“Aluminum incorporation into MCM-48 toward the creation of Brønsted acidity”. Collart O, Cool P, van der Voort P, Meynen V, Vansant EF, Houthoofd KJ, Grobet PJ, Lebedev OI, Van Tendeloo G, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 108, 13905 (2004). http://doi.org/10.1021/jp049837x
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 13
DOI: 10.1021/jp049837x
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“Approaches to calculation of exciton interaction energies for a molecular dimer”. Howard IA, Zutterman F, Deroover G, Lamoen D, van Alsenoy C, Journal Of Physical Chemistry B 108, 19155 (2004). http://doi.org/10.1021/jp040417h
Keywords: A1 Journal article; Electron Microscopy for Materials Science (EMAT);
Impact Factor: 3.177
Times cited: 35
DOI: 10.1021/jp040417h
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“Hydrothermal synthesis and characterization of nanorods of various titanates and titanium dioxide”. Kolen'ko YV, Kovnir KA, Gavrilov AI, Garshev AV, Frantti J, Lebedev OI, Churagulov BR, Van Tendeloo G, Yoshimura M, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 110, 4030 (2006). http://doi.org/10.1021/jp055687u
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.177
Times cited: 234
DOI: 10.1021/jp055687u
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“The influence of the alcohol concentration on the structural ordering of mesoporous silica: cosurfactant versus cosolvent”. Liu S, Cool P, Collart O, van der Voort P, Vansant EF, Lebedev OI, Van Tendeloo G, Jiang M, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 107, 10405 (2003). http://doi.org/10.1021/jp034410w
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 134
DOI: 10.1021/jp034410w
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“Investigation of the morphology of the mesoporous SBA-16 and SBA-15 materials”. Stevens WJJ, Lebeau K, Mertens M, Van Tendeloo G, Cool P, Vansant EF, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 110, 9183 (2006). http://doi.org/10.1021/jp0548725
Keywords: A1 Journal article; Laboratory of adsorption and catalysis (LADCA); Electron microscopy for materials research (EMAT)
Impact Factor: 3.177
Times cited: 109
DOI: 10.1021/jp0548725
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“Leached natural saponite as the silicate source in the synthesis of aluminosilicate hexagonal mesoporous materials”. Linssen T, Cool P, Baroudi M, Cassiers K, Vansant EF, Lebedev O, van Landuyt J, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 106, 4470 (2002). http://doi.org/10.1021/jp015578p
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 23
DOI: 10.1021/jp015578p
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“Phase transitions in C60 and the related microstructure: a study by electron diffraction and electron microscopy”. Van Tendeloo G, van Heurck C, van Landuyt J, Amelinckx S, Verheijen MA, van Loosdrecht PHM, Meijer G, Journal of physical chemistry 96, 7424 (1992). http://doi.org/10.1021/j100197a054
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Times cited: 33
DOI: 10.1021/j100197a054
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“Structural, textural, and electronic properties of a nanosized mesoporous ZnxTi1-xO2-x solid solution prepared by a supercritical drying route”. Kolen'ko YV, Kovnir KA, Gavrilov AI, Garshev AV, Meskin PE, Churagulov BR, Bouchard M, Colbeau-Justin C, Lebedev OI, Van Tendeloo G, Yoshimura M, Journal of physical chemistry B 109, 20303 (2005). http://doi.org/10.1021/jp0535341
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 3.177
Times cited: 34
DOI: 10.1021/jp0535341
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“TEM observation of aggregation steps in room-temperature silicalite-1 zeolite formation”. Liang D, Follens LRA, Aerts A, Martens JA, Van Tendeloo G, Kirschhock CEA, Journal of physical chemistry C 111, 14283 (2007). http://doi.org/10.1021/jp074960k
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
Times cited: 41
DOI: 10.1021/jp074960k
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“Two-Dimensional CdSe-PbSe Heterostructures and PbSe Nanoplatelets: Formation, Atomic Structure, and Optical Properties”. Salzmann BBV, Wit J de, Li C, Arenas-Esteban D, Bals S, Meijerink A, Vanmaekelbergh D, The journal of physical chemistry: C : nanomaterials and interfaces 126, 1513 (2022). http://doi.org/10.1021/acs.jpcc.1c09412
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 3.7
Times cited: 12
DOI: 10.1021/acs.jpcc.1c09412
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“Optimized 3D Reconstruction of Large, Compact Assemblies of Metallic Nanoparticles”. Altantzis T, Wang D, Kadu A, van Blaaderen A, Bals S, Journal Of Physical Chemistry C 125, 26240 (2021). http://doi.org/10.1021/acs.jpcc.1c08478
