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Author |
Ben Dkhil, S.; Pfannmöller, M.; Ata, I.; Duche, D.; Gaceur, M.; Koganezawa, T.; Yoshimoto, N.; Simon, J.-J.; Escoubas, L.; Videlot-Ackermann, C.; Margeat, O.; Bals, S.; Bauerle, P.; Ackermann, J. |
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Title |
Time evolution studies of dithieno[3,2-b:2 ',3 '-d] pyrrole-based A-D-A oligothiophene bulk heterojunctions during solvent vapor annealing towards optimization of photocurrent generation |
Type |
A1 Journal article |
| |
Year |
2017 |
Publication |
Journal of materials chemistry A : materials for energy and sustainability |
Abbreviated Journal |
J Mater Chem A |
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Volume |
5 |
Issue |
5 |
Pages |
1005-1013 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Solvent vapor annealing (SVA) is one of the main techniques to improve the morphology of bulk heterojunction solar cells using oligomeric donors. In this report, we study time evolution of nanoscale morphological changes in bulk heterojunctions based on a well-studied dithienopyrrole-based A-D-A oligothiophene (dithieno[3,2-b: 2',3'-d] pyrrole named here 1) blended with [6,6]-phenyl-C-71-butyric acid methyl ester (PC71BM) to increase photocurrent density by combining scanning transmission electron microscopy and low-energy-loss spectroscopy. Our results show that SVA transforms the morphology of 1 : PC71BM blends by a three-stage mechanism: highly intermixed phases evolve into nanostructured bilayers that correspond to an optimal blend morphology. Additional SVA leads to completely phaseseparated micrometer-sized domains. Optical spacers were used to increase light absorption inside optimized 1 : PC71BM blends leading to solar cells of 7.74% efficiency but a moderate photocurrent density of 12.3 mA cm (-2). Quantum efficiency analyses reveal that photocurrent density is mainly limited by losses inside the donor phase. Indeed, optimized 1 : PC71BM blends consist of large donor-enriched domains not optimal for exciton to photocurrent conversion. Shorter SVA times lead to smaller domains; however they are embedded in large mixed phases suggesting that introduction of stronger molecular packing may help us to better balance phase separation and domain size enabling more efficient bulk heterojunction solar cells. |
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Corporate Author |
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Thesis |
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Place of Publication  |
Cambridge |
Editor |
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Language |
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Wos |
000394430800018 |
Publication Date |
2016-11-30 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2050-7488; 2050-7496 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.867 |
Times cited |
19 |
Open Access |
Not_Open_Access |
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Notes |
; We acknowledge financial support by the French Fond Unique Interministeriel (FUI) under the project “SFUMATO” (Grant number: F1110019V/201308815) as well as by the European Commission under the Project “SUNFLOWER” (FP7-ICT-2011-7, Grant number: 287594). The synchrotron radiation experiments were performed at BL19B2 in SPring-8 with the approval of Japan Synchrotron Radiation Research Institute (JASRI) (Proposal No. 2016A1568). We further acknowledge financial support via ERC Starting Grant Colouratoms (335078). ; |
Approved |
Most recent IF: 8.867 |
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Call Number |
UA @ lucian @ c:irua:142602UA @ admin @ c:irua:142602 |
Serial |
4695 |
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Author |
Aierken, Y.; Sevik, C.; Gulseren, O.; Peeters, F.M.; Çakir, D. |
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Title |
MXenes/graphene heterostructures for Li battery applications : a first principles study |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Journal of materials chemistry A : materials for energy and sustainability |
Abbreviated Journal |
J Mater Chem A |
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| |
Volume |
6 |
Issue |
5 |
Pages |
2337-2345 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Condensed Matter Theory (CMT) |
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Abstract |
MXenes are the newest class of two-dimensional (2D) materials, and they offer great potential in a wide range of applications including electronic devices, sensors, and thermoelectric and energy storage materials. In this work, we combined the outstanding electrical conductivity, that is essential for battery applications, of graphene with MXene monolayers (M2CX2 where M = Sc, Ti, V and X = OH, O) to explore its potential in Li battery applications. Through first principles calculations, we determined the stable stacking configurations of M2CX2/graphene bilayer heterostructures and their Li atom intercalation by calculating the Li binding energy, diffusion barrier and voltage. We found that: (1) for the ground state stacking, the interlayer binding is strong, yet the interlayer friction is small; (2) Li binds more strongly to the O-terminated