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Rakesh Gupta, Imran Khan, Firasat Hussain, A Martin Bossoh, Israël M Mbomekallé, Pedro de Oliveira, Masahiro Sadakane, Chisato Kato, Katsuya Ichihashi, Katsuya Inoue, Sadafumi Nishihara
Herein we report two pentanuclear Mn(II)-substituted sandwich-type polyoxotungstate complexes, [{Mn(bpy)}2Na(H2O)2(MnCl)2{Mn(H2O)}(AsW9O33)2](9-) and [{Mn(bpy)}2Na(H2O)2(MnCl){Mn(H2O)}2(SbW9O33)2](8-) (bpy = 2,2'-bipyridine), whose structures have been obtained by single-crystal X-ray diffraction (SCXRD), complemented by results obtained from elemental analysis, electrospray ionization mass spectrometry, Fourier transform infrared spectroscopy, and thermogravimetric analysis. They consist of two [B-α-XW9O33](9-) subunits sandwiching a cyclic assembly of the hexagonal [{Mn(bpy)}2Na(H2O)2(MnCl)2{Mn(H2O)}](9+) and [{Mn(bpy)}2Na(H2O)2(MnCl){Mn(H2O)}2](10+) moieties, respectively, and represent the first pentanuclear Mn(II)-substituted sandwich-type polyoxometalates (POMs)...
July 19, 2017: Inorganic Chemistry
Xinyi Chia, Zdeněk Sofer, Jan Luxa, Martin Pumera
Owing to the anisotropic nature, layered transition metal dichalcogenides (TMDs) have captured tremendous attention for their promising uses in a plethora of applications. Currently, bulk of the research is centered on Group 6 TMDs. Layered noble metal dichalcogenides, in particular the noble metal tellurides, belong to a subset of Group 10 TMDs, wherein the transition metal is a noble metal of either palladium or platinum. We address here a lack of contemporary knowledge on these compounds by providing a comprehensive study on the electrochemistry of layered noble metal tellurides, PdTe2 and PtTe2, and their efficiency as electrocatalysts toward the hydrogen evolution reaction (HER)...
July 19, 2017: ACS Applied Materials & Interfaces
Elżbieta U Stolarczyk, Krzysztof Stolarczyk, Marta Łaszcz, Marek Kubiszewski, Andrzej Leś, Olga Michalak
Gold nanoparticles (AuNPs) have been widely used as nanocarriers in drug delivery application. However, the binding mechanism between AuNPs and drug bases still remains a puzzle. Our study included: (i) optimization of three synthesis of the AuNPs-pemetrexed (PE) nanocomposites formation which was monitored by UV-Vis spectroscopy, (ii) identification of PE in gold nanocomposites and mechanism of PE interaction with gold nanoparticles by electrochemistry, NMR and Raman measurements, (iii) characterization of the three nanocomposites by TEM, DSL, ESL, zeta potential, XRPD and TGA analysis...
July 11, 2017: European Journal of Pharmaceutical Sciences
Elin Moe, Filipe Rollo, Célia M Silveira, Murat Sezer, Peter Hildebrandt, Smilja Todorovic
Endonuclease III is a Fe-S containing bifunctional DNA glycosylase which is involved in the repair of oxidation damaged DNA. Here we employ surface enhanced IR spectroelectrochemistry and electrochemistry to study the enzyme from the highly radiation- and desiccation-resistant bacterium Deinococcus radiodurans (DrEndoIII2). The experiments are designed to shed more light onto specific parameters that are currently proposed to govern damage search and recognition by endonucleases III. We demonstrate that electrostatic interactions required for the redox activation of DrEndoIII2 may result in high electric fields that alter its structural and thermodynamic properties...
