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Journal of Physical Chemistry. C, Nanomaterials and Interfaces

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https://www.readbyqxmd.com/read/28936278/modulating-the-catalytic-activity-of-cerium-oxide-nanoparticles-with-the-anion-of-the-precursor-salt
#1
Swetha Barkam, Julian Ortiz, Shashank Saraf, Nicholas Eliason, Rameech Mccormack, Soumen Das, Ankur Gupta, Craig Neal, Alex Petrovici, Cameron Hanson, Michael D Sevilla, Amitava Adhikary, Sudipta Seal
In this work, we tested our hypothesis that surface chemistry and antioxidant properties of cerium nanoparticles (CNPs) are affected by presence of counterions. We first employed various precursor cerium (III) (Ce(III)) salts with different counterions (acetate, nitrate, chloride, sulfate) to synthesize CNPs following the same wet chemical methodology. Electron spin resonance (ESR) studies provided evidence for the formation of radicals from counterions (e.g., NO3•(2-) from reduction of NO3(-) in CNPs synthesized from Ce(III) nitrate)...
September 14, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28936277/self-limiting-adsorption-of-wo3-oligomers-on-oxide-substrates-in-solution
#2
Matthias Müllner, Jan Balajka, Michael Schmid, Ulrike Diebold, Stijn F L Mertens
Electrochemical surface science of oxides is an emerging field with expected high impact in developing, for instance, rationally designed catalysts. The aim in such catalysts is to replace noble metals by earth-abundant elements, yet without sacrificing activity. Gaining an atomic-level understanding of such systems hinges on the use of experimental surface characterization techniques such as scanning tunneling microscopy (STM), in which tungsten tips have been the most widely used probes, both in vacuum and under electrochemical conditions...
September 14, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28919935/hybridization-of-single-nanocrystals-of-cs4pbbr6-and-cspbbr3
#3
Chris de Weerd, Junhao Lin, Leyre Gomez, Yasufumi Fujiwara, Kazutomo Suenaga, Tom Gregorkiewicz
Nanocrystals of all-inorganic cesium lead halide perovskites (CsPbX3, X = Cl, Br, I) feature high absorption and efficient narrow-band emission which renders them promising for future generation of photovoltaic and optoelectronic devices. Colloidal ensembles of these nanocrystals can be conveniently prepared by chemical synthesis. However, in the case of CsPbBr3, its synthesis can also yield nanocrystals of Cs4PbBr6 and the properties of the two are easily confused. Here, we investigate in detail the optical characteristics of simultaneously synthesized green-emitting CsPbBr3 and insulating Cs4PbBr6 nanocrystals...
September 7, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28919934/probing-the-influence-of-disorder-on-lanthanide-luminescence-using-eu-doped-lapo4-nanoparticles
#4
Jacobine J H A van Hest, Gerhard A Blab, Hans C Gerritsen, Celso de Mello Donega, Andries Meijerink
Lanthanide-doped nanocrystals (NCs) differ from their bulk counterparts due to their large surface to volume ratio. It is generally assumed that the optical properties are not affected by size effects as electronic transitions occur within the well-shielded 4f shell of the lanthanide dopant ions. However, defects and disorder in the surface layer can affect the luminescence properties. Trivalent europium is a suitable ion to investigate the subtle influence of the surface, because of its characteristic luminescence and high sensitivity to the local environment...
September 7, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28883897/mobility-and-decay-dynamics-of-charge-carriers-in-one-dimensional-selenium-van-der-waals-solid
#5
Prashant Bhaskar, Alexander W Achtstein, Silke L Diedenhofen, Laurens D A Siebbeles
Trigonal selenium is a semiconducting van der Waals solid that consists of helical atomic chains. We studied the mobility and decay dynamics of excess electrons and holes moving along the selenium chains. Excess charge carriers were generated by irradiation of powdered selenium with 3 MeV electron pulses. Their mobility and decay via trapping or recombination was studied by time-resolved microwave conductivity measurements as a function of temperature. The mobility of charge carriers along the Se chains is at least ca...
