Lithium-ion batteries and fuel cells - research and development

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Lithium-ion batteries and fuel cells - research and development (en)
Литијум-јон батерије и горивне ћелије-истраживање и развој (sr)
Litijum-jon baterije i gorivne ćelije-istraživanje i razvoj (sr_RS)
Authors

Publications

Composition, structure and potential energy application of nitrogen doped carbon cryogels

Kalijadis, Ana; Gavrilov, Nemanja M.; Jokić, Bojan M.; Gilić, Martina; Krstić, Aleksandar D.; Pašti, Igor A.; Babić, Biljana M.

(2020)

TY  - JOUR
AU  - Kalijadis, Ana
AU  - Gavrilov, Nemanja M.
AU  - Jokić, Bojan M.
AU  - Gilić, Martina
AU  - Krstić, Aleksandar D.
AU  - Pašti, Igor A.
AU  - Babić, Biljana M.
PY  - 2020
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5887
AB  - Resorcinol–formaldehyde (RF) cryogels were synthesized by sol–gel polycondensation of resorcinol with formaldehyde and freeze-drying was carried out with t-butanol. Carbon cryogel (CC) was obtained by pyrolyzing RF cryogels in an inert atmosphere to 950 °C. Nitrogen doped CCs (CCN) were synthesized by introducing melamine into RF precursor mixture solution to obtain nitrogen concentration 2, 6 and 10 wt.%. Material was characterized by elemental analysis, nitrogen adsorption– desorption measurements, scanning electron microscopy (SEM), Raman spectroscopy, FT-IR Spectroscopy. Cyclic voltammetry (CV) was used to investigate capacitive and electrocatalytic properties. Conductivity measurement was also performed. Elemental analysis results confirmed presence of nitrogen in CCN samples in the range from 0.45 to 1.15 wt.%. Raman spectroscopy of the samples showed increase of D and G peak integrated intensity ratio (ID/IG) with nitrogen doping suggesting that the structural disorder as well as edge plane density increase, but according to similar ID/IG values for CCN samples, their share is not directly related to the amount of incorporated N. Characterization by nitrogen adsorption showed that overall specific surface and maximum mesopores are achieved in CCN sample with medium nitrogen concentration. Results of cyclic voltammetry experiments demonstrated maximum capacitance for CCN sample with smallest N wt.% indicating that narrow pore size distribution and high specific surface area are dominant factors to achieve good capacitive behavior. The relatively low doping level of nitrogen reached in CCN samples may be the reason for the incomplete reduction of oxygen to hydroxide and furthermore it turned out that presence of N in the structure of CC had a negligible effect on the otherwise relatively high conductivity of CC. © 2019 Elsevier B.V.
T2  - Materials Chemistry and Physics
T1  - Composition, structure and potential energy application of nitrogen doped carbon cryogels
SP  - 122120
VL  - 239
DO  - 10.1016/j.matchemphys.2019.122120
ER  - 
@article{
author = "Kalijadis, Ana and Gavrilov, Nemanja M. and Jokić, Bojan M. and Gilić, Martina and Krstić, Aleksandar D. and Pašti, Igor A. and Babić, Biljana M.",
year = "2020",