monolayer, bilayer and heterostructure MXene systems when compared with the OHterminated MXenes due to the H+ induced repulsion to the Li atoms. The binding energy of Li decreases as the Li concentration increases due to enhanced repulsive interaction between the positively charged Li ions; (3) Ti2CO2/graphene and V2CO2/graphene heterostructures exhibit large Li atom binding energies making them the most promising candidates for battery applications. When fully loaded with Li atoms, the binding energy is -1.43 eV per Li atom and -1.78 eV per Li atom for Ti2CO2/graphene and V2CO2/graphene, respectively. These two heterostructures exhibit a nice compromise between storage capacity and kinetics. For example, the diffusion barrier of Li in Ti2CO2/graphene is around 0.3 eV which is comparable to that of graphite. Additionally, the calculated average voltages are 1.49 V and 1.93 V for Ti2CO2/graphene and V2CO2/graphene structures, respectively; (4) a small change in the in-plane lattice parameters (<1%), interatomic bond lengths and interlayer distances (<0.5 angstrom) proves the stability of the heterostructures against Li intercalation, and the impending phase separation into constituent layers and capacity fading during charge-discharge cycles in real battery applications; (5) as compared to bare M2CX2 bilayers, M2CX2/graphene heterostructures have lower molecular mass, offering high storage capacity; (6) the presence of graphene ensures good electrical conductivity that is essential for battery applications. Given these advantages, Ti2CO2/graphene and V2CO2/graphene heterostructures are predicted to be promising for lithium-ion battery applications. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Cambridge |
Editor |
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Language |
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Wos |
000423981200049 |
Publication Date |
2018-01-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
2050-7488; 2050-7496 |
ISBN |
|
Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
8.867 |
Times cited |
131 |
Open Access |
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Notes |
; This work was supported by the bilateral project between the Scientific and Technological Research Council of Turkey (TUBITAK) and FWO-Flanders, Flemish Science Foundation (FWO-Vl) and the Methusalem foundation of the Flemish government. Computational resources were provided by the TUBITAK ULAKBIM, High Performance and Grid Computing Center (TRGrid e-Infrastructure), and HPC infrastructure of the University of Antwerp (CalcUA) a division of the Flemish Supercomputer Center (VSC), which is funded by the Hercules foundation. We acknowledge the support from the TUBITAK (Grant No. 115F024 and 116F080). Part of this work was supported by the BAGEP Award of the Science Academy. ; |
Approved |
Most recent IF: 8.867 |
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| |
Call Number |
UA @ lucian @ c:irua:149265UA @ admin @ c:irua:149265 |
Serial |
4945 |
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Author |
Delmelle, R.; Amin-Ahmadi, B.; Sinnaeve, M.; Idrissi, H.; Pardoen, T.; Schryvers, D.; Proost, J. |
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Title |
Effect of structural defects on the hydriding kinetics of nanocrystalline Pd thin films |
Type |
A1 Journal article |
| |
Year |
2015 |
Publication |
International journal of hydrogen energy |
Abbreviated Journal |
Int J Hydrogen Energ |
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| |
Volume |
40 |
Issue |
40 |
Pages |
7335-7347 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
While the microstructure of a metal is well-known to affect its equilibrium hydrogen uptake and therefore the hydriding thermodynamics, microstructural effects on the hydriding kinetics are much less documented. Moreover, for thin film systems, such microstructural effects are difficult to separate from the internal stress effect, since most defects generate internal stresses. Such a decoupling has been achieved in this paper for nanocrystalline Pd thin film model systems through the use of a high-resolution, in-situ curvature measurement set-up during Pd deposition, annealing and hydriding. This set-up allowed producing Pd thin films with similar internal stress levels but significantly different microstructures. This was evidenced from detailed defect statistics obtained by transmission electron microscopy, which showed that the densities of grain boundaries, dislocations and twin boundaries have all been lowered by annealing. The same set-up was then used to study the hydriding equilibrium and kinetic behaviour of the resulting films at room temperature. A full quantitative analysis of their hydriding cycles showed that the rate constants of both the adsorption- and absorption-limited kinetic regimes were strongly affected by microstructure. Defect engineering was thereby shown to increase the rate constants for hydrogen adsorption and absorption in Pd by a factor 40 and 30, respectively. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Oxford |
Editor |
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Language |
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Wos |
000355884300012 |
Publication Date |
