-09-02
  • Aluminum electrolytes for Al dual-ion batteries
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-28
    Kostiantyn V. Kravchyk; Maksym V. Kovalenko

    In the search for sustainable energy storage systems, aluminum dual-ion batteries have recently attracted considerable attention due to their low cost, safety, high energy density (up to 70 kWh kg−1), energy efficiency (80–90%) and long cycling life (thousands of cycles and potentially more), which are needed attributes for grid-level stationary energy storage. Overall, such batteries are composed

    更新日期:2020-08-28
  • Chiral lanthanide lumino-glass for a circularly polarized light security device
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-25
    Yuichi Kitagawa; Satoshi Wada; M. D. Jahidul Islam; Kenichiro Saita; Masayuki Gon; Koji Fushimi; Kazuo Tanaka; Satoshi Maeda; Yasuchika Hasegawa

    Artificial light plays an essential role in information technologies such as optical telecommunications, data storage, security features, and the display of information. Here, we show a chiral lanthanide lumino-glass with extra-large circularly polarized luminescence (CPL) for advanced photonic security device applications. The chiral lanthanide glass is composed of a europium complex with the chiral

    更新日期:2020-08-25
  • Sigmoidally hydrochromic molecular porous crystal with rotatable dendrons
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-17
    Hiroshi Yamagishi; Sae Nakajima; Jooyoung Yoo; Masato Okazaki; Youhei Takeda; Satoshi Minakata; Ken Albrecht; Kimihisa Yamamoto; Irene Badía-Domínguez; Maria Moreno Oliva; M. Carmen Ruiz Delgado; Yuka Ikemoto; Hiroyasu Sato; Kenta Imoto; Kosuke Nakagawa; Hiroko Tokoro; Shin-ichi Ohkoshi; Yohei Yamamoto

    Vapochromic behaviour of porous crystals is beneficial for facile and rapid detection of gaseous molecules without electricity. Toward this end, tailored molecular designs have been established for metal–organic, covalent-bonded and hydrogen-bonded frameworks. Here, we explore the hydrochromic chemistry of a van der Waals (VDW) porous crystal. The VDW porous crystal VPC-1 is formed from a novel aromatic

    更新日期:2020-08-17
  • Coagulation using organic carbonates opens up a sustainable route towards regenerated cellulose films
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-13
    Mai N. Nguyen; Udo Kragl; Ingo Barke; Regina Lange; Henrik Lund; Marcus Frank; Armin Springer; Victoria Aladin; Björn Corzilius; Dirk Hollmann

    Due to their biodegradability, biocompatibility and sustainable nature, regenerated cellulose (RC) films are of enormous relevance for green applications including medicinal, environmental and separation technologies. However, the processes used so far are very hazardous to the environment and health. Here, we disclose a simple, fast, environmentally friendly, nontoxic and cost-effective processing

    更新日期:2020-08-14
  • Visualization and quantitation of electronic communication pathways in a series of redox-active pillar[6]arene-based macrocycles
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-13
    Mehdi Rashvand Avei; Sedigheh Etezadi; Burjor Captain; Angel E. Kaifer

    While oxidized pillar[5]arenes with 1-5 benzoquinone units are known, very few examples of oxidized pillar[6]arenes have been reported. We describe here the synthesis, characterization and electrochemical behavior of a series of macrocyclic hosts prepared by the stepwise oxidation of 1,4-diethoxypillar[6]arene, resulting in high-yield and high-purity isolation of two constitutional isomers for each

    更新日期:2020-08-14
  • Synthesis, properties, and catalysis of p-block complexes supported by bis(arylimino)acenaphthene ligands
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-12
    Jingyi Wang; Han Sen Soo; Felipe Garcia

    Bis(arylimino)acenaphthene (Ar-BIAN) ligands have been recognized as robust scaffolds for metal complexes since the 1990 s and most of their coordination chemistry was developed with transition metals. Notably, there have been relatively few reports on complexes comprising main group elements, especially those capitalizing on the redox non-innocence of Ar-BIAN ligands supporting p-block elements. Here