abstract = "Resorcinol–formaldehyde (RF) cryogels were synthesized by sol–gel polycondensation of resorcinol with formaldehyde and freeze-drying was carried out with t-butanol. Carbon cryogel (CC) was obtained by pyrolyzing RF cryogels in an inert atmosphere to 950 °C. Nitrogen doped CCs (CCN) were synthesized by introducing melamine into RF precursor mixture solution to obtain nitrogen concentration 2, 6 and 10 wt.%. Material was characterized by elemental analysis, nitrogen adsorption– desorption measurements, scanning electron microscopy (SEM), Raman spectroscopy, FT-IR Spectroscopy. Cyclic voltammetry (CV) was used to investigate capacitive and electrocatalytic properties. Conductivity measurement was also performed. Elemental analysis results confirmed presence of nitrogen in CCN samples in the range from 0.45 to 1.15 wt.%. Raman spectroscopy of the samples showed increase of D and G peak integrated intensity ratio (ID/IG) with nitrogen doping suggesting that the structural disorder as well as edge plane density increase, but according to similar ID/IG values for CCN samples, their share is not directly related to the amount of incorporated N. Characterization by nitrogen adsorption showed that overall specific surface and maximum mesopores are achieved in CCN sample with medium nitrogen concentration. Results of cyclic voltammetry experiments demonstrated maximum capacitance for CCN sample with smallest N wt.% indicating that narrow pore size distribution and high specific surface area are dominant factors to achieve good capacitive behavior. The relatively low doping level of nitrogen reached in CCN samples may be the reason for the incomplete reduction of oxygen to hydroxide and furthermore it turned out that presence of N in the structure of CC had a negligible effect on the otherwise relatively high conductivity of CC. © 2019 Elsevier B.V.",
journal = "Materials Chemistry and Physics",
title = "Composition, structure and potential energy application of nitrogen doped carbon cryogels",
pages = "122120",
volume = "239",
doi = "10.1016/j.matchemphys.2019.122120"
}
Kalijadis, A., Gavrilov, N. M., Jokić, B. M., Gilić, M., Krstić, A. D., Pašti, I. A.,& Babić, B. M.. (2020). Composition, structure and potential energy application of nitrogen doped carbon cryogels. in Materials Chemistry and Physics, 239, 122120.
https://doi.org/10.1016/j.matchemphys.2019.122120
Kalijadis A, Gavrilov NM, Jokić BM, Gilić M, Krstić AD, Pašti IA, Babić BM. Composition, structure and potential energy application of nitrogen doped carbon cryogels. in Materials Chemistry and Physics. 2020;239:122120.
doi:10.1016/j.matchemphys.2019.122120 .
Kalijadis, Ana, Gavrilov, Nemanja M., Jokić, Bojan M., Gilić, Martina, Krstić, Aleksandar D., Pašti, Igor A., Babić, Biljana M., "Composition, structure and potential energy application of nitrogen doped carbon cryogels" in Materials Chemistry and Physics, 239 (2020):122120,
https://doi.org/10.1016/j.matchemphys.2019.122120 . .
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The influence of synthesis conditions on the redox behaviour of LiFePO4 in aqueous solution