2015-05-02 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0360-3199; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.582 |
Times cited |
13 |
Open Access |
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Notes |
Iap 7/21 |
Approved |
Most recent IF: 3.582; 2015 IF: 3.313 |
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Call Number |
c:irua:126429 |
Serial |
838 |
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| Permanent link to this record |
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Author |
Pasquini, L.; Sacchi, M.; Brighi, M.; Boelsma, C.; Bals, S.; Perkisas, T.; Dam, B. |
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Title |
Hydride destabilization in core-shell nanoparticles |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
International journal of hydrogen energy |
Abbreviated Journal |
Int J Hydrogen Energ |
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Volume |
39 |
Issue |
5 |
Pages |
2115-2123 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
We present a model that describes the effect of elastic constraint on the thermodynamics of hydrogen absorption and desorption in biphasic core-shell nanoparticles, where the core is a hydride forming metal. In particular, the change of the hydride formation enthalpy and of the equilibrium pressure for the metal/hydride transformation are described as a function of nanoparticles radius, shell thickness, and elastic properties of both core and shell. To test the model, the hydrogen sorption isotherms of Mg-MgO core-shell nanoparticles, synthesized by inert gas condensation, were measured by means of optical hydrogenography. The model's predictions are in good agreement with the experimentally determined plateau pressure of hydrogen absorption. The features that a core-shell systems should exhibit in view of practical hydrogen storage applications are discussed with reference to the model and the experimental results. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved. |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Oxford |
Editor |
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Language |
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Wos |
000331344800022 |
Publication Date |
2014-01-04 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0360-3199; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.582 |
Times cited |
32 |
Open Access |
Not_Open_Access |
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| |
Notes |
COST Action MP1103 |
Approved |
Most recent IF: 3.582; 2014 IF: 3.313 |
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Call Number |
UA @ lucian @ c:irua:115785 |
Serial |
1528 |
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Author |
Snoeckx, R.; Setareh, M.; Aerts, R.; Simon, P.; Maghari, A.; Bogaerts, A. |
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Title |
Influence of N2 concentration in a CH4/N2 dielectric barrier discharge used for CH4 conversion into H2 |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
International journal of hydrogen energy |
Abbreviated Journal |
Int J Hydrogen Energ |
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Volume |
38 |
Issue |
36 |
Pages |
16098-16120 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Plasma Lab for Applications in Sustainability and Medicine – Antwerp (PLASMANT) |
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Abstract |
We present a combined study of experimental and computational work for a dielectric barrier discharge (DBD) used for CH4 conversion into H2. More specifically, we investigated the influence of N2 as an impurity (150,000 ppm) and as additive gas (199%) on the CH4 conversion and H2 yield. For this purpose, a zero-dimensional chemical kinetics model is applied to study the plasma chemistry. The calculated conversions and yields for various gas mixing ratios are compared to the obtained experimental values, and good agreement is achieved. The study reveals the significance of the View the MathML source and View the MathML source metastable states for the CH4 conversion into H2, based on a kinetic analysis of the reaction chemistry. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Oxford |
Editor |
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Language |
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Wos |
000327904500027 |
Publication Date |
2013-10-23 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0360-3199; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.582 |
Times cited |
40 |
Open Access |
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Notes |
|
Approved |
Most recent IF: 3.582; 2013 IF: 2.930 |
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Call Number |
UA @ lucian @ c:irua:111372 |
Serial |
1642 |
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Author |
Simon, Q.; Barreca, D.; Bekermann, D.; Gasparotto, A.; Maccato, C.; Comini, E.; Gombac, V.; Fornasiero, P.; Lebedev, O.I.; Turner, S.; Devi, A.; Fischer, R.A.; Van Tendeloo, G. |
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Title |
Plasma-assisted synthesis of Ag/ZnO nanocomposites : first example of photo-induced H2 production and sensing |
Type |
A1 Journal article |
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Year |