    更新日期:2020-08-12
  • Evidence on the formation of dimers of polycyclic aromatic hydrocarbons in a laminar diffusion flame
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-11
    Alessandro Faccinetto; Cornelia Irimiea; Patrizia Minutolo; Mario Commodo; Andrea D’Anna; Nicolas Nuns; Yvain Carpentier; Claire Pirim; Pascale Desgroux; Cristian Focsa; Xavier Mercier

    The role of polycyclic aromatic hydrocarbons (PAHs) in the formation of nascent soot particles in flames is well established and yet the detailed mechanisms are still not fully understood. Here we provide experimental evidence of the occurrence of dimerization of PAHs in the gas phase before soot formation in a laminar diffusion methane flame, supporting the hypothesis of stabilization of dimers through

    更新日期:2020-08-11
  • Optical and theoretical study of strand recognition by nucleic acid probes
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-11
    Ivana Domljanovic; Maria Taskova; Pâmella Miranda; Gerald Weber; Kira Astakhova

    Detection of nucleic acids is crucial to the study of their basic properties and consequently to applying this knowledge to the determination of pathologies such as cancer. In this work, our goal is to determine new trends for creating diagnostic tools for cancer driver mutations. Herein, we study a library of natural and modified oligonucleotide duplexes by a combination of optical and theoretical

    更新日期:2020-08-11
  • Open questions on nonequilibrium thermodynamics of chemical reaction networks
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Massimiliano Esposito

    Chemical reaction networks (CRNs) are prototypical complex systems because reactions are nonlinear and connected in intricate ways, and they are also essential to understand living systems. Here, the author discusses how recent developments in nonequilibrium thermodynamics provide new insight on how CRNs process energy and perform sophisticated tasks, and describes open challenges in the field.

    更新日期:2020-08-08
  • Open questions in chemistry
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07

    Today, Communications Chemistry launches a series of Comment articles discussing key open questions in specific fields of fundamental chemical research. Here we outline the aims of this series and highlight each contribution within.

    更新日期:2020-08-08
  • Open questions in transplutonium coordination chemistry
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Korey P. Carter; Roger M. Pallares; Rebecca J. Abergel

    Over the past decade, momentous progress has been made in the characterization of late actinide compounds. Here the authors highlight how advances in spectroscopic and computational tools have developed our understanding of fundamental transplutonium bonding interactions, and discuss whether covalency and heterogeneity changes in 5f-orbital bonding could be harnessed in environmentally and industrially

    更新日期:2020-08-08
  • Mapping protein glycosylation through oxocarbenium ion generation
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Andrew J. Bissette

    Mass spectrometry allows the pattern of glycosylation in proteins to be mapped, but can be limited by the lability of glycosidic bonds. Now, a method exploiting this lability allows for direct mapping of glycan moieties in glycoproteins.

    更新日期:2020-08-08
  • Spontaneous void formation in antimony alloy anodes
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Teresa S. Ortner

    Lithium-ion batteries suffer from stability issues. Now, spontaneously formed, stable voids in antimony alloy anodes offer a simple remedy.

    更新日期:2020-08-08
  • Open questions on the structures of crystalline water ices
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Thomas Loerting; Violeta Fuentes-Landete; Christina M. Tonauer; Tobias M. Gasser

    Water can form a vast number of topological frameworks owing to its hydrogen-bonding ability, with 19 different forms of ice experimentally confirmed at present. Here, the authors comment on open questions and possible future discoveries, covering negative to ultrahigh pressures.

    更新日期:2020-08-08
  • Open questions in chemical glycobiology
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Mia I. Zol-Hanlon; Benjamin Schumann

    Glycans are ubiquitous in biology, but their complex structure and biosynthesis have challenged research of their wide-ranging roles. Here, the authors comment on current trends on the role of chemical methodologies in the field of glycobiology. Glycans are ubiquitous in biology, but their complex structure and biosynthesis have challenged research of their wide-ranging roles. Here, the authors comment

    更新日期:2020-08-08
  • Open questions on the chemical composition of airborne particles
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Barbara J. Finlayson-Pitts; Lisa M. Wingen; Véronique Perraud; Michael J. Ezell

    Airborne particles have significant impacts on health, visibility, and climate. Here, an overview of what is known about particle chemical composition is presented, along with open questions and challenges that are central to relating composition to life cycles and impacts.