Georgijević, Radovan; Vujković, Milica; Gutić, Sanjin J.; Aliefendić, Meho; Jugović, Dragana; Mitrić, Miodrag; Đokić, Veljko; Mentus, Slavko

(Elsevier Science Sa, Lausanne, 2019)

TY  - JOUR
AU  - Georgijević, Radovan
AU  - Vujković, Milica
AU  - Gutić, Sanjin J.
AU  - Aliefendić, Meho
AU  - Jugović, Dragana
AU  - Mitrić, Miodrag
AU  - Đokić, Veljko
AU  - Mentus, Slavko
PY  - 2019
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/4329
AB  - To contribute to the knowledge on the influence of synthesis procedure on the intercalation kinetics of lithium ions into phospho-olivines, LiFePO4/C composite samples (LFPC) were synthesized in two ways, the first one in a sol-gel procedure (SG), and the other in a solid-state reaction (SS). The X-ray diffractograms (XRD) of both samples overlapped with that of pure LiFePO4, taken from the crystallographic database. Scanning electron microscopy pictures indicated the high degree of interparticle sintering, which caused a considerable agglomerate growth. The results of potentiodynamic measurements in aqueous LiNO3 solution revealed that for SS sample, three times higher initial capacity from that of SG one, (amounting to 74 mAh g(-1) at 5 mV s(-1)). However, capacity fade on rising scan rate is much more expressed for SS sample than for SG one. We suggest that a different degree of material utilization due to the incomplete coverage of olivine particles by carbon explains this difference. The technique of separation of diffusion and capacitance currents was applied in a kinetic analysis, but it was shown to be inappropriate. We suggest the inapplicability of classic CV theory to the intercalation system accompanied by phase transition. Instead, a model of ohmic resistance determination of process kinetics was considered. LFPC-SS sample delivers three times larger capacity in LiNO3, amounting to 74 mAh g(-1) at 1 mV s(-1).
PB  - Elsevier Science Sa, Lausanne
T2  - Journal of Alloys and Compounds
T1  - The influence of synthesis conditions on the redox behaviour of LiFePO4 in aqueous solution
EP  - 485
SP  - 475
VL  - 776
DO  - 10.1016/j.jallcom.2018.10.246
ER  - 
@article{
author = "Georgijević, Radovan and Vujković, Milica and Gutić, Sanjin J. and Aliefendić, Meho and Jugović, Dragana and Mitrić, Miodrag and Đokić, Veljko and Mentus, Slavko",
year = "2019",
abstract = "To contribute to the knowledge on the influence of synthesis procedure on the intercalation kinetics of lithium ions into phospho-olivines, LiFePO4/C composite samples (LFPC) were synthesized in two ways, the first one in a sol-gel procedure (SG), and the other in a solid-state reaction (SS). The X-ray diffractograms (XRD) of both samples overlapped with that of pure LiFePO4, taken from the crystallographic database. Scanning electron microscopy pictures indicated the high degree of interparticle sintering, which caused a considerable agglomerate growth. The results of potentiodynamic measurements in aqueous LiNO3 solution revealed that for SS sample, three times higher initial capacity from that of SG one, (amounting to 74 mAh g(-1) at 5 mV s(-1)). However, capacity fade on rising scan rate is much more expressed for SS sample than for SG one. We suggest that a different degree of material utilization due to the incomplete coverage of olivine particles by carbon explains this difference. The technique of separation of diffusion and capacitance currents was applied in a kinetic analysis, but it was shown to be inappropriate. We suggest the inapplicability of classic CV theory to the intercalation system accompanied by phase transition. Instead, a model of ohmic resistance determination of process kinetics was considered. LFPC-SS sample delivers three times larger capacity in LiNO3, amounting to 74 mAh g(-1) at 1 mV s(-1).",
publisher = "Elsevier Science Sa, Lausanne",
journal = "Journal of Alloys and Compounds",
title = "The influence of synthesis conditions on the redox behaviour of LiFePO4 in aqueous solution",
pages = "485-475",
volume = "776",
doi = "10.1016/j.jallcom.2018.10.246"
}
Georgijević, R., Vujković, M., Gutić, S. J., Aliefendić, M., Jugović, D., Mitrić, M., Đokić, V.,& Mentus, S.. (2019). The influence of synthesis conditions on the redox behaviour of LiFePO4 in aqueous solution. in Journal of Alloys and Compounds
Elsevier Science Sa, Lausanne., 776, 475-485.
https://doi.org/10.1016/j.jallcom.2018.10.246
Georgijević R, Vujković M, Gutić SJ, Aliefendić M, Jugović D, Mitrić M, Đokić V, Mentus S. The influence of synthesis conditions on the redox behaviour of LiFePO4 in aqueous solution. in Journal of Alloys and Compounds. 2019;776:475-485.
doi:10.1016/j.jallcom.2018.10.246 .
Georgijević, Radovan, Vujković, Milica, Gutić, Sanjin J., Aliefendić, Meho, Jugović, Dragana, Mitrić, Miodrag, Đokić, Veljko, Mentus, Slavko, "The influence of synthesis conditions on the redox behaviour of LiFePO4 in aqueous solution" in Journal of Alloys and Compounds, 776 (2019):475-485,
https://doi.org/10.1016/j.jallcom.2018.10.246 . .
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The influence of fluorine doping on the structural and electrical properties of the LiFePO4 powder

Jugović, Dragana; Mitrić, Miodrag; Milović, Miloš; Cvjetićanin, Nikola; Jokić, Bojan; Umićević, Ana; Uskoković, Dragan

(Elsevier, 2017)