Abstract: 3D characterization of assemblies of nanoparticles is of great importance to determine their structure-property connection. Such investigations become increasingly more challenging when the assemblies become larger and more compact. In this paper, we propose an optimized approach for electron tomography to minimize artefacts related to beam broadening in High Angle Annular Dark-Field Scanning Transmission Electron Microscopy mode. These artefacts are typically present at one side of the reconstructed 3D data set for thick nanoparticle assemblies. To overcome this problem, we propose a procedure in which two tomographic tilt series of the same sample are acquired. After acquiring the first series, the sample is flipped over 180o, and a second tilt series is acquired. By merging the two reconstructions, blurring in the reconstructed volume is minimized. Next, this approach is combined with an advanced three-dimensional reconstruction algorithm yielding quantitative structural information. Here, the approach is applied to a thick and compact assembly of spherical Au nanoparticles, but the methodology can we used to investigate a broad range of samples.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 4.536
Times cited: 4
DOI: 10.1021/acs.jpcc.1c08478
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“CO2 conversion in a microwave plasma reactor in the presence of N2 : elucidating the role of vibrational levels”. Heijkers S, Snoeckx R, Kozák T, Silva T, Godfroid T, Britun N, Snyders R, Bogaerts A, The journal of physical chemistry: C : nanomaterials and interfaces 119, 12815 (2015). http://doi.org/10.1021/acs.jpcc.5b01466
Abstract: A chemical kinetics model is developed for a CO2/N2 microwave plasma, focusing especially on the vibrational levels of both CO2 and N2. The model is used to calculate the CO2 and N2 conversion as well as the energy efficiency of CO2 conversion for different power densities and for N2 fractions in the CO2/N2 gas mixture ranging from 0 to 90%. The calculation results are compared with measurements, and agreements within 23% and 33% are generally found for the CO2 conversion and N2 conversion, respectively. To explain the observed trends, the destruction and formation processes of both CO2 and N2 are analyzed, as well as the vibrational distribution functions of both CO2 and N2. The results indicate that N2 contributes in populating the lower asymmetric levels of CO2, leading to a higher absolute CO2 conversion upon increasing N2 fraction. However, the effective CO2 conversion drops because there is less CO2 initially present in the gas mixture; thus, the energy efficiency also drops with rising N2 fraction.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 56
DOI: 10.1021/acs.jpcc.5b01466
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“Probing the electron beam-induced structural evolution of halide perovskite thin films by scanning transmission electron microscopy”. Zhou X-G, Yang C-Q, Sang X, Li W, Wang L, Yin Z-W, Han J-R, Li Y, Ke X, Hu Z-Y, Cheng Y-B, Van Tendeloo G, Journal Of Physical Chemistry C 125, 10786 (2021). http://doi.org/10.1021/ACS.JPCC.1C02156
Abstract: A deep understanding of the fine structure at the atomic scale of halide perovskite materials has been limited by their sensitivity to the electron beam that is widely used for structural characterization. The sensitivity of a gamma-CsPbIBr2 perovskite thin film under electron beam irradiation is revealed by scanning transmission electron microscopy (STEM) through a universal large-range electron dose measurement, which is based on discrete single-electron events in the STEM mode. Our research indicates that the gamma-CsPbIBr2 thin film undergoes structural changes with increasing electron overall dose (e(-).A(-2)) rather than dose rate (e(-).A(-2).s(-1)), which suggests that overall dose is the key operative parameter. The electron beam-induced structural evolution of gamma-CsPbIBr2 is monitored by fine control of the electron beam dose, together with the analysis of high-resolution (S)TEM, diffraction, and energy-dispersive X-ray spectroscopy. Our results show that the gamma-CsPbIBr2 phase first forms an intermediate phase [e.g., CsPb(1-x)(IBr)((3-y))] with a superstructure of ordered vacancies in the pristine unit cell, while a fraction of Pb2+ is reduced to Pb-0. As the electron dose increases, Pb nanoparticles precipitate, while the remaining framework forms the Cs2IBr phase, accompanied by some amorphization. This work provides guidelines to minimize electron beam irradiation artifacts for atomic-resolution imaging on CsPbIBr2 thin films.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
DOI: 10.1021/ACS.JPCC.1C02156
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“Kinetics of energy selective Cs encapsulation in single-walled carbon nanotubes for damage-free and position-selective doping”. Kato T, Neyts EC, Abiko Y, Akama T, Hatakeyama R, Kaneko T, The journal of physical chemistry: C : nanomaterials and interfaces 119, 11903 (2015). http://doi.org/10.1021/acs.jpcc.5b00300
Abstract: A method has been developed for damage-free cesium (Cs) encapsulation within single-walled carbon nanotubes (SWNTs) with fine position selectivity. Precise energy tuning of Cs-ion irradiation revealed that there is a clear energy window (2060 eV) for the efficient encapsulation of Cs through the hexagonal network of SWNT sidewalls without causing significant damage. This minimum energy threshold of Cs-ion encapsulation (∼20 eV) matches well with the value obtained by ab initio simulation (∼22 eV). Furthermore, position-selective Cs encapsulation was carried out, resulting in the successful formation of pn-junction SWNT thin films with excellent environmental stability.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 3