    更新日期:2020-08-08
  • Open questions on the physical properties of aerosols
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Bryan R. Bzdek; Jonathan P. Reid; Michael I. Cotterell

    Aerosols are highly dynamic, non-equilibrium systems exhibiting unique microphysical properties relative to bulk systems. Here the authors discuss the roles aerosols play in (bio)chemical transformations and identify open questions in aerosol-mediated reaction rate accelerations, aerosol optical properties, and microorganism survival. Aerosols are highly dynamic, non-equilibrium systems exhibiting

    更新日期:2020-08-08
  • Open questions on atmospheric nanoparticle growth
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Taina Yli-Juuti; Claudia Mohr; Ilona Riipinen

    Cloud droplets form in the atmosphere on aerosol particles, many of which result from nucleation of vapors. Here the authors comment on current knowledge and open questions regarding the condensational growth of nucleated particles to sizes where they influence cloud formation.

    更新日期:2020-08-08
  • Open questions on the biological roles of first-row transition metals
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Debbie C. Crans; Kateryna Kostenkova

    First-row transition metals play several roles in biological processes and in medicine, but can be toxic in high concentrations. Here the authors comment on the sensitive biochemistry and speciation chemistry of the first-row transition metals, and outline some of the remaining questions that have yet to be answered. First-row transition metals play several roles in biological processes and in medicine

    更新日期:2020-08-08
  • Secondary extended mannan side chains and attachment of the arabinan in mycobacterial lipoarabinomannan
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Shiva K. Angala; Wei Li; Claudia M. Boot; Mary Jackson; Michael R. McNeil

    Mycobacterial lipoarabinomannan (LAM) is in an essential cell envelope lipopolysaccharide anchored both to the plasma and outer membranes. To understand critical biological questions such as the biosynthesis, spatial organization of LAM within the cell envelope, structural remodeling during growth, and display or lack of display of LAM-based antigenicity requires a basic understanding of the primary

    更新日期:2020-08-08
  • Quantifying the thermodynamics of protein unfolding using 2D NMR spectroscopy
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-07
    Rita Puglisi; Oliver Brylski; Caterina Alfano; Stephen R. Martin; Annalisa Pastore; Piero A. Temussi

    A topic that has attracted considerable interest in recent years is the possibility to perform thermodynamic studies of proteins directly in-cell or in complex environments which mimic the cellular interior. Nuclear magnetic resonance (NMR) could be an attractive technique for these studies but its applicability has so far been limited by technical issues. Here, we demonstrate that 2D NMR methods can

    更新日期:2020-08-08
  • Bulk and local structures of metal–organic frameworks unravelled by high-resolution electron microscopy
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-06
    Lingmei Liu; Daliang Zhang; Yihan Zhu; Yu Han

    The periodic bulk structures of metal–organic frameworks (MOFs) can be solved by diffraction-based techniques; however, their non-periodic local structures—such as crystal surfaces, grain boundaries, defects, and guest molecules—have long been elusive due to a lack of suitable characterization tools. Recent advances in (scanning) transmission electron microscopy ((S)TEM) has made it possible to probe

    更新日期:2020-08-06
  • Photocatalytic radical defluoroalkylation of unactivated alkenes via distal heteroaryl ipso -migration
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-04
    Xin Yuan; Kai-Qiang Zhuang; Yu-Sheng Cui; Long-Zhou Qin; Qi Sun; Xiu Duan; Lin Chen; Ning Zhu; Guigen Li; Jiang-Kai Qiu; Kai Guo

    Currently, the selective activation of C(sp3)–F bonds and C–C bonds constitute one of the most widely used procedures for the synthesis of high-value products that range from pharmaceuticals to agrochemical applications. While numerous examples of these two methods have been reported in their respective fields, the processes which merge the activation of both single C(sp3)-F bonds and C–C bonds in