August 31, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28883896/near-wall-molecular-ordering-of-dilute-ionic-liquids
#6
Monchai Jitvisate, James R T Seddon
The interfacial behavior of ionic liquids promises tunable lubrication as well as playing an integral role in ion diffusion for electron transfer. Diluting the ionic liquids optimizes bulk parameters, such as electric conductivity, and one would expect dilution to disrupt the near-wall molecular ordering. We study this ordering in the ionic liquids [Emim](+)[NTf2](-), [Emim](+)[DCA](-), and [C4mpyr](+)[NTf2](-), diluted in the solvent dimethyl sulfoxide. We found a structural crossover from well-ordered ionic liquids to a well-ordered solvent with increasing dilution, but this occurs nonlinearly, with solvent molecules initially space-filling and solvating and later disrupting the ionic layers...
August 31, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28845208/in-situ-2p3d-resonant-inelastic-x-ray-scattering-tracking-cobalt-nanoparticle-reduction
#7
Boyang Liu, Matti M van Schooneveld, Yi-Tao Cui, Jun Miyawaki, Yoshihisa Harada, Thomas O Eschemann, Krijn P de Jong, Mario U Delgado-Jaime, Frank M F de Groot
In-situ carbon-thermal reduction of cobalt oxide nanoparticles supported on carbon nanotubes was studied by cobalt 2p3d resonant inelastic X-ray scattering (RIXS). The in-situ 2p X-ray absorption spectroscopy (XAS) and RIXS measurements were performed at 500, 600, and 700 °C, where four consistent excitation energies were used for RIXS acquisitions. After 700 °C reduction, the XAS spectrum shows a cobalt metal-like shape, while the RIXS spectra reveal the minority cobalt monoxide phase. The holistic fit on both XAS and RIXS data reveals the respective contributions from metal and monoxide...
August 17, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28845207/electrochemical-co-oxidation-at-platinum-on-carbon-studied-through-analysis-of-anomalous-in-situ-ir-spectra
#8
Ian J McPherson, Philip A Ash, Lewys Jones, Aakash Varambhia, Robert M J Jacobs, Kylie A Vincent
The oxidation of adsorbed CO is a key reaction in electrocatalysis. It has been studied extensively on both extended model surfaces and on nanoparticles; however, correlation between the two is far from simple. Molecular insight into the reaction is often provided using in situ IR spectroscopy; however, practical challenges mean in situ studies on nanoparticles have yet to provide the same level of detail as those on model surfaces. Here we use a new approach to in situ IR spectroscopy to study the mechanism of CO adlayer oxidation on a commercial carbon-supported Pt catalyst...
August 17, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28798858/generation-of-subsurface-voids-incubation-effect-and-formation-of-nanoparticles-in-short-pulse-laser-interactions-with-bulk-metal-targets-in-liquid-molecular-dynamics-study
#9
Cheng-Yu Shih, Maxim V Shugaev, Chengping Wu, Leonid V Zhigilei
The ability of short pulse laser ablation in liquids to produce clean colloidal nanoparticles and unusual surface morphology has been employed in a broad range of practical applications. In this paper, we report the results of large-scale molecular dynamics simulations aimed at revealing the key processes that control the surface morphology and nanoparticle size distributions by pulsed laser ablation in liquids. The simulations of bulk Ag targets irradiated in water are performed with an advanced computational model combining a coarse-grained representation of liquid environment and an atomistic description of laser interaction with metal targets...
August 3, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28751927/an-nmr-crystallographic-investigation-of-the-relationships-between-the-crystal-structure-and-29-si-isotropic-chemical-shift-in-silica-zeolites
#10
Daniel M Dawson, Robert F Moran, Sharon E Ashbrook
NMR crystallography has recently been applied to great effect for silica zeolites. Here we investigate whether it is possible to extend the structural information available from routine NMR spectra via a simple structure-spectrum relationship. Unlike previous empirically derived relationships that have compared experimental crystal structures for (often disordered) silicates with experimental NMR spectra, where the structure may not be an accurate representation of the material studied experimentally, we use NMR parameters calculated by density functional theory (DFT) for both model Si(OSi(OH)3)4 clusters and also extended zeolitic SiO2 frameworks, for which the input structure corresponding to the NMR parameters is known exactly...