DOI: 10.1021/acs.jpcc.5b00300
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“Electronic properties of oxidized graphene : effects of strain and an electric field on flat bands and the energy gap”. Alihosseini M, Ghasemi S, Ahmadkhani S, Alidoosti M, Esfahani DN, Peeters FM, Neek-Amal M, The journal of physical chemistry letters (2021). http://doi.org/10.1021/ACS.JPCLETT.1C03286
Abstract: A multiscale modeling and simulation approach, including first-principles calculations, ab initio molecular dynamics simulations, and a tight binding approach, is employed to study band flattening of the electronic band structure of oxidized monolayer graphene. The width offlat bands can be tuned by strain, the external electric field, and the density of functional groups and their distribution. A transition to a conducting state is found for monolayer graphene with impurities when it is subjected to an electric field of similar to 1.0 V/angstrom. Several parallel impurity-induced flat bands appear in the low-energy spectrum of monolayer graphene when the number of epoxy groups is changed. The width of the flat band decreases with an increase in tensile strain but is independent of the electric field strength. Here an alternative and easy route for obtaining band flattening in thermodynamically stable functionalized monolayer graphene is introduced. Our work discloses a new avenue for research on band flattening in monolayer graphene.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 9.353
Times cited: 7
DOI: 10.1021/ACS.JPCLETT.1C03286
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“The Dominant Pathways for the Conversion of Methane into Oxygenates and Syngas in an Atmospheric Pressure Dielectric Barrier Discharge”. De Bie C, van Dijk J, Bogaerts A, The journal of physical chemistry: C : nanomaterials and interfaces 119, 22331 (2015). http://doi.org/10.1021/acs.jpcc.5b06515
Abstract: A one-dimensional fluid model for a dielectric barrier discharge in CH4/O2 and CH4/CO2 gas mixtures is developed. The model describes the gas-phase chemistry for partial oxidation and for dry reforming of methane. The spatially averaged densities of the various plasma species are presented as a function of time and initial gas mixing ratio. Besides, the conversion of the inlet gases and the selectivities of the reaction products are calculated. Syngas, higher hydrocarbons, and higher oxygenates are typically found to be important reaction products. Furthermore, the main underlying reaction pathways for the formation of syngas, methanol, formaldehyde, and other higher oxygenates are determined.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 46
DOI: 10.1021/acs.jpcc.5b06515
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“Chemical structure of nitrogen-doped graphene with single platinum atoms and atomic clusters as a platform for the PEMFC electrode”. Stambula S, Gauquelin N, Bugnet M, Gorantla S, Turner S, Sun S, Liu J, Zhang G, Sun X, Botton GA, The journal of physical chemistry: C : nanomaterials and interfaces 118, 3890 (2014). http://doi.org/10.1021/jp408979h
Abstract: A platform for producing stabilized Pt atoms and clusters through the combination of an N-doped graphene support and atomic layer deposition (ALD) for the Pt catalysts was investigated using transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM). It was determined, using imaging and spectroscopy techniques, that a wide range of N-dopant types entered the graphene lattice through covalent bonds without largely damaging its structure. Additionally and most notably, Pt atoms and atomic clusters formed in the absence of nanoparticles. This work provides a new strategy for experimentally producing stable atomic and subnanometer cluster catalysts, which can greatly assist the proton exchange membrane fuel cell (PEMFC) development by producing the ultimate surface area to volume ratio catalyst.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT)
Impact Factor: 4.536
Times cited: 57
DOI: 10.1021/jp408979h
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“First-principles investigation of bilayer fluorographene”. Sivek J, Leenaerts O, Partoens B, Peeters FM, The journal of physical chemistry: C : nanomaterials and interfaces 116, 19240 (2012). http://doi.org/10.1021/jp3027012
Abstract: Ab initio calculations within the density functional theory formalism are performed to investigate the stability and electronic properties of fluorinated bilayer graphene (bilayer fluorographene). A comparison is made to previously investigated graphane, bilayer graphane, and fluorographene. Bilayer fluorographene is found to be a much more stable material than bilayer graphane. Its electronic band structure is similar to that of monolayer fluorographene, but its electronic band gap is significantly larger (about 1 eV). We also calculate the effective masses around the Gamma-point for fluorographene and bilayer fluorographene and find that they are isotropic, in contrast to earlier reports. Furthermore, it is found that bilayer fluorographene is almost as strong as graphene, as its 2D Young's modulus is approximately 300 N m(-1).