    更新日期:2020-08-04
  • Programmed folding into spiro -multicyclic polymer topologies from linear and star-shaped chains
    Commun. Chem. (IF 4.253) Pub Date : 2020-08-04
    Yoshinobu Mato; Kohei Honda; Brian J. Ree; Kenji Tajima; Takuya Yamamoto; Tetsuo Deguchi; Takuya Isono; Toshifumi Satoh

    The development of precise folding techniques for synthetic polymer chains that replicate the unique structures and functions of biopolymers has long been a key challenge. In particular, spiro-type (i.e., 8-, trefoil-, and quatrefoil-shaped) polymer topologies remain challenging due to their inherent structural complexity. Herein, we establish a folding strategy to produce spiro-type multicyclic polymers

    更新日期:2020-08-04
  • Intramolecular crossover from unconventional diamagnetism to paramagnetism of palladium ions probed by soft X-ray magnetic circular dichroism
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-31
    Alevtina Smekhova; Detlef Schmitz; Natalya V. Izarova; Maria Stuckart; S. Fatemeh Shams; Konrad Siemensmeyer; Frank M. F. de Groot; Paul Kögerler; Carolin Schmitz-Antoniak

    The case of palladium(II) ions in molecular polyoxopalladates highlights the importance of accounting not only for nearest neighbour atoms or ions in order to understand, model or predict magnetic characteristics. Here, using site-specific soft X-ray magnetic circular dichroism (XMCD), the effects of different bond lengths, delocalization of 4d electrons, and 4d spin-orbit coupling on the electronic

    更新日期:2020-07-31
  • Simultaneous determination of transient free radicals and reaction kinetics by high-resolution time-resolved dual-comb spectroscopy
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-30
    Pei-Ling Luo; Er-Chien Horng

    Quantitative determination of multiple transient species is critical in investigating reaction mechanisms and kinetics under various conditions. Dual-comb spectroscopy, a comb-laser-based multi-heterodyne interferometric technique that enables simultaneous achievement of broadband, high-resolution, and rapid spectral acquisition, opens a new era of time-resolved spectroscopic measurements. Employing

    更新日期:2020-07-30
  • The phenine concept delivers a nitrogen-doped nanotube and evokes infinite possibilities
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-28
    Joshua C. Walsh; Graham J. Bodwell

    Isobe et al. recently introduced the phenine concept, whereby a 1,3,5-trisubstituted benzene system (a phenine unit) is used as a basic building block instead of an sp2-hybridized carbon atom. Now, they apply it in a concise synthesis of a nitrogen-doped phenine nanotube.

    更新日期:2020-07-28
  • Equilibrium and thermodynamic studies of chromic overcrowded fluorenylidene-acridanes with modified fluorene moieties
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-24
    Ya Wang; Yue Ma; Keisuke Ogumi; Bing Wang; Takafumi Nakagawa; Yao Fu; Yutaka Matsuo

    Chromic materials, an important class of stimuli-responsive materials, have aroused extensive attention in recent years. Normally, their color is based on changes in morphology. Few examples of chromic material based on conformational isomerization, such as in overcrowded alkenes, have been reported previously. Furthemore, experimental thermodynamic studies of overcrowded bistricyclic aromatic enes

    更新日期:2020-07-24
  • Wet carbonate-promoted radical arylation of vinyl pinacolboronates with diaryliodonium salts yields substituted olefins
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-22
    Chao Wu; Chongyang Zhao; Jun Zhou; Han-Shi Hu; Jun Li; Panpan Wu; Chao Chen

    Since the landmark work of Heck, Negishi and Suzuki on Pd-catalyzed crossing coupling reactions, innovative discovery of new reactions forming C-C bonds and constructing functional olefins via nonmetal catalysts remains an imperative area in organic chemistry. Herein, we report a transition-metal-free arylation method of vinyl pinacolboronates with diaryliodonium salts to form C(sp2)-C(sp2) bond and

    更新日期:2020-07-22
  • Organophosphorus zwitterions engaged in a conjugated macrocycle on fullerene
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-21
    Yoshifumi Hashikawa; Shu Okamoto; Yasujiro Murata

    Organophosphorus zwitterions are one of the most important but elusive intermediates for carbon–carbon bond formation in synthetic chemistry and biology. However, a lack of isolated examples due to their lability has hampered in-depth understanding of structures and their reaction mechanisms. In this study, we crystallographically reveal the solid-state structure of a phosha-Michael adduct engaged