July 5, 2017: Spectrochimica Acta. Part A, Molecular and Biomolecular Spectroscopy
Yijia Wang, Xinying Zhang, Lang Zhao, Ting Bao, Wei Wen, Xiuhua Zhang, Shengfu Wang
MicroRNA 21 (MIR21) has garnered much attention in recent years as an important disease biomarker. The detection of it in human system shows great significance for the healthy evaluation and major diseases early detection. Herein, a novel approach tactfully manipulates the in-situ precise preparation of copper nanoclusters on overlapping Y-shaped ds-DNA for MIR21 analysis were developed in the proposed integrated aptasensor. In the presence of target MIR21, overlapping Y-shaped ds-DNA was constructed on electrode...
July 5, 2017: Biosensors & Bioelectronics
Janneke Veerbeek, Alejandro Méndez-Ardoy, Jurriaan Huskens
Functionalization of silicon-based sensing devices with self-assembled receptor monolayers offers flexibility and specificity towards the requested analyte as well as the possibility of sensor reuse. As electrical sensor performance is determined by electron transfer, we functionalized H-terminated silicon substrates with β-cyclodextrin (β-CD) molecules to investigate the electronic coupling between these host monolayers and the substrate. A trivalent (one ferrocene and two adamantyl moieties), redox-active guest was bound to the β-CD surface with a coverage of about 10(-11) mol/cm(2) and an overall binding constant of 1...
June 2017: ChemElectroChem
Łukasz Klapiszewski, Tadeusz J Szalaty, Beata Kurc, Małgorzata Stanisz, Andrzej Skrzypczak, Teofil Jesionowski
Kraft lignin (KL) was activated using selected ionic liquids (ILs). The activated form of the biopolymer, due to the presence of carbonyl groups, can be used in electrochemical tests. To increase the application potential of the system in electrochemistry, activated lignin forms were combined with manganese dioxide, and the most important physicochemical and morphological-microstructural properties of the novel, functional hybrid systems were determined using Fourier transform infrared spectroscopy (FTIR), elemental analysis (EA), scanning electron microscopy (SEM), zeta potential analysis, thermal stability (TGA/DTG) and porous structure analysis...
July 12, 2017: International Journal of Molecular Sciences
Koji Nakano, Junichi Tanabe, Ryoichi Ishimatsu, Toshihiko Imato
A new peptide nucleic acid (PNA) with an installed peroxidase function has been developed. Fmoc solid phase peptide synthesis prepared a PNA hybrid (VQKCAQCHTVE-(C2H4O)2CH2-[PNA(T)]6-G) that renders the microperoxidase backbone, followed by reconstitution with hemin. The resulting holocompound catalyzed the oxidation of 3,3',5,5'-tetramthylbenzidine by H2O2 to 50% that of natural microperoxidase-11, whereas the apo-form and hemin gave no responses. The peroxidase domain was found to be active toward direct electrochemistry and the PNA hybrid served for gene sensor; in the presence of the target DNA (5'-CATGTATAAAAAA-3'), an electrode-attached DNA probe (5'-TsTsTsTsTsTCTCATACATG-3') showed the ferric-to-ferrous quasi-reversible wave (-276 mV vs...
July 11, 2017: Bioconjugate Chemistry
Fuming Chen, Yinxi Huang, Lu Guo, Meng Ding, Hui Ying Yang
Novel desalination technologies with high ion removal capacity and low energy consumption are desirable to tackle the water shortage challenge. Herein, we report a dual-ion electrochemistry deionization (DEDI) system with silver chloride as the electrochemical chloride release/capture anode, sodium manganese oxide as the electrochemical sodium release/capture cathode, and flow salt solution as the electrolyte. Sodium and chloride ions are synergistically released to the flow electrolyte feed at an applied positive current...