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 4.536
Times cited: 39
DOI: 10.1021/jp3027012
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“Identification of a unique pyridinic FeN4Cx electrocatalyst for N₂, reduction : tailoring the coordination and carbon topologies”. Nematollahi P, Neyts EC, Journal Of Physical Chemistry C 126, 14460 (2022). http://doi.org/10.1021/ACS.JPCC.2C03577
Abstract: Although the heterogeneity of pyrolyzed Fe???N???C materials is known and has been reported previously, the atomic structure of the active sites and their detailed reaction mechanisms are still unknown. Here, we identified two pyridinic Fe???N4-like centers with different local C coordinates, i.e., FeN4C8 and FeN4C10, and studied their electrocatalytic activity for the nitrogen reduction reaction (NRR) based on density functional theory (DFT) calculations. We also discovered the influence of the adsorption of NH2 as a functional ligand on catalyst performance on the NRR. We confirmed that the NRR selectivity of the studied catalysts is essentially governed either by the local C coordination or by the dynamic structure associated with the FeII/FeIII. Our investigations indicate that the proposed traditional pyridinic FeN4C10 has higher catalytic activity and selectivity for the NRR than the robust FeN4C8 catalyst, while it may have outstanding activity for promoting other (electro)catalytic reactions. <comment>Superscript/Subscript Available</comment
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 3.7
DOI: 10.1021/ACS.JPCC.2C03577
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“A counterion-catalyzed (S0H+)(X-I+) pathway toward heat- and steam-stable mesostructured silica assembled from amines in acidic conditions”. Cassiers K, van der Voort P, Linssen T, Vansant EF, Lebedev O, van Landuyt J, The journal of physical chemistry : B : condensed matter, materials, surfaces, interfaces and biophysical 107, 3690 (2003). http://doi.org/10.1021/jp026696v
Abstract: An alternative pathway to assemble mesoporous molecular sieve silicas is developed using nonionic alkylamines and N,N-dimethylalkylamines (SO) as structure-directing agents in acidic conditions. The synthesized mesostructures possess wormhole-like frameworks with pore sizes and pore volumes in the range of 20-90 Angstrom and 0.5-1.3 cm(3)/g, respectively. The formation of the mesophase is controlled by a counterion-mediated mechanism of the type (S(0)H(+))(X(-)I(+)), where S(0)H(+) are protonated water molecules that are hydrogen bonded to the lone electron pairs on the amine surfactant headgroups (S(0)H(+)), X(-) is the counteranion originating from the acid, and I(+) are the positively charged (protonated) silicate species. We found that the stronger the ion X(-) is bonded to S(0)H(+), the more it catalyzes the silica condensation into (S(0)H(+))(X(-)I(+)). Br(-) is shown to be a strong binding anion and therefore a fast silica polymerization promoter compared to Cl(-) resulting in the formation of a higher quality mesophase for the Br(-) syntheses. We also showed that the polymerization rate of the silica, dictated by the counterion, controls the morphology of the mesostructures from nonuniform agglomerated blocks in the case of Br(-) syntheses to spherical particles for the Cl(-) syntheses. Next to many benefits such as low temperature, short synthesis time, and the use of inexpensive, nontoxic, and easily extractable amine templates, the developed materials have a remarkable higher thermal and hydrothermal stability compared to hexagonal mesoporous silica, which is also prepared with nonionic amines but formed through the S(0)I(0) mechanism.
Keywords: A1 Journal article; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 3.177
Times cited: 9
DOI: 10.1021/jp026696v
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“Mechanistic Insight into the Photocatalytic Working of Fluorinated Anatase {001} Nanosheets”. Kus M, Altantzis T, Vercauteren S, Caretti I, Leenaerts O, Batenburg KJ, Mertens M, Meynen V, Partoens B, Van Doorslaer S, Bals S, Cool P, The journal of physical chemistry: C : nanomaterials and interfaces 121, 26275 (2017). http://doi.org/10.1021/acs.jpcc.7b05586
Abstract: Anatase nanosheets with exposed {001} facets
have gained increasing interest for photocatalytic applications. To
fully understand the structure-to-activity relation, combined
experimental and computational methods have been exploited.