    更新日期:2020-07-21
  • Carbon dioxide adsorption in open nanospaces formed by overlap of saponite clay nanosheets
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-21
    Kiminori Sato; Michael Hunger

    Nanoscale open spaces formed by partial overlap of two-dimensional nanosheets in clays, abundantly and ubiquitously available, possess reactive molecular sites such as nanosheet edges in their interior. Here, the capture and storage of CO2 molecules in open spaces within saponite clay are explored by solid-state nuclear magnetic resonance coupled with open space analysis using positronium. CO2 physisorption

    更新日期:2020-07-21
  • p K a of the ligand water molecules in the oxygen-evolving Mn 4 CaO 5 cluster in photosystem II
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-16
    Keisuke Saito; Minesato Nakagawa; Hiroshi Ishikita

    Release of the protons from the substrate water molecules is prerequisite for O2 evolution in photosystem II (PSII). Proton-releasing water molecules with low pKa values at the catalytic moiety can be the substrate water molecules. In some studies, one of the ligand water molecules, W2, is regarded as OH−. However, the PSII crystal structure shows neither proton acceptor nor proton-transfer pathway

    更新日期:2020-07-16
  • Revealing structural evolution occurring from photo-initiated polymer network formation
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-10
    C. J. Brett; S. Montani; M. Schwartzkopf; R. A. T. M. van Benthem; J. F. G. A. Jansen; G. Griffini; S. V. Roth; M. K. G. Johansson

    Photopolymerization is a key enabling technology offering spatial and temporal control to allow for future functional materials to be made to meet societal needs. However, gaining access to robust experimental techniques to describe the evolution of nanoscale morphology in photo-initiated polymeric systems has proven so far to be a challenging task. Here, we show that these physical transformations

    更新日期:2020-07-10
  • Spontaneous redox continuum reveals sequestered technetium clusters and retarded mineral transformation of iron
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-10
    Daria Boglaienko; Jennifer A. Soltis; Ravi K. Kukkadapu; Yingge Du; Lucas E. Sweet; Vanessa E. Holfeltz; Gabriel B. Hall; Edgar C. Buck; Carlo U. Segre; Hilary P. Emerson; Yelena Katsenovich; Tatiana G. Levitskaia

    The sequestration of metal ions into the crystal structure of minerals is common in nature. To date, the incorporation of technetium(IV) into iron minerals has been studied predominantly for systems under carefully controlled anaerobic conditions. Mechanisms of the transformation of iron phases leading to incorporation of technetium(IV) under aerobic conditions remain poorly understood. Here we investigate

    更新日期:2020-07-10
  • Probing the temperature of supported platinum nanoparticles under microwave irradiation by in situ and operando XAFS
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-03
    Taishi Ano; Shuntaro Tsubaki; Anyue Liu; Masayuki Matsuhisa; Satoshi Fujii; Ken Motokura; Wang-Jae Chun; Yuji Wada

    Microwave irradiation can cause high local temperatures at supported metal nanoparticles, which can enhance reaction rates. Here we discuss the temperature of platinum nanoparticles on γ-Al2O3 and SiO2 supports under microwave irradiation using the Debye–Waller factor obtained from in situ extended X-ray absorption fine structure (EXAFS) measurements. Microwave irradiation exhibits considerably smaller

    更新日期:2020-07-03
  • The orphan nuclear receptor Nurr1 is responsive to non-steroidal anti-inflammatory drugs
    Commun. Chem. (IF 4.253) Pub Date : 2020-07-03
    Sabine Willems; Whitney Kilu; Xiaomin Ni; Apirat Chaikuad; Stefan Knapp; Jan Heering; Daniel Merk

    Nuclear receptor related 1 (Nurr1) is an orphan ligand-activated transcription factor and considered as neuroprotective transcriptional regulator with great potential as therapeutic target for neurodegenerative diseases. However, the collection of available Nurr1 modulators and mechanistic understanding of Nurr1 are limited. Here, we report the discovery of several structurally diverse non-steroidal