2011 |
Publication |
International journal of hydrogen energy |
Abbreviated Journal |
Int J Hydrogen Energ |
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Volume |
36 |
Issue |
24 |
Pages |
15527-15537 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Ag/ZnO nanocomposites were developed by a plasma-assisted approach. The adopted strategy exploits the advantages of Plasma Enhanced-Chemical Vapor Deposition (PE-CVD) for the growth of columnar ZnO arrays on Si(100) and Al2O3 substrates, in synergy with the infiltration power of the Radio Frequency (RF)-sputtering technique for the subsequent dispersion of different amounts of Ag nanoparticles (NPs). The resulting composites, both as-prepared and after annealing in air, were thoroughly characterized with particular attention on their morphological organization, structure and composition. For the first time, the above systems have been used as catalysts in the production of hydrogen by photo-reforming of alcoholic solutions, yielding a stable H2 evolution even by the sole use of simulated solar radiation. In addition, Ag/ZnO nanocomposites presented an excellent response in the gas-phase detection of H2, opening attractive perspectives for advanced technological applications. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Oxford |
Editor |
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Language |
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Wos |
000297089700006 |
Publication Date |
2011-10-14 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0360-3199; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.582 |
Times cited |
62 |
Open Access |
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Notes |
Esteem 026019; Fwo |
Approved |
Most recent IF: 3.582; 2011 IF: 4.054 |
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Call Number |
UA @ lucian @ c:irua:91901 |
Serial |
2627 |
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Author |
Mooij, L.; Perkisas, T.; Palsson, G.; Schreuders, H.; Wolff, M.; Hjorvarsson, B.; Bals, S.; Dam, B. |
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Title |
The effect of microstructure on the hydrogenation of Mg/Fe thin film multilayers |
Type |
A1 Journal article |
| |
Year |
2014 |
Publication |
International journal of hydrogen energy |
Abbreviated Journal |
Int J Hydrogen Energ |
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Volume |
39 |
Issue |
30 |
Pages |
17092-17103 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Nanoconfined magnesium hydride can be simultaneously protected and thermodynamically destabilized when interfaced with materials such as Ti and Fe. We study the hydrogenation of thin layers of Mg (<14 nm) nanoconfined in one dimension within thin film Fe/Mg/Fe/Pd multilayers by the optical technique Hydrogenography. The hydrogenation of nanosized magnesium layers in Fe/Mg/Fe multilayers surprisingly shows the presence of multiple plateau pressures, whose nature is thickness dependent. In contrast, hydrogen desorption occurs via a single plateau which does not depend on the Mg layer thickness. From structural and morphological analyses with X-ray diffraction/reflectometry and cross-section TEM, we find that the Mg layer roughness is large when deposited on Fe and furthermore contains high-angle grain boundaries (GB's). When grown on Ti, the Mg layer roughness is low and no high-angle GB's are detected. From a Ti/Mg/Fe multilayer, in which the Mg layer is flat and has little or no GB's, we conclude that MgH2 is indeed destabilized by the interface with Fe. In this case, both the ab- and desorption plateau pressures are increased by a factor two compared to the hydrogenation of Mg within Ti/Mg/Ti multilayers. We hypothesize that the GB's in the Fe/Mg/Fe multilayer act as diffusion pathways for Pd, which is known to greatly alter the hydrogenation behavior of Mg when the two materials share an interface. Copyright (C) 2014, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
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Place of Publication |
Oxford |
Editor |
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Language |
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Wos |
000343839000031 |
Publication Date |
2014-09-10 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0360-3199; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.582 |
Times cited |
15 |
Open Access |
Not_Open_Access |
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Notes |
COST Action MP1103 |
Approved |
Most recent IF: 3.582; 2014 IF: 3.313 |
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Call Number |
UA @ lucian @ c:irua:121175 |
Serial |
3575 |
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Author |
Callini, E.; Aguey-Zinsou, K.F.; Ahuja, R.; Ares, J.R.; Bals, S.; Biliškov, N.; Chakraborty, S.; Charalambopoulou, G.; Chaudhary, A.L.; Cuevas, F.; Dam, B.; de Jongh, P.; Dornheim, M.; Filinchuk, Y.; Grbović Novaković, J.; Hirscher, M.; Jensen, T.R.; Jensen, P.B.; Novaković, N.; Lai, Q.; Leardini, F.; Gattia, D.M.; Pasquini, L.; Steriotis, T.; Turner, S.; Vegge, T.; Züttel, A.; Montone, A. |
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Title |