Anatase nanosheets were prepared under hydrothermal conditions
in the presence of fluorine ions. High resolution scanning
transmission electron microscopy was used to fully characterize
the synthesized material, confirming the TiO2 nanosheet
morphology. Moreover, the surface structure and composition
of a single nanosheet could be determined by annular bright-field
scanning transmission electron microscopy (ABF-STEM) and
STEM electron energy loss spectroscopy (STEM-EELS). The photocatalytic activity was tested for the decomposition of organic
dyes rhodamine 6G and methyl orange and compared to a reference TiO2 anatase sample. The anatase nanosheets with exposed
{001} facets revealed a significantly lower photocatalytic activity compared to the reference. In order to understand the
mechanism for the catalytic performance, and to investigate the role of the presence of F−, light-induced electron paramagnetic
resonance (EPR) experiments were performed. The EPR results are in agreement with TEM, proving the presence of Ti3+
species close to the surface of the sample and allowing the analysis of the photoinduced formation of paramagnetic species.
Further, ab initio calculations of the anisotropic effective mass of electrons and electron holes in anatase show a very high effective
mass of electrons in the [001] direction, having a negative impact on the mobility of electrons toward the {001} surface and thus
the photocatalysis. Finally, motivated by the experimental results that indicate the presence of fluorine atoms at the surface, we
performed ab initio calculations to determine the position of the band edges in anatase slabs with different terminations of the
{001} surface. The presence of fluorine atoms near the surface is shown to strongly shift down the band edges, which indicates
another reason why it can be expected that the prepared samples with a large amount of {001} surface, but with fluorine atoms
near the surface, show only a low photocatalytic activity.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Condensed Matter Theory (CMT); Laboratory of adsorption and catalysis (LADCA)
Impact Factor: 4.536
Times cited: 20
DOI: 10.1021/acs.jpcc.7b05586
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“Coupled plasmon modes in 2D gold nanoparticle clusters and their effect on local temperature control”. Borah R, Verbruggen SW, The journal of physical chemistry: C : nanomaterials and interfaces 123, 30594 (2019). http://doi.org/10.1021/ACS.JPCC.9B09048
Abstract: Assemblies of closely separated gold nanoparticles exhibit a strong collective plasmonic response due to coupling of the plasmon modes of the individual nanostructures. In the context of self-assembly of nanoparticles, close-packed two-dimensional (2D) clusters of spherical nanoparticles present an important composite system that promises numerous applications. The present study probes the collective plasmonic characteristics and resulting photothermal behavior of close-packed 2D Au nanoparticle clusters to delineate the effects of the cluster size, interparticle distance, and particle size. Smaller nanoparticles (20 and 40 nm in diameter) that exhibit low individual scattering and high absorption were considered for their relevance to photothermal applications. In contrast to typical literature studies, the present study compares the optical response of clusters of different sizes ranging from a single nanoparticle up to large assemblies of 61 nanoparticles. Increasing the cluster size induces significant changes to the spectral position and optophysical characteristics. Based on the model outcome, an optimal cluster size for maximum absorption per nanoparticle is also determined for enhanced photothermal effects. The effect of the particle size and interparticle distance is investigated to elucidate the nature of interaction in terms of near-field and far-field coupling. The photothermal effect resulting from absorption is compared for different cluster sizes and interparticle distances considering a homogeneous water medium. A strong dependence of the steady-state temperature of the nanoparticles on the cluster size, particle position in the cluster, incident light polarization, and interparticle distance provides new physical insight into the local temperature control of plasmonic nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 4.536
DOI: 10.1021/ACS.JPCC.9B09048
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“Atomic layer deposition of Ruthenium on Ruthenium surfaces : a theoretical study”. Quan Manh P, Pourtois G, Swerts J, Pierloot K, Delabie A, The journal of physical chemistry: C : nanomaterials and interfaces 119, 6592 (2015). http://doi.org/10.1021/jp5125958