    更新日期:2020-07-03
  • Effect of intramolecular hydrogen-bond formation on the molecular conformation of amino acids
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-30
    Giulia Giubertoni; Oleksandr O. Sofronov; Huib J. Bakker

    The molecular conformation of the carboxyl group can be crucial for its chemical properties and intermolecular interactions, especially in complex molecular environments such as polypeptides. Here, we study the conformational behaviour of the model amino acid N-acetylproline in solution at room temperature with two-dimensional infrared spectroscopy. We find that the carboxyl group of N-acetylproline

    更新日期:2020-06-30
  • Metallically gradated silicon nanowire and palladium nanoparticle composites as robust hydrogenation catalysts
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-26
    Yoichi M. A. Yamada; Heeyoel Baek; Takuma Sato; Aiko Nakao; Yasuhiro Uozumi

    Heterogeneous catalysis of alkenes to alkanes is of great importance in chemical industry, but more efficient and reusable heterogeneous catalysts are still demanded. Here, we report a metallically gradated composite of a silicon nanowire array and palladium nanoparticles which are reused for the hydrogenation of an alkene. The catalyst promotes the hydrogenation of stilbene with atmospheric hydrogen

    更新日期:2020-06-26
  • Molecular design strategy of fluorogenic probes based on quantum chemical prediction of intramolecular spirocyclization
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-26
    Ryo Tachibana; Mako Kamiya; Satoshi Suzuki; Keiji Morokuma; Aika Nanjo; Yasuteru Urano

    Fluorogenic probes are essential tools for real-time visualization of dynamic intracellular processes in living cells, but so far, their design has been largely dependent on trial-and-error methods. Here we propose a quantum chemical calculation-based method for rational prediction of the fluorescence properties of hydroxymethyl rhodamine (HMR)-based fluorogenic probes. Our computational analysis of

    更新日期:2020-06-26
  • Dehydration entropy drives liquid-liquid phase separation by molecular crowding
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-26
    Sohee Park; Ryan Barnes; Yanxian Lin; Byoung-jin Jeon; Saeed Najafi; Kris T. Delaney; Glenn H. Fredrickson; Joan-Emma Shea; Dong Soo Hwang; Songi Han

    Complex coacervation driven liquid-liquid phase separation (LLPS) of biopolymers has been attracting attention as a novel phase in living cells. Studies of LLPS in this context are typically of proteins harboring chemical and structural complexity, leaving unclear which properties are fundamental to complex coacervation versus protein-specific. This study focuses on the role of polyethylene glycol

    更新日期:2020-06-26
  • Spatial molecular-dynamically ordered NMR spectroscopy of intact bodies and heterogeneous systems
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-26
    Kengo Ito; Yuuri Tsuboi; Jun Kikuchi

    Noninvasive evaluation of the spatial distribution of chemical composition and diffusion behavior of materials is becoming possible by advanced nuclear magnetic resonance (NMR) pulse sequence editing. However, there is room for improvement in the spectral resolution and analytical method for application to heterogeneous samples. Here, we develop applications for comprehensively evaluating compounds

    更新日期:2020-06-26
  • Direct identification of reaction sites on ferrihydrite
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-19
    Jean-François Boily; Xiaowei Song

    Hydroxyl groups are the cornerstone species driving catalytic reactions on mineral nanoparticles of Earth’s crust, water, and atmosphere. Here we directly identify populations of these groups on ferrihydrite, a key yet misunderstood iron oxyhydroxide nanomineral in natural sciences. This is achieved by resolving an enigmatic set of vibrational spectroscopic signatures of reactive hydroxo groups and

    更新日期:2020-06-19
  • Amino acid dependent formaldehyde metabolism in mammals
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-16
    Matthias Pietzke; Guillermo Burgos-Barragan; Niek Wit; Jacqueline Tait-Mulder; David Sumpton; Gillian M. Mackay; Ketan J. Patel; Alexei Vazquez

    Aldehyde dehydrogenase class 3, encoded by ADH5 in humans, catalyzes the glutathione dependent detoxification of formaldehyde. Here we show that ADH5 deficient cells turn over formaldehyde using alternative pathways starting from the reaction of formaldehyde with free amino acids. When mammalian cells are exposed to formaldehyde, the levels of the reaction products of formaldehyde with the amino acids

    更新日期:2020-06-16
  • Developing a new generation of scientist communicators through effective public outreach
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-12
    Sean M. Mackay; Eng Wui Tan; David S. Warren

    Science disengagement amongst school children remains a global challenge, leading to calls for more scientists to engage with the public. Here the authors discuss how a voluntary, flexible program can enhance graduate attributes in addition to addressing barriers to public engagement.