TY  - JOUR
AU  - Jugović, Dragana
AU  - Mitrić, Miodrag
AU  - Milović, Miloš
AU  - Cvjetićanin, Nikola
AU  - Jokić, Bojan
AU  - Umićević, Ana
AU  - Uskoković, Dragan
PY  - 2017
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5856
AB  - Low intrinsic electronic conductivity is the main disadvantage of LiFePO4 when used as a cathode material in lithium ion batteries. The paper offers experimental proofs of the theoretical prediction that fluorine doping of LiFePO4 can enhance its electrical conductivity. The LiFePO4 and fluorine-doped LiFePO4 olivine type, carbon-free powders are synthesized and examined. The crystal structure refinements in the Pnma space group reveal that doping with fluorine ions preserves the olivine structure, while reducing both the lattice parameters and the antisite defect, and increasing the crystallite size. A small amount of incorporated fluorine enhances the electrical conductivity from 4.6×10−7 S cm−1 to 2.3×10−6 S cm−1 and has a positive impact on the electrochemical performance. Several spectroscopy techniques (Mössbauer, FTIR, and Raman) reveal differences between the two powders and additionally support the findings of both the Rietveld refinement and the conductivity measurements.
PB  - Elsevier
T2  - Ceramics International
T1  - The influence of fluorine doping on the structural and electrical properties of the LiFePO4 powder
EP  - 3230
IS  - 3
SP  - 3224
VL  - 43
DO  - 10.1016/j.ceramint.2016.11.149
UR  - https://hdl.handle.net/21.15107/rcub_dais_2352
ER  - 
@article{
author = "Jugović, Dragana and Mitrić, Miodrag and Milović, Miloš and Cvjetićanin, Nikola and Jokić, Bojan and Umićević, Ana and Uskoković, Dragan",
year = "2017",
abstract = "Low intrinsic electronic conductivity is the main disadvantage of LiFePO4 when used as a cathode material in lithium ion batteries. The paper offers experimental proofs of the theoretical prediction that fluorine doping of LiFePO4 can enhance its electrical conductivity. The LiFePO4 and fluorine-doped LiFePO4 olivine type, carbon-free powders are synthesized and examined. The crystal structure refinements in the Pnma space group reveal that doping with fluorine ions preserves the olivine structure, while reducing both the lattice parameters and the antisite defect, and increasing the crystallite size. A small amount of incorporated fluorine enhances the electrical conductivity from 4.6×10−7 S cm−1 to 2.3×10−6 S cm−1 and has a positive impact on the electrochemical performance. Several spectroscopy techniques (Mössbauer, FTIR, and Raman) reveal differences between the two powders and additionally support the findings of both the Rietveld refinement and the conductivity measurements.",
publisher = "Elsevier",
journal = "Ceramics International",
title = "The influence of fluorine doping on the structural and electrical properties of the LiFePO4 powder",
pages = "3230-3224",
number = "3",
volume = "43",
doi = "10.1016/j.ceramint.2016.11.149",
url = "https://hdl.handle.net/21.15107/rcub_dais_2352"
}
Jugović, D., Mitrić, M., Milović, M., Cvjetićanin, N., Jokić, B., Umićević, A.,& Uskoković, D.. (2017). The influence of fluorine doping on the structural and electrical properties of the LiFePO4 powder. in Ceramics International
Elsevier., 43(3), 3224-3230.
https://doi.org/10.1016/j.ceramint.2016.11.149
https://hdl.handle.net/21.15107/rcub_dais_2352
Jugović D, Mitrić M, Milović M, Cvjetićanin N, Jokić B, Umićević A, Uskoković D. The influence of fluorine doping on the structural and electrical properties of the LiFePO4 powder. in Ceramics International. 2017;43(3):3224-3230.
doi:10.1016/j.ceramint.2016.11.149
https://hdl.handle.net/21.15107/rcub_dais_2352 .
Jugović, Dragana, Mitrić, Miodrag, Milović, Miloš, Cvjetićanin, Nikola, Jokić, Bojan, Umićević, Ana, Uskoković, Dragan, "The influence of fluorine doping on the structural and electrical properties of the LiFePO4 powder" in Ceramics International, 43, no. 3 (2017):3224-3230,
https://doi.org/10.1016/j.ceramint.2016.11.149 .,
https://hdl.handle.net/21.15107/rcub_dais_2352 .
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Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media

Stojmenović, Marija; Momčilović, Milan Z.; Gavrilov, Nemanja M.; Pašti, Igor A.; Mentus, Slavko V.; Jokić, Bojan M.; Babić, Biljana M.