Abstract: Atomic, layer deposition,(ALD of ruthenium using two ruthenium precursors, i.e., Ru(C5H5)(2) (RuCp2) and Ru(C5H5)(C4H4N) (RuCpPy), is studied using density functional theory. By investigating the reaction mechanisms On bare ruthenium surfaces, i.e., (001), (101), and (100), and H-terminated surfaces, an atomistic insight in the Ru ALD is provided. The calculated results show that on the Ru surfaces both RuCp2 and RuCpPy an undergo dehydrogenation and ligand dissociation reactions. RuCpPy is more reactive than RuCp2. By forming a, strong, bond between N of Py and Ru of the surface, RuCpPy can easily chemisorb on the surfaces. The reactions of RuCp2,On the Surfaces are less favorable the adsorption is not strong enough This could be a,factor contributing to the higher growth-per-cycle of Ru using RuCpPy, as observed experimentally. By Studying, the adsorption on H-terminated Ru surfaces, We showed that H Can prevent the adsorption of the precursors, thus inhibiting the growth of Ru. Our calculations indicate that the H content on the surface can have an impact on the growth-per-cycle. Finally, our simulations also demonstrate large impacts of the surface structure on the reaction mechanisms. Of the three surfaces, the (100) surface, which is the less stable and has a zigzag surface structure, is also the most reactive one.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 10
DOI: 10.1021/jp5125958
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“Structural transitions in monolayer MOS2 by lithium adsorption”. Esfahani, Leenaerts O, Sahin H, Partoens B, Peeters FM, The journal of physical chemistry: C : nanomaterials and interfaces 119, 10602 (2015). http://doi.org/10.1021/jp510083w
Abstract: Based on first-principles calculations, we study the structural stability of the H and T phases of monolayer MoS2 upon Li doping. Our calculations demonstrate that it is possible to stabilize a distorted T phase of MoS2 over the H phase through adsorption of Li atoms on the MoS2 surface. Through molecular dynamics and phonon calculations, we show that the T phase of MoS2 is dynamically unstable and undergoes considerable distortions. The type of distortion depends on the concentration of adsorbed Li atoms and changes from zigzag-like to diamond-like when increasing the Li doping. There exists a substantial energy barrier to transform the stable H phase to the distorted T phases, which is considerably reduced by increasing the concentration of Li atoms. We show that it is necessary that the Li atoms adsorb on both sides of the MoS2 monolayer to reduce the barrier sufficiently. Two processes are examined that allow for such two-sided adsorption, namely, penetration through the MoS2 layer and diffusion over the MoS2 surface. We show that while there is only a small barrier of 0.24 eV for surface diffusion, the amount of energy needed to pass through a pure MoS2 layer is of the order of similar or equal to 2 eV. However, when the MoS2 layer is covered with Li atoms the amount of energy that Li atoms should gain to penetrate the layer is drastically reduced and penetration becomes feasible.
Keywords: A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT)
Impact Factor: 4.536
Times cited: 96
DOI: 10.1021/jp510083w
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“Atomic layer deposition of ruthenium on a titanium nitride surface : a density functional theory study”. Phung QM, Vancoillie S, Pourtois G, Swerts J, Pierloot K, Delabie A, The journal of physical chemistry: C : nanomaterials and interfaces 117, 19442 (2013). http://doi.org/10.1021/jp405489w
Abstract: Because of its excellent properties in nanotechnology applications, atomic layer deposition of ruthenium (Ru) has been the subject of numerous experimental studies. Recently, two different Ru precursors were compared for plasma-enhanced atomic layer deposition (PEALD) of Ru, and their reactivity was found to be different. Inhibition was observed for bis(ethylcyclopentadienyl)ruthenium (Ru(EtCp)(2)), while nearly linear growth behavior was observed for (methylcyclopentadienyl-pyrrolyl)ruthenium (Ru(MeCp)Py). To understand this difference in reactivity, we investigate the adsorption of RuCp, and RuCpPy (i.e., without substituents) on a TiN surface using calculations based on periodic boundary conditions density functional theory (DFT) combined with experiments based on Rutherford backscattering spectroscopy (RBS). The calculations demonstrate that the RuCpPy precursor chemisorbs on the TiN(100) surface while the RuCp2 precursor only physisorbs. We propose a reaction mechanism for the chemisorption of RuCpPy. The area density of the calculated RuCpPy surface species is compared with the experimental values from RBS. The impact of a H-plasma is also investigated. The DFT calculations and experimental results from RBS provide insight into the adsorption processes of the RuCpPy and RuCp2 precursors on the TiN(100) surface.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 6
DOI: 10.1021/jp405489w
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“Modeling Plasma-based CO2and CH4Conversion in Mixtures with N2, O2, and H2O: The Bigger Plasma Chemistry Picture”. Wang W, Snoeckx R, Zhang X, Cha MS, Bogaerts A, The journal of physical chemistry: C : nanomaterials and interfaces 122, 8704 (2018). http://doi.org/10.1021/acs.jpcc.7b10619