Nanostructured materials for solid-state hydrogen storage : a review of the achievement of COST Action MP1103 |
Type |
A1 Journal article |
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Year |
2016 |
Publication |
International journal of hydrogen energy
T2 – E-MRS Fall Meeting / Symposium C on Hydrogen Storage in Solids -, Materials, Systems and Aplication Trends, SEP 15-18, 2015, Warsaw, POLAND |
Abbreviated Journal |
Int J Hydrogen Energ |
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Volume |
41 |
Issue |
41 |
Pages |
14404-14428 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
In the framework of the European Cooperation in Science and Technology (COST) Action MP1103 Nanostructured Materials for Solid-State Hydrogen Storage were synthesized, characterized and modeled. This Action dealt with the state of the art of energy storage and set up a competitive and coordinated network capable to define new and unexplored ways for Solid State Hydrogen Storage by innovative and interdisciplinary research within the European Research Area. An important number of new compounds have been synthesized: metal hydrides, complex hydrides, metal halide ammines and amidoboranes. Tuning the structure from bulk to thin film, nanoparticles and nanoconfined composites improved the hydrogen sorption properties and opened the perspective to new technological applications. Direct imaging of the hydrogenation reactions and in situ measurements under operando conditions have been carried out in these studies. Computational screening methods allowed the prediction of suitable compounds for hydrogen storage and the modeling of the hydrogen sorption reactions on mono-, bi-, and three-dimensional systems. This manuscript presents a review of the main achievements of this Action. (C) 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved. |
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Address |
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Corporate Author |
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Thesis |
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Publisher |
Pergamon-elsevier science ltd |
Place of Publication |
Oxford |
Editor |
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Language |
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Wos |
000381950800051 |
Publication Date |
2016-05-08 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
0360-3199 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.582 |
Times cited |
89 |
Open Access |
Not_Open_Access |
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Notes |
All the authors greatly thank the COST Action MP1103 for financial support. |
Approved |
Most recent IF: 3.582 |
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Call Number |
UA @ lucian @ c:irua:135723 |
Serial |
4307 |
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Author |
Lutz, L.; Corte, D.A.D.; Chen, Y.; Batuk, D.; Johnson, L.R.; Abakumov, A.; Yate, L.; Azaceta, E.; Bruce, P.G.; Tarascon, J.-M.; Grimaud, A. |
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Title |
The role of the electrode surface in Na-Air batteries : insights in electrochemical product formation and chemical growth of NaO2 |
Type |
A1 Journal article |
| |
Year |
2018 |
Publication |
Advanced energy materials |
Abbreviated Journal |
Adv Energy Mater |
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Volume |
8 |
Issue |
4 |
Pages |
1701581 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The Na-air battery, because of its high energy density and low charging overpotential, is a promising candidate for low-cost energy storage, hence leading to intensive research. However, to achieve such a battery, the role of the positive electrode material in the discharge process must be understood. This issue is herein addressed by exploring the electrochemical reduction of oxygen, as well as the chemical formation and precipitation of NaO2 using different electrodes. Whereas a minor influence of the electrode surface is demonstrated on the electrochemical formation of NaO2, a strong dependence of the subsequent chemical precipitation of NaO2 is identified. In the origin, this effect stems from the surface energy and O-2/O-2(-) affinity of the electrode. The strong interaction of Au with O-2/O-2(-) increases the nucleation rate and leads to an altered growth process when compared to C surfaces. Consequently, thin (3 mu m) flakes of NaO2 are found on Au, whereas on C large cubes (10 mu m) of NaO2 are formed. This has significant impact on the cell performance and leads to four times higher capacity when C electrodes with low surface energy and O-2/O-2(-) affinity are used. It is hoped that these findings will enable the design of new positive electrode materials with optimized surfaces. |
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Corporate Author |
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Thesis |
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Publisher |
WILEY-VCH Verlag GmbH & Co. |
Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000424152200009 |
Publication Date |
2017-09-25 |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1614-6832; 1614-6840 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.721 |
Times cited |
13 |
Open Access |
Not_Open_Access |