    更新日期:2020-06-12
  • Membrane protein mediated bilayer communication in networks of droplet interface bilayers
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-12
    Stuart Haylock; Mark S. Friddin; James W. Hindley; Enrique Rodriguez; Kalypso Charalambous; Paula J. Booth; Laura M. C. Barter; Oscar Ces

    Droplet interface bilayers (DIBs) are model membranes formed between lipid monolayer-encased water droplets in oil. Compared to conventional methods, one of the most unique properties of DIBs is that they can be connected together to generate multi-layered ‘tissue-like’ networks, however introducing communication pathways between these compartments typically relies on water-soluble pores that are unable

    更新日期:2020-06-12
  • A small-molecule inhibitor of lectin-like oxidized LDL receptor-1 acts by stabilizing an inactive receptor tetramer state
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-10
    Gisela Schnapp; Heike Neubauer; Frank H. Büttner; Sandra Handschuh; Iain Lingard; Ralf Heilker; Klaus Klinder; Jürgen Prestle; Rainer Walter; Michael Wolff; Markus Zeeb; Francois Debaene; Herbert Nar; Dennis Fiegen

    The C-type lectin family member lectin-like oxidized LDL receptor-1 (LOX-1) has been object of intensive research. Its modulation may offer a broad spectrum of therapeutic interventions ranging from cardiovascular diseases to cancer. LOX-1 mediates uptake of oxLDL by vascular cells and plays an important role in the initiation of endothelial dysfunction and its progression to atherosclerosis. So far

    更新日期:2020-06-10
  • Extended Experimental Inferential Structure Determination Method in Determining the Structural Ensembles of Disordered Protein States.
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-09
    James Lincoff,Mojtaba Haghighatlari,Mickael Krzeminski,João M C Teixeira,Gregory-Neal W Gomes,Claudiu C Gradinaru,Julie D Forman-Kay,Teresa Head-Gordon

    Proteins with intrinsic or unfolded state disorder comprise a new frontier in structural biology, requiring the characterization of diverse and dynamic structural ensembles. Here we introduce a comprehensive Bayesian framework, the Extended Experimental Inferential Structure Determination (X-EISD) method, which calculates the maximum log-likelihood of a disordered protein ensemble. X-EISD accounts

    更新日期:2020-06-09
  • Controlled hydrogenation into defective interlayer bismuth oxychloride via vacancy engineering
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-05
    Dandan Cui; Kang Xu; Xingan Dong; Dongdong Lv; Fan Dong; Weichang Hao; Yi Du; Jun Chen

    Hydrogenation is an effective approach to improve the performance of photocatalysts within defect engineering methods. The mechanism of hydrogenation and synergetic effects between hydrogen atoms and local electronic structures, however, remain unclear due to the limits of available photocatalytic systems and technical barriers to observation and measurement. Here, we utilize oxygen vacancies as residential

    更新日期:2020-06-05
  • Three-dimensional covariance-map imaging of molecular structure and dynamics on the ultrafast timescale
    Commun. Chem. (IF 4.253) Pub Date : 2020-06-05
    Jason W. L. Lee; Hansjochen Köckert; David Heathcote; Divya Popat; Richard T. Chapman; Gabriel Karras; Paulina Majchrzak; Emma Springate; Claire Vallance

    Ultrafast laser pump-probe methods allow chemical reactions to be followed in real time, and have provided unprecedented insight into fundamental aspects of chemical reactivity. While evolution of the electronic structure of the system under study is evident from changes in the observed spectral signatures, information on rearrangement of the nuclear framework is generally obtained indirectly. Disentangling

    更新日期:2020-06-05
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