Abstract: Because of the unique properties of plasma technology, its use in gas conversion applications is gaining significant interest around the globe. Plasma-based CO2 and CH4 conversion has become a major research area. Many investigations have already been performed regarding the single-component gases, that is, CO2 splitting and CH4 reforming, as well as for two-component mixtures, that is, dry reforming of methane
(CO2/CH4), partial oxidation of methane (CH4/O2), artificial photosynthesis (CO2/H2O), CO2 hydrogenation (CO2/H2), and even first steps toward the influence of N2 impurities have been taken, that is, CO2/N2 and CH4/N2. In this Feature Article we briefly discuss the advances made in literature for these different steps from a plasma chemistry modeling point of view. Subsequently, we present a comprehensive plasma chemistry set, combining the knowledge gathered in this field so far and supported with extensive experimental data. This set can be used for chemical kinetics plasma modeling for all possible combinations of CO2, CH4, N2, O2, and H2O to investigate the bigger picture of the underlying plasmachemical pathways for these mixtures in a dielectric barrier discharge plasma. This is extremely valuable
for the optimization of existing plasma-based CO2 conversion and CH4 reforming processes as well as for investigating the influence of N2, O2, and H2O on these processes and even to support plasma-based multireforming processes.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 28
DOI: 10.1021/acs.jpcc.7b10619
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“Bifunctional nickel-nitrogen-doped-carbon-supported copper electrocatalyst for CO2 reduction”. Choukroun D, Daems N, Kenis T, Van Everbroeck T, Hereijgers J, Altantzis T, Bals S, Cool P, Breugelmans T, Journal Of Physical Chemistry C 124, 1369 (2020). http://doi.org/10.1021/ACS.JPCC.9B08931
Abstract: Bifunctionality is a key feature of many industrial catalysts, supported metal clusters and particles in particular, and the development of such catalysts for the CO2 reduction reaction (CO2RR) to hydrocarbons and alcohols is gaining traction in light of recent advancements in the field. Carbon-supported Cu nanoparticles are suitable candidates for integration in the state-of-the-art reaction interfaces, and here, we propose, synthesize, and evaluate a bifunctional Ni–N-doped-C-supported Cu electrocatalyst, in which the support possesses active sites for selective CO2 conversion to CO and Cu nanoparticles catalyze either the direct CO2 or CO reduction to hydrocarbons. In this work, we introduce the scientific rationale behind the concept, its applicability, and the challenges with regard to the catalyst. From the practical aspect, the deposition of Cu nanoparticles onto carbon black and Ni–N–C supports via an ammonia-driven deposition precipitation method is reported and explored in more detail using X-ray diffraction, thermogravimetric analysis, and hydrogen temperature-programmed reduction. High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) and energy-dispersive X-ray spectroscopy (EDXS) give further evidence of the presence of Cu-containing nanoparticles on the Ni–N–C supports while revealing an additional relationship between the nanoparticle’s composition and the electrode’s electrocatalytic performance. Compared to the benchmark carbon black-supported Cu catalysts, Ni–N–C-supported Cu delivers up to a 2-fold increase in the partial C2H4 current density at −1.05 VRHE (C1/C2 = 0.67) and a concomitant 10-fold increase of the CO partial current density. The enhanced ethylene production metrics, obtained by virtue of the higher intrinsic activity of the Ni–N–C support, point out toward a synergistic action between the two catalytic functionalities.
Keywords: A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT); Laboratory of adsorption and catalysis (LADCA); Applied Electrochemistry & Catalysis (ELCAT)
Impact Factor: 3.7
Times cited: 24
DOI: 10.1021/ACS.JPCC.9B08931
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“Stabilities of bimetallic nanoparticles for chirality-selective carbon nanotube growth and the effect of carbon interstitials”. Vets C, Neyts EC, The journal of physical chemistry: C : nanomaterials and interfaces 121, 15430 (2017). http://doi.org/10.1021/ACS.JPCC.7B02880
Abstract: Bimetallic nanoparticles play a crucial role in various applications. A better understanding of their properties would facilitate these applications and possibly even enable chirality-specific growth of carbon nanotubes (CNTs). We here examine the stabilities of NiFe, NiGa, and FeGa nanoparticles and the effect of carbon dissolved in NiFe nanoparticles through density functional theory (DFT) calculations and Born Oppenheimer molecular dynamics (BOMD) simulations. We establish that nanoparticles with more Fe in the core and more Ga on the surface are more stable and compare these results with well-known properties such as surface energy and atom size. Furthermore, we find that the nanoparticles become more stable with increasing carbon content, both at 0 K and at 700 K. These results provide a basis for further research into the chirality-specific growth of CNT's.