(2015)

TY  - JOUR
AU  - Stojmenović, Marija
AU  - Momčilović, Milan Z.
AU  - Gavrilov, Nemanja M.
AU  - Pašti, Igor A.
AU  - Mentus, Slavko V.
AU  - Jokić, Bojan M.
AU  - Babić, Biljana M.
PY  - 2015
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5776
AB  - Ordered mesoporous carbon, volume-doped up to 3w.% with Pt, Ru and Pt-Ru nanoparticles was synthesized by evaporation-induced self-assembly method, under acidic conditions. The content of incorporated metal was determined by EDX analysis. The X-ray diffractometry confirmed the existence of highly dispersed metallic phases in doped samples. Specific surface area was determined by N-2-physisorption measurements to range between 452 and 545m(2) g(-1). Raman spectroscopy of investigated materials indicated highly disordered carbon structure with crystallite sizes around 1.4 nm. In a form of thin-layer electrode on glassy carbon support, in 0.1M KOH solution, the prepared materials displayed high activity toward oxygen reduction reaction (ORR) in alkaline media, with onset potentials more positive than -0.10 V vs. SCE. The kinetics of O-2 reduction was found to be affected by both the specific surface area and the concentration of metal dopants. The ethanol tolerance of (Pt, Ru)-doped OMCs was found to be higher than that of common Pt/C ORR catalysts. Presented study provides a new route for the synthesis of active and selective ORR catalysts in alkaline media, being competitive with, or superior to, the existing ones in terms of performance and price. (C) 2014 Elsevier Ltd. All rights reserved.
T2  - Electrochimica Acta
T1  - Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media
EP  - 139
SP  - 130
VL  - 153
DO  - 10.1016/j.electacta.2014.11.080
ER  - 
@article{
author = "Stojmenović, Marija and Momčilović, Milan Z. and Gavrilov, Nemanja M. and Pašti, Igor A. and Mentus, Slavko V. and Jokić, Bojan M. and Babić, Biljana M.",
year = "2015",
abstract = "Ordered mesoporous carbon, volume-doped up to 3w.% with Pt, Ru and Pt-Ru nanoparticles was synthesized by evaporation-induced self-assembly method, under acidic conditions. The content of incorporated metal was determined by EDX analysis. The X-ray diffractometry confirmed the existence of highly dispersed metallic phases in doped samples. Specific surface area was determined by N-2-physisorption measurements to range between 452 and 545m(2) g(-1). Raman spectroscopy of investigated materials indicated highly disordered carbon structure with crystallite sizes around 1.4 nm. In a form of thin-layer electrode on glassy carbon support, in 0.1M KOH solution, the prepared materials displayed high activity toward oxygen reduction reaction (ORR) in alkaline media, with onset potentials more positive than -0.10 V vs. SCE. The kinetics of O-2 reduction was found to be affected by both the specific surface area and the concentration of metal dopants. The ethanol tolerance of (Pt, Ru)-doped OMCs was found to be higher than that of common Pt/C ORR catalysts. Presented study provides a new route for the synthesis of active and selective ORR catalysts in alkaline media, being competitive with, or superior to, the existing ones in terms of performance and price. (C) 2014 Elsevier Ltd. All rights reserved.",
journal = "Electrochimica Acta",
title = "Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media",
pages = "139-130",
volume = "153",
doi = "10.1016/j.electacta.2014.11.080"
}
Stojmenović, M., Momčilović, M. Z., Gavrilov, N. M., Pašti, I. A., Mentus, S. V., Jokić, B. M.,& Babić, B. M.. (2015). Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media. in Electrochimica Acta, 153, 130-139.
https://doi.org/10.1016/j.electacta.2014.11.080
Stojmenović M, Momčilović MZ, Gavrilov NM, Pašti IA, Mentus SV, Jokić BM, Babić BM. Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media. in Electrochimica Acta. 2015;153:130-139.
doi:10.1016/j.electacta.2014.11.080 .
Stojmenović, Marija, Momčilović, Milan Z., Gavrilov, Nemanja M., Pašti, Igor A., Mentus, Slavko V., Jokić, Bojan M., Babić, Biljana M., "Incorporation of Pt, Ru and Pt-Ru nanoparticles into ordered mesoporous carbons for efficient oxygen reduction reaction in alkaline media" in Electrochimica Acta, 153 (2015):130-139,
https://doi.org/10.1016/j.electacta.2014.11.080 . .
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Platinum deposition from hydrogen-ion beam irradiated solid precursor