July 20, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28751926/origin-of-the-strong-interaction-between-polar-molecules-and-copper-ii-paddle-wheels-in-metal-organic-frameworks
#11
Daniele Ongari, Davide Tiana, Samuel J Stoneburner, Laura Gagliardi, Berend Smit
The copper paddle-wheel is the building unit of many metal organic frameworks. Because of the ability of the copper cations to attract polar molecules, copper paddle-wheels are promising for carbon dioxide adsorption and separation. They have therefore been studied extensively, both experimentally and computationally. In this work we investigate the copper-CO2 interaction in HKUST-1 and in two different cluster models of HKUST-1: monocopper Cu(formate)2 and dicopper Cu2(formate)4. We show that density functional theory methods severely underestimate the interaction energy between copper paddle-wheels and CO2, even including corrections for the dispersion forces...
July 20, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28729893/mechanically-and-electrically-robust-self-assembled-monolayers-for-large-area-tunneling-junctions
#12
Yanxi Zhang, Xinkai Qiu, Pavlo Gordiichuk, Saurabh Soni, Theodorus L Krijger, Andreas Herrmann, Ryan C Chiechi
This paper examines the relationship between mechanical deformation and the electronic properties of self-assembled monolayers (SAMs) of the oligothiophene 4-([2,2':5',2″:5″,2‴-quaterthiophen]-5-yl)butane-1-thiol (T4C4) in tunneling junctions using conductive probe atomic force microscopy (CP-AFM) and eutectic Ga-In (EGaIn). We compared shifts in conductivity, transition voltages of T4C4 with increasing AFM tip loading force to alkanethiolates. While these shifts result from an increasing tilt angle from penetration of the SAM by the AFM tip for the latter, we ascribe them to distortions of the π system present in T4C4, which is more mechanically robust than alkanethiolates of comparable length; SAMs comprising T4C4 shows about five times higher Young's modulus than alkanethiolates...
July 13, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28729892/reversible-charge-trapping-in-bis-carbazole-diimide-redox-polymers-with-complete-luminescence-quenching-enabling-nondestructive-read-out-by-resonance-raman-spectroscopy
#13
Luuk Kortekaas, Federico Lancia, Jorn D Steen, Wesley R Browne
The coupling of substituted carbazole compounds through carbon-carbon bond formation upon one-electron oxidation is shown to be a highly versatile approach to the formation of redox polymer films. Although the polymerization of single carbazole units has been proposed earlier, we show that by tethering pairs of carbazoles double sequential dimerization allows for facile formation of redox polymer films with fine control over film thickness. We show that the design of the monomers and in particular the bridging units is key to polymer formation, with the diaminobenzene motif proving advantageous, in terms of the matching to the redox potentials of the monomer and polymer film and thereby avoiding limitations in film thickness (autoinsulation), but introduces unacceptable instability due to the intrinsic redox activity of this moiety...
July 13, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28729891/vibrational-excitation-of-h2-scattering-from-cu-111-effects-of-surface-temperature-and-of-allowing-energy-exchange-with-the-surface
#14
Geert-Jan Kroes, J I Juaristi, M Alducin
In scattering of H2 from Cu(111), vibrational excitation has so far defied an accurate theoretical description. To expose the causes of the large discrepancies with experiment, we investigate how the feature due to vibrational excitation (the "gain peak") in the simulated time-of-flight spectrum of (v = 1, j = 3) H2 scattering from Cu(111) depends on the surface temperature (Ts) and the possibility of energy exchange with surface phonons and electron-hole pairs (ehp's). Quasi-classical dynamics calculations are performed on the basis of accurate semiempirical density functionals for the interaction with H2 + Cu(111)...
June 29, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28804530/evolution-of-reduced-graphene-oxide-sns2-hybrid-nanoparticle-electrodes-in-li-ion-batteries
#15
Mohammad H Modarres, Jonathan Hua-Wei Lim, Chandramohan George, Michael De Volder
Hybrid nanomaterials where active battery nanoparticles are synthesized directly onto conductive additives such as graphene hold the promise of improving the cyclability and energy density of conversion and alloying type Li-ion battery electrodes. Here we investigate the evolution of hybrid reduced graphene oxide-tin sulfide (rGO-SnS2) electrodes during battery cycling. These hybrid nanoparticles are synthesized by a one-step solvothermal microwave reaction which allows for simultaneous synthesis of the SnS2 nanocrystals and reduction of GO...