July 11, 2017: Nanoscale
Yong Xiao, Enhua Zhang, Jingdong Zhang, Youfen Dai, Zhaohui Yang, Hans E M Christensen, Jens Ulstrup, Feng Zhao
Microorganisms exploit extracellular electron transfer (EET) in growth and information exchange with external environments or with other cells. Every microbial cell is surrounded by extracellular polymeric substances (EPS). Understanding the roles of three-dimensional (3D) EPS in EET is essential in microbiology and microbial exploitation for mineral bio-respiration, pollutant conversion, and bioenergy production. We have addressed these challenges by comparing pure and EPS-depleted samples of three representative electrochemically active strains viz Gram-negative Shewanella oneidensis MR-1, Gram-positive Bacillus sp...
July 2017: Science Advances
Chang-Wook Lee, Quan Pang, Seungbum Ha, Lei Cheng, Sang-Don Han, Kevin R Zavadil, Kevin G Gallagher, Linda F Nazar, Mahalingam Balasubramanian
The lithium-sulfur battery has long been seen as a potential next generation battery chemistry for electric vehicles owing to the high theoretical specific energy and low cost of sulfur. However, even state-of-the-art lithium-sulfur batteries suffer from short lifetimes due to the migration of highly soluble polysulfide intermediates and exhibit less than desired energy density due to the required excess electrolyte. The use of sparingly solvating electrolytes in lithium-sulfur batteries is a promising approach to decouple electrolyte quantity from reaction mechanism, thus creating a pathway toward high energy density that deviates from the current catholyte approach...
June 28, 2017: ACS Central Science
Louis Sieuw, Bruno Ernould, Jean-François Gohy, Alexandru Vlad
The electrochemistry of poly(2,5-dihydroxyaniline) (PDHA), a novel hybrid molecular configuration with redox active sites and electrical charge conduction along the polymer chain, has been recently reported. The theoretical capacity of this material is estimated at 443 mAh g(-1), with high power performances being proposed given the intrinsic electrical conductivity. However, the initial results were below the expectations: only half the theoretical capacity attained, poor cycling stability and modest power behavior calling for further investigations on improving these performances...
July 7, 2017: Scientific Reports
G Di Martino, V A Turek, A Lombardi, I Szabó, B de Nijs, A Kuhn, E Rosta, J J Baumberg
We study in real time the optical response of individual plasmonic nanoparticles on a mirror, utilized as electrodes in an electrochemical cell when a voltage is applied. In this geometry, Au nanoparticles are separated from a bulk Au film by an ultrathin molecular spacer. The nanoscale plasmonic hotspot underneath the nanoparticles locally reveals the modified charge on the Au surface and changes in the polarizability of the molecular spacer. Dark-field and Raman spectroscopy performed on the same nanoparticle show our ability to exploit isolated plasmonic junctions to track the dynamics of nanoelectrochemistry...
July 17, 2017: Nano Letters
Sudipta Chatterjee, Kushal Sengupta, Biswajit Mondal, Subal Dey, Abhishek Dey
Reactivity as well as selectivity are crucial in the activation and electrocatalytic reduction of molecular oxygen. Recent developments in the understanding of the mechanism of electrocatalytic O2 reduction by iron porphyrin complexes in situ using surface enhanced resonance Raman spectroscopy coupled to rotating disc electrochemistry (SERRS-RDE) in conjunction with H/D isotope effects on electrocatalytic current reveals that the rate of O2 reduction, ∼10(4) to 10(5) M(-1) s(-1) for simple iron porphyrins, is limited by the rate of O-O bond cleavage of an intermediate ferric peroxide species (Fe(III)-OOH)...
July 7, 2017: Accounts of Chemical Research
Rongfang Zhao, Xiao Shen, Qianhui Wu, Xiue Zhang, Wenlong Li, Ge Gao, Lingyun Zhu, Lubin Ni, Guowang Diao, Ming Chen
Among the numerous candidate materials for lithium ion batteries (LIBs), ferroferric oxide (Fe3O4) has been extensively concerned as a prospective anode material because of its high theoretical specific capacity, abundant resources, low cost and non-toxic. Here, we have designed and fabricated a unique yolk-shell construction by generating heterogeneous double shelled SnO2 and nitrogen-doped carbon on Fe3O4 yolk (denoted as Fe3O4@SnO2@C-N nanoboxes). The yolk-shell structured Fe3O4@SnO2@C-N nanoboxes have the adjustable void space, which permits the free expansion of Fe3O4 yolks without breaking the double shells during the lithiation/delithiation processes, avoiding the structural pulverization...
