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Atomic Scale Design of Clean Energy Materials: Efficient Solar Energy Conversion and Gas Sensing
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Materials Theory.
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The focus of this doctoral thesis is the atomic level design of photocatalysts and gas sensing materials. The band gap narrowing in the metal oxides for the visible-light driven photocatalyst as well as the interaction of water and gas molecules on the reactive surfaces of metal oxides and the electronic structure of kaolinite has been studied by the state-of-art calculations. Present thesis is organized into three sections.

The first section discusses the possibility of converting UV active photocatalysts (such as Sr2Nb2O7, NaTaO3, SrTiO3, BiTaO4 and BiNbO4) into a visible active photocatalysts by their band gap engineering. Foreign elements doping in wide band gap semiconductors is an important strategy to reduce their band gap. Therefore, we have investigated the importance of mono- and co-anionic/cationic doping on UV active photocatalysts. The semiconductor's band edge position is calculated with respect to the water oxidation/reduction potential for various doping. Moreover, the tuning of valence and conduction band edge position is discussed on the basis of dopant's p/d orbital energy.

In the second section of thesis the energetic, electronic and optical properties of TiO2, NiO and β-Si3N4 have been discussed to describe the adsorption mechanism of gas molecules at the surfaces. The dissociation of water into H+ or OH- occurs on the O-vacancy site of the (001)-surface of rutile TiO2 nanowire, which is due to the charge transfer from Ti atom to water molecule. The dissociation of water into OH- and imino (NH) groups is also observed on the β-Si3N4 (0001)-surface due to the dangling bonds of the lower coordinated N and Si surface atoms. Fixation of the SO2 molecules on the anatase TiO2 surfaces with O-deficiency have been investigated by Density Functional Theory (DFT) simulation and Fourier Transform Infrared (FTIR) spectroscopy. DFT calculations have been employed to explore the gas-sensing mechanism of NiO (100)-surface on the basis of energetic and electronic properties.

In the final section the focus is to describe the optical band gap of pristine kaolinite using the hybrid functional method and GW approach. Different possible intrinsic defects in the kaolinite (001) basal surface have been studied and their effect on the electronic structure has been explained. The detailed electronic structure of natural kaolinite has been determined by the combined efforts of first principles calculations and Near Edge X-ray Absorption Fine Structure (NEXAFS).

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2012. , p. 68
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 958
Keyword [en]
Photocatalysts, Band gap narrowing, Water dissociation, Density functional theory, Gas sensing, Kaolinite
National Category
Condensed Matter Physics Nano Technology Atom and Molecular Physics and Optics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-179372ISBN: 978-91-554-8436-1 (print)OAI: oai:DiVA.org:uu-179372DiVA, id: diva2:544591
Public defence
2012-09-28, Häggsalen, Ångström Laboratory, Lägerhyddsvägen 1, Uppsala, 10:15 (English)
Opponent
Supervisors
Available from: 2012-09-06 Created: 2012-08-14 Last updated: 2013-01-22
List of papers
1. Hole mediated coupling in Sr2Nb2O7 for visible light photocatalysis
Open this publication in new window or tab >>Hole mediated coupling in Sr2Nb2O7 for visible light photocatalysis
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2012 (English)In: Physical Chemistry, Chemical Physics - PCCP, ISSN 1463-9076, E-ISSN 1463-9084, Vol. 14, no 14, p. 4891-4897Article in journal (Refereed) Published
Abstract [en]

The band gap reduction and effective utilization of visible solar light are possible by introducing the anionic hole–hole mediated coupling in Sr2Nb2O7. By using the first principles calculations, we have investigated the mono- and co-anionic doping (S, N and C) in layered perovskite Sr2Nb2O7 for the visible-light photocatalysis. Our electronic structure and optical absorption study shows that the mono- (N and S) and co-anionic doped (N–N and C–S) Sr2Nb2O7 systems are promising materials for the visible light photocatalysis. The calculated binding energies show that if the hole–hole mediated coupling could be introduced, the co-doped systems would be more stable than their respective mono-doped systems. Optical absorption curves indicate that doping S, (N–N) and (C–S) in Sr2Nb2O7 can harvest a longer wavelength of the visible light spectrum as compared to the pure Sr2Nb2O7 for efficient photocatalysis.