June 22, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28663772/proton-environments-in-biomimetic-calcium-phosphates-formed-from-mesoporous-bioactive-cao-sio2-p2o5-glasses-in-vitro-insights-from-solid-state-nmr
#16
Renny Mathew, Claudia Turdean-Ionescu, Yang Yu, Baltzar Stevensson, Isabel Izquierdo-Barba, Ana García, Daniel Arcos, María Vallet-Regí, Mattias Edén
When exposed to body fluids, mesoporous bioactive glasses (MBGs) of the CaO-SiO2-P2O5 system develop a bone-bonding surface layer that initially consists of amorphous calcium phosphate (ACP), which transforms into hydroxy-carbonate apatite (HCA) with a very similar composition as bone/dentin mineral. Information from various (1)H-based solid-state nuclear magnetic resonance (NMR) experiments was combined to elucidate the evolution of the proton speciations both at the MBG surface and within each ACP/HCA constituent of the biomimetic phosphate layer formed when each of three MBGs with distinct Ca, Si, and P contents was immersed in a simulated body fluid (SBF) for variable periods between 15 min and 30 days...
June 22, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28620448/influence-of-film-and-substrate-structure-on-photoelectron-momentum-maps-of-coronene-thin-films-on-ag-111
#17
Christian Udhardt, Felix Otto, Christian Kern, Daniel Lüftner, Tobias Huempfner, Tino Kirchhuebel, Falko Sojka, Matthias Meissner, Bernd Schröter, Roman Forker, Peter Puschnig, Torsten Fritz
Angle-resolved ultraviolet photoelectron spectroscopy (ARUPS) was measured for one-monolayer coronene films deposited on Ag(111). The (kx ,ky )-dependent photoelectron momentum maps (PMMs), which were extracted from the ARUPS data by cuts at fixed binding energies, show finely structured patterns for the highest and the second-highest occupied molecular orbitals. While the substructure of the PMM main features is related to the 4 × 4 commensurate film structure, various features with three-fold symmetry imply an additional influence of the substrate...
June 8, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28620447/photoelectrochemistry-by-design-tailoring-the-nanoscale-structure-of-pt-nio-composites-leads-to-enhanced-photoelectrochemical-hydrogen-evolution-performance
#18
András Sápi, András Varga, Gergely F Samu, Dorina Dobó, Koppány L Juhász, Bettina Takács, Erika Varga, Ákos Kukovecz, Zoltán Kónya, Csaba Janáky
Photoelectrochemical hydrogen evolution is a promising avenue to store the energy of sunlight in the form of chemical bonds. The recent rapid development of new synthetic approaches enables the nanoscale engineering of semiconductor photoelectrodes, thus tailoring their physicochemical properties toward efficient H2 formation. In this work, we carried out the parallel optimization of the morphological features of the semiconductor light absorber (NiO) and the cocatalyst (Pt). While nanoporous NiO films were obtained by electrochemical anodization, the monodisperse Pt nanoparticles were synthesized using wet chemical methods...
June 8, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28736586/photothermal-microscopy-of-coupled-nanostructures-and-the-impact-of-nanoscale-heating-in-surface-enhanced-raman-spectroscopy
#19
Zhi-Cong Zeng, Hao Wang, Paul Johns, Gregory V Hartland, Zachary D Schultz
The optical properties of plasmonic nanoparticles are strongly dependent on interactions with other nanoparticles, which complicates analysis for systems larger than a few particles. In this work we examined heat dissipation in aggregated nanoparticles, and its influence on surface enhanced Raman scattering (SERS), through correlated photothermal heterodyne imaging, electron microscopy and SERS measurements. For dimers the per particle absorption cross-sections show evidence of interparticle coupling, however, the effects are much smaller than those for the field enhancements that are important for SERS...
June 1, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
https://www.readbyqxmd.com/read/28603579/in-situ-optical-reflectance-difference-observations-of-co-oxidation-over-pd-100
#20
Willem G Onderwaater, Andriy Taranovskyy, Gertjan C van Baarle, Joost W M Frenken, Irene M N Groot
Using a home-built reflectometer, we have investigated the changes in the optical reflectivity of a Pd(100) model catalyst during CO oxidation under high-pressure, high-temperature conditions. We observe changes in optical contrast when exposing the surface to CO oxidation conditions at 200 mbar from room temperature up to 400 °C. These changes in reflectivity are a result both of the formation of a surface oxide layer and of a change in surface roughness because of gas exposure. However, the reflectivity is more sensitive to the presence of a thin, flat oxide layer than to surface roughness...
June 1, 2017: Journal of Physical Chemistry. C, Nanomaterials and Interfaces
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