Jovanović, Zoran M.; Pašti, Igor A.; Kalijadis, Ana; Lausevic, Mila; Mentus, Slavko V.; Laušević, Zoran

(2011)

TY  - JOUR
AU  - Jovanović, Zoran M.
AU  - Pašti, Igor A.
AU  - Kalijadis, Ana
AU  - Lausevic, Mila
AU  - Mentus, Slavko V.
AU  - Laušević, Zoran
PY  - 2011
UR  - http://TechnoRep.tmf.bg.ac.rs/handle/123456789/5649
AB  - We report a particular method of Pt/glassy carbon (GC) surface formation, based on a 15 key H(+/-) ion beam irradiation of thin H(2)PtCl(6)xnH(2)O layer placed over the GC surface. Hydrogen-ion beam irradiation provided an excellent adherence of Pt deposit, unlike to any other Pt-deposition method. Furthermore, the morphology and electrochemical activity of GC/Pt catalyst obtained at the fluence of 5 x 10(17) cm(-2) was found to be sensitive to the sign of charge of hydrogen ions. The electrochemical activity of such obtained Pt/GC surface toward oxygen reduction and ethanol oxidation was compared with the activity of the Pt deposits obtained by other more common reduction procedures. (C) 2011 Elsevier B.V. All rights reserved.
T2  - Materials Letters
T1  - Platinum deposition from hydrogen-ion beam irradiated solid precursor
EP  - 2657
IS  - 17-18
SP  - 2655
VL  - 65
DO  - 10.1016/j.matlet.2011.05.015
ER  - 
@article{
author = "Jovanović, Zoran M. and Pašti, Igor A. and Kalijadis, Ana and Lausevic, Mila and Mentus, Slavko V. and Laušević, Zoran",
year = "2011",
abstract = "We report a particular method of Pt/glassy carbon (GC) surface formation, based on a 15 key H(+/-) ion beam irradiation of thin H(2)PtCl(6)xnH(2)O layer placed over the GC surface. Hydrogen-ion beam irradiation provided an excellent adherence of Pt deposit, unlike to any other Pt-deposition method. Furthermore, the morphology and electrochemical activity of GC/Pt catalyst obtained at the fluence of 5 x 10(17) cm(-2) was found to be sensitive to the sign of charge of hydrogen ions. The electrochemical activity of such obtained Pt/GC surface toward oxygen reduction and ethanol oxidation was compared with the activity of the Pt deposits obtained by other more common reduction procedures. (C) 2011 Elsevier B.V. All rights reserved.",
journal = "Materials Letters",
title = "Platinum deposition from hydrogen-ion beam irradiated solid precursor",
pages = "2657-2655",
number = "17-18",
volume = "65",
doi = "10.1016/j.matlet.2011.05.015"
}
Jovanović, Z. M., Pašti, I. A., Kalijadis, A., Lausevic, M., Mentus, S. V.,& Laušević, Z.. (2011). Platinum deposition from hydrogen-ion beam irradiated solid precursor. in Materials Letters, 65(17-18), 2655-2657.
https://doi.org/10.1016/j.matlet.2011.05.015
Jovanović ZM, Pašti IA, Kalijadis A, Lausevic M, Mentus SV, Laušević Z. Platinum deposition from hydrogen-ion beam irradiated solid precursor. in Materials Letters. 2011;65(17-18):2655-2657.
doi:10.1016/j.matlet.2011.05.015 .
Jovanović, Zoran M., Pašti, Igor A., Kalijadis, Ana, Lausevic, Mila, Mentus, Slavko V., Laušević, Zoran, "Platinum deposition from hydrogen-ion beam irradiated solid precursor" in Materials Letters, 65, no. 17-18 (2011):2655-2657,
https://doi.org/10.1016/j.matlet.2011.05.015 . .
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