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Notes |
; L.L. thanks ALISTORE-ERI for his PhD grant. P.G.B. is indebted to the EPSRC for financial support, including the Supergen Energy Storage grant. ; |
Approved |
Most recent IF: 16.721 |
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Call Number |
UA @ lucian @ c:irua:149269 |
Serial |
4951 |
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Author |
Dimitrievska, M.; Shea, P.; Kweon, K.E.; Bercx, M.; Varley, J.B.; Tang, W.S.; Skripov, A.V.; Stavila, V.; Udovic, T.J.; Wood, B.C. |
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Title |
Carbon Incorporation and Anion Dynamics as Synergistic Drivers for Ultrafast Diffusion in Superionic LiCB11H12 and NaCB11H12 |
Type |
A1 Journal article |
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Year |
2018 |
Publication |
Advanced energy materials |
Abbreviated Journal |
Adv Energy Mater |
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Volume |
8 |
Issue |
15 |
Pages |
1703422 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
The disordered phases of LiCB11H12 and NaCB11H12 possess superb superionic conductivities that make them suitable as solid electrolytes. In these materials, cation diffusion correlates with high orientational mobilities of the CB11H12- anions; however, the precise relationship has yet to be demonstrated. In this work, ab initio molecular dynamics and quasielastic neutron scattering are combined to probe anion reorientations and their mechanistic connection to cation mobility over a range of timescales and temperatures. It is found that anions do not rotate freely, but rather transition rapidly between orientations defined by the cation sublattice symmetry. The symmetry-breaking carbon atom in CB11H12- also plays a critical role by perturbing the energy landscape along the instantaneous orientation of the anion dipole, which couples fluctuations in the cation probability density directly to the anion motion. Anion reorientation rates exceed 3 x 10(10) s(-1), suggesting the underlying energy landscape fluctuates dynamically on diffusion-relevant timescales. Furthermore, carbon is found to modify the orientational preferences of the anions and aid rotational mobility, creating additional symmetry incompatibilities that inhibit ordering. The results suggest that synergy between the anion reorientational dynamics and the carbon-modified cation-anion interaction accounts for the higher ionic conductivity in CB11H12- salts compared with B12H122-. |
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Corporate Author |
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Publisher |
WILEY-VCH Verlag GmbH & Co. |
Place of Publication |
Weinheim |
Editor |
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Language |
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Wos |
000434031400026 |
Publication Date |
2018-02-21 |
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Series Editor |
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Series Title |
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Abbreviated Series Title |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1614-6832; 1614-6840 |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
16.721 |
Times cited |
20 |
Open Access |
OpenAccess |
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Notes |
; This work was performed in part under the auspices of the U.S. Department of Energy at Lawrence Livermore National Laboratory (LLNL) under Contract No. DE-AC52-07NA27344 and funded by Laboratory Directed Research and Development Grant 15-ERD-022. Computing support came from the LLNL Institutional Computing Grand Challenge program. This work was also performed in part within the assignment of the Russian Federal Agency of Scientific Organizations (program “Spin” No. 01201463330). The authors gratefully acknowledge support from the Russian Foundation for Basic Research under Grant No. 15-03-01114 and the Ural Branch of the Russian Academy of Sciences under Grant No. 15-9-2-9. A.V.S. gratefully acknowledges travel support from CRDF Global in conjunction with this work under Grant No. FSCX-15-61826-0. M.D. gratefully acknowledges research support from the Hydrogen Materials-Advanced Research Consortium (HyMARC), established as part of the Energy Materials Network under the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office, under Contract No. DE-AC36-08GO28308. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy National Nuclear Security Administration under Contract No. DE-AC04-94AL85000. This work utilized facilities supported in part by the National Science Foundation under Agreement No. DMR-1508249. The views, opinions, findings, and conclusions stated herein are those of the authors and do not necessarily reflect those of CRDF Global, or the United States Government or any agency thereof. Neither the United States Government nor any agency thereof, nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. ; |
Approved |
Most recent IF: 16.721 |
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| |
Call Number |
UA @ lucian @ c:irua:152045 |
Serial |
5015 |
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| Permanent link to this record |