July 6, 2017: ACS Applied Materials & Interfaces
R Götz, H K Ly, P Wrzolek, M Schwalbe, I M Weidinger
Drycast methods have been used frequently in recent decades to adsorb a range of synthetic catalysts on electrodes. The uncoordinated multilayers that are formed via this immobilization method can however have a strong impact on the electrocatalytic reaction pathway as slow electron transfer and intermolecular interactions can alter the chemistry of the catalysts on the surface. To gain insight into the structure of Fe porphyrin Hangman catalysts during electrocatalytic oxygen reduction a combination of electrochemistry and surface enhanced resonance Raman spectroscopy (SERRS) was applied...
July 6, 2017: Dalton Transactions: An International Journal of Inorganic Chemistry
Magdalena Kundys, Michal Nejbauer, Martin Jönsson-Niedziolka, Wojciech Adamiak
In this work, we explore generation-collection electrochemistry in a rotating droplet hydrodynamic system, where a 70 μL droplet containing a redox active species (ferrocyanide) is sandwiched between an upper rotating rod and bottom nonmoving generator and collector planar electrodes. In such a system, we studied the effect of the counter electrode reaction on the recorded generator current, and the effect of the generator-collector distance (ranging from 3 to ca. 500 μm) on the collection efficiencies obtained at rotation rates ranging from 50 to 1100 rpm...
July 17, 2017: Analytical Chemistry
Zaisheng Yan, Yuhong He, Haiyuan Cai, Joy D Van Nostrand, Zhili He, Jizhong Zhou, Lee R Krumholz, He-Long Jiang
Sediment microbial fuel cells (SMFCs) can stimulate the degradation of polycyclic aromatic hydrocarbons in sediments, but the mechanism of this process is poorly understood at the microbial functional gene level. Here, the use of SMFC resulted in 92% benzo[a]pyrene (BaP) removal over 970 days relative to 54% in the controls. Sediment functions, microbial community structure, and network interactions were dramatically altered by the SMFC employment. Functional gene analysis showed that c-type cytochrome genes for electron transfer, aromatic degradation genes, and extracellular ligninolytic enzymes involved in lignin degradation were significantly enriched in bulk sediments during SMFC operation...
July 14, 2017: Environmental Science & Technology
Mark W Rutland
It is an honour to be charged with providing the concluding remarks for a Faraday Discussion. As many have remarked before, it is nonetheless a prodigious task, and what follows is necessarily a personal, and probably perverse, view of a watershed event in the Chemical Physics of Electroactive materials. The spirit of the conference was captured in a single sentence during the meeting itself."It is the nexus between rheology, electrochemistry, colloid science and energy storage". The current scientific climate is increasingly dominated by a limited number of global challenges, and there is thus a tendency for research to resemble a football match played by 6 year olds, where everyone on the field chases the (funding) ball instead of playing to their "discipline"...
July 1, 2017: Faraday Discussions
Emel Önal, Sevinc Zehra Topal, Ismail Fidan, Savaş Berber, Fabienne Dumoulin, Catherine Hirel
A systematic structure-photoproperties relationship study of the interactions of porphyrin-fullerene dyads with molecular oxygen was conducted on a set of three porphyrin-fullerene dyads, as this approach of related applications - oxygen sensitivity and photo-induced singlet oxygen generation - of such dyads remained to be endeavoured. To promote energy transfers between the porphyrin and fullerene units and limit undesired charge separation, a particular attention was devoted to the choice of the solvents for the photoproperties determination...
June 30, 2017: Journal of Fluorescence
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