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-173841 (URN)10.1039/c2cp23912d (DOI)000301494400026 ()
Available from: 2012-05-08 Created: 2012-05-07 Last updated: 2017-12-07Bibliographically approved
2. Band gap engineering by anion doping in the photocatalyst BiTaO4: First principle calculations
Open this publication in new window or tab >>Band gap engineering by anion doping in the photocatalyst BiTaO4: First principle calculations
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2012 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 37, no 4, p. 3014-3018Article in journal (Refereed) Published
Abstract [en]

We have shown the effect of mono and co-doping of non-metallic anion atoms on the electronic structure in BiTaO4 using the first-principles method. It can improve the photocatalytic efficiency for hydrogen production in the presence of visible sunlight. It is found that the band gap of BiTaO4 has been reduced significantly up to 54% with different nonmetallic doping. Electronic structure analysis shows that the doping of nitrogen is able to reduce the band gap of BiTaO4 due to the impurity N 2p state at the upper edge of the valence band. In case of C or C-S doped BiTaO4, double occupied (filled) states have been observed deep inside the band gap of BiTaO4. The large reduction of band gap has been achieved, which increases the visible light absorption. These results indicate that the doping of non-metallic element in BiTaO4 is a promising candidate for the photocatalyst due to its reasonable band gap.

Keyword
Band gap engineering, Photocatalysis, Anionic doping in BiTaO4
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-173827 (URN)10.1016/j.ijhydene.2011.11.068 (DOI)000301615100004 ()
Conference
International Conference on Renewable Energy (ICRE 2011)
Available from: 2012-05-09 Created: 2012-05-07 Last updated: 2017-12-07Bibliographically approved
3. Band gap engineering in BiNbO4 for visible-light photocatalysis
Open this publication in new window or tab >>Band gap engineering in BiNbO4 for visible-light photocatalysis
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2012 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 100, no 18, p. 182102-Article in journal (Refereed) Published
Abstract [en]

We have investigated the electronic structure of anionic mono- (S, N, and C) and co-doping (N-N, C-N, S-C, and S-N) on BiNbO4 for the visible-light photocatalysis. The maximum band gap reduction of pure BiNbO4 is possible with the (C-S) co-doping and minimum with N mono-doping. The calculated binding energies show that the co-doped systems are more stable than their mono-doped counterparts. Our optical absorption curves indicate that the mono- (C) and co-anionic doped (N-N and C-S) BiNbO4 systems are promising materials for visible light photocatalysis.

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-174927 (URN)10.1063/1.4709488 (DOI)000303598600026 ()
Available from: 2012-05-30 Created: 2012-05-30 Last updated: 2017-12-07Bibliographically approved
4. Study of electronic and optical properties of BiTaO4 for photocatalysis
Open this publication in new window or tab >>Study of electronic and optical properties of BiTaO4 for photocatalysis
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2012 (English)In: Physica Status Solidi. C, Current topics in solid state physics, ISSN 1610-1634, E-ISSN 1610-1642, Vol. 9, no 7, p. 1593-1596Article in journal (Refereed) Published
Abstract [en]

We present the optical absorption spectrum of BiTaO4 using the photo acoustic spectroscopy (PAS) technique and first principle approach. Band gap have been estimated 2.65 and 2.45 eV using PAS method and DFT calculations, respectively. Position of reduction and oxidation level with respect to vacuum level are identified, which shows that BiTaO4 can be used as photocatalyst for hydrogen production. Electronic structure is explained by plotting total density of states (TDOS).