Keywords: A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT)
Impact Factor: 4.536
Times cited: 2
DOI: 10.1021/ACS.JPCC.7B02880
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“Silver–Gold Bimetallic Alloy versus Core–Shell Nanoparticles: Implications for Plasmonic Enhancement and Photothermal Applications”. Borah R, Verbruggen SW, Journal Of Physical Chemistry C , acs.jpcc.0c02630 (2020). http://doi.org/10.1021/acs.jpcc.0c02630
Abstract: Bimetallic plasmonic nanoparticles enable tuning of the optical response and chemical stability by variation of the composition. The present numerical simulation study compares Ag–Au alloy, Ag@Au core–shell, and Au@Ag core–shell bimetallic plasmonic nanoparticles of both spherical and anisotropic (nanotriangle and nanorods) shapes. By studying both spherical and anisotropic (with LSPR in the near-infrared region) shapes, cases with and without interband transitions of Au can be decoupled. Explicit comparisons are facilitated by numerical models supported by careful validation and examination of optical constants of Au–Ag alloys reported in the literature. Although both Au–Ag core–shell and alloy nanoparticles exhibit an intermediary optical response between that of pure Ag and Au nanoparticles, there are noticeable differences in the spectral characteristics. Also, the effect of the bimetallic constitution in anisotropic nanoparticles is starkly different from that in spherical nanoparticles due to the absence of Au interband transitions in the former case. In general, the improved chemical stability of Ag nanoparticles by incorporation of Au comes with a cost of reduction in plasmonic enhancement, also applicable to anisotropic nanoparticles with a weaker effect. A photothermal heat transfer study confirms that increased absorption by the incorporation of Au in spherical Ag nanoparticles also results in an increased steady-state temperature. On the other hand, anisotropic nanoparticles are inherently better absorbers and hence better photothermal sources, and their photothermal properties are apparently not strongly affected by the incorporation of one metal in the other. This study of the optical/spectral and photothermal characteristics of bimetallic Au–Ag alloy versus core–shell nanoparticles provides detailed physical insight for development of new taylor-made plasmonic nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3.7
DOI: 10.1021/acs.jpcc.0c02630
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“Silver–Gold Bimetallic Alloy versus Core–Shell Nanoparticles: Implications for Plasmonic Enhancement and Photothermal Applications”. Borah R, Verbruggen SW, Journal Of Physical Chemistry C (2020). http://doi.org/10.1021/acs.jpcc.0c02630
Abstract: Bimetallic plasmonic nanoparticles enable tuning of the optical response and chemical stability by variation of the composition. The present numerical simulation study compares Ag–Au alloy, Ag@Au core–shell, and Au@Ag core–shell bimetallic plasmonic nanoparticles of both spherical and anisotropic (nanotriangle and nanorods) shapes. By studying both spherical and anisotropic (with LSPR in the near-infrared region) shapes, cases with and without interband transitions of Au can be decoupled. Explicit comparisons are facilitated by numerical models supported by careful validation and examination of optical constants of Au–Ag alloys reported in the literature. Although both Au–Ag core–shell and alloy nanoparticles exhibit an intermediary optical response between that of pure Ag and Au nanoparticles, there are noticeable differences in the spectral characteristics. Also, the effect of the bimetallic constitution in anisotropic nanoparticles is starkly different from that in spherical nanoparticles due to the absence of Au interband transitions in the former case. In general, the improved chemical stability of Ag nanoparticles by incorporation of Au comes with a cost of reduction in plasmonic enhancement, also applicable to anisotropic nanoparticles with a weaker effect. A photothermal heat transfer study confirms that increased absorption by the incorporation of Au in spherical Ag nanoparticles also results in an increased steady-state temperature. On the other hand, anisotropic nanoparticles are inherently better absorbers and hence better photothermal sources, and their photothermal properties are apparently not strongly affected by the incorporation of one metal in the other. This study of the optical/spectral and photothermal characteristics of bimetallic Au–Ag alloy versus core–shell nanoparticles provides detailed physical insight for development of new taylor-made plasmonic nanostructures.
Keywords: A1 Journal article; Engineering sciences. Technology; Sustainable Energy, Air and Water Technology (DuEL)
Impact Factor: 3.7
DOI: 10.1021/acs.jpcc.0c02630
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