Place, publisher, year, edition, pages
Wiley-VCH Verlagsgesellschaft, 2012
Keyword
photocatalysts, water splitting, hydrogen production
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-179326 (URN)10.1002/pssc.201100654 (DOI)000306479300019 ()
Conference
16th International Semiconducting and Insulating Materials Conference (SIMC-XVI), 19-23 June 2011, Stockholm, Sweden.
Funder
Swedish Research Council
Available from: 2012-08-13 Created: 2012-08-13 Last updated: 2017-12-07Bibliographically approved
5. Hybrid density functional study on SrTiO3 for visible light photocatalysis
Open this publication in new window or tab >>Hybrid density functional study on SrTiO3 for visible light photocatalysis
2012 (English)In: International journal of hydrogen energy, ISSN 0360-3199, E-ISSN 1879-3487, Vol. 37, no 16, p. 11611-11617Article in journal (Refereed) Published
Abstract [en]

Hybrid Density Functional calculations have been performed on the electronic structure of anionic mono- (S, N, P, and C) and co-doped (N-N, N-P, N-S, P-P) SrTiO3 to improve their visible light photocatalytic activity. The electronic band position of doped system has been aligned with respect to the water oxidation/reduction potential. The electronic band position and optical absorption study shows that the mono- (S) and co-doped (N-N, N-P and P-P) SrTiO3 systems are promising materials for the visible-light photocatalysis. The calculated binding energies show that the co-doped systems are more stable than their respective mono-doped systems.

Place, publisher, year, edition, pages
Elsevier, 2012
Keyword
Hybrid density function calculations, Electronic band allignment, photocatalysts, Optical absorption, Doped system
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-179330 (URN)10.1016/j.ijhydene.2012.05.038 (DOI)000307147500005 ()
Funder
Swedish Research Council
Available from: 2012-08-13 Created: 2012-08-13 Last updated: 2017-12-07Bibliographically approved
6. Electronic structure, optical properties and photocatalytic activities of LaFeO3-NaTaO3 solid solution
Open this publication in new window or tab >>Electronic structure, optical properties and photocatalytic activities of LaFeO3-NaTaO3 solid solution
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2012 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 116, no 43, p. 22767-22773Article in journal (Refereed) Published
Abstract [en]

A solid solution photocatalyst, Na1–xLaxFe1–xTaxO3 (x up to 0.06), was prepared by the conventional solid-state method. The photophysical properties of the samples were studied by various experimental techniques and the electronic structures were investigated by using screened hybrid density functional (HSE06) calculations. The solid solution photocatalyst showed absorption of visible light extending up to 450 nm. Upon loading of platinum nanoparticles cocatalyst, the photocatalytic hydrogen evolution of 0.81 μ·mol·h–1·g–1 was obtained for 2% doping of LaFeO3 in NaTaO3, under visible radiation (λ > 390 nm; 20% methanol solution). The photocatalytic properties of the solid solution were found to be better than Fe doped NaTaO3 compounds on account of the suitable band structure. The electronic structure analysis revealed that, in the case of Fe doping at the Ta site, unoccupied electronic states in between the band gap appear that are responsible for the visible-light absorption. However, in the case of La and Fe codoping (passivated doping) the mid-gap electronic states are completely filled, which makes the band structure suitable for the visible-light photocatalysis. The present solid solution of perovskites (LaFeO3 and NaTaO3) sheds light on the interesting photophysical properties and photocatalytic activities which could be beneficial for the photocatalysts derived from these compounds.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2012
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-179336 (URN)10.1021/jp307857h (DOI)000310482900014 ()
Funder
Swedish Research Council
Available from: 2012-08-13 Created: 2012-08-13 Last updated: 2017-12-07Bibliographically approved
7. Screened hybrid density functional study on Sr2Nb2O7 for visible light photocatalysis
Open this publication in new window or tab >>Screened hybrid density functional study on Sr2Nb2O7 for visible light photocatalysis
2012 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 100, no 18, p. 181903-Article in journal (Refereed) Published
Abstract [en]

The electronic structure of pure Sr2Nb2O7 and its electronic band position are being aligned with respect to the water oxidation/reduction potential level using hybrid functional (HSE06) theory. The experimental band gap (3.90 eV) of pure Sr2Nb2O7 can be reproduced (3.92 eV) using this level of theory. The cationic-anionic co-doping (Mo-N) in layered perovskite Sr2Nb2O7 structure reduces the band gap significantly, and its electronic band position is excellent for the visible-light photocatalysis. The respective cationic and anionic mono-doped systems create an occupied or unoccupied impurity states in the band gap, which can reduce the efficiency of the photocatalysis.

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-174926 (URN)10.1063/1.4709486 (DOI)000303598600019 ()
Available from: 2012-05-30 Created: 2012-05-30 Last updated: 2017-12-07Bibliographically approved
8. Mo- and N-doped BiNbO(4) for photocatalysis applications
Open this publication in new window or tab >>Mo- and N-doped BiNbO(4) for photocatalysis applications
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2011 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 99, no 5, p. 051909-Article in journal (Refereed) Published
Abstract [en]

The electronic structure of pure BiNbO(4) has been calculated and their electronic band positions have been aligned with respect to the water oxidation/reduction potential. The effect of cationic (Mo), anionic (N), and co-doping (Mo-N) on BiNbO(4) has been studied and discussed with respect to the standard redox potential levels. Our results show that co-doping of Mo and N in BiNbO(4) reduces the band gap up to 31.8%, thus making it a potential candidate for the photocatalysis of water for hydrogen production. The relative stability between the mono-and co-doped BiNbO(4) materials show that co-doped material is more stable and feasible in comparison to the mono-doped materials.

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-159057 (URN)10.1063/1.3622659 (DOI)000293617300023 ()
Available from: 2011-09-22 Created: 2011-09-21 Last updated: 2017-12-08Bibliographically approved
9. Water Interaction with native defects on rutile TiO2 nanowire: Ab initio calculations
Open this publication in new window or tab >>Water Interaction with native defects on rutile TiO2 nanowire: Ab initio calculations
2011 (English)In: Applied Physics Letters, ISSN 0003-6951, E-ISSN 1077-3118, Vol. 98, no 8, p. 083115-Article in journal (Refereed) Published
Abstract [en]

Adsorption of water molecules on stoichiometric and defective surfaces of rutile TiO2 nanowire oriented along the [(1) over bar 10] direction is investigated using density function theory calculations. We have investigated, in particular, O and Ti vacancies where energetic, structural, and electronic properties were evaluated. It was found that the water molecules interacting with O-vacancy undergo spontaneous dissociation, forming hydroxyl groups bound to Ti atoms and other OH groups formed by surface O and H-water. The same is not found in the case of perfect and Ti-vacancy containing nanowire. This dissociation of water molecules is due to charge transfer from neighboring Ti atom, which is polarized due to the O-vacancy.

National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-149060 (URN)10.1063/1.3556276 (DOI)000287764300079 ()
Available from: 2011-03-15 Created: 2011-03-15 Last updated: 2017-12-11Bibliographically approved
10. Structural, electronic and energetic properties of water adsorbed on beta-Si3N4 (0001) surface: First-principles calculations
Open this publication in new window or tab >>Structural, electronic and energetic properties of water adsorbed on beta-Si3N4 (0001) surface: First-principles calculations
2010 (English)In: Surface Science, ISSN 0039-6028, E-ISSN 1879-2758, Vol. 604, no 5-6, p. 617-622Article in journal (Refereed) Published
Abstract [en]

Structural, energetic and electronic properties of water molecules adsorbed on beta-Si3N4 (0 00 1) surface, at various coverages, are investigated using density functional theory. At low coverages (0 <= 0.5), it is found that all H2O molecules undergo spontaneous dissociation forming hydroxyl (OH) and imino (NH) groups where the reactive sites are identified, a result shown for the first time using ab initio theory. For higher coverages (0 > 0.5), only partial dissociation takes place where some of the molecules stay intact being bound via H-bond in good agreement with experimental findings. The driving force for the water dissociation has been identified to be dangling bonds on lower coordinated N and Si surface atoms showing that not all surface atoms are reactive corroborating with previous experimental findings. (C) 2010 Elsevier B.V. All rights reserved.

Keyword
Water-semiconductor interface, Silicon nitride, Density functional theory
National Category
Physical Sciences Engineering and Technology
Identifiers
urn:nbn:se:uu:diva-137099 (URN)10.1016/j.susc.2010.01.001 (DOI)000276297000024 ()
Available from: 2010-12-15 Created: 2010-12-15 Last updated: 2017-12-11Bibliographically approved
11. SO2 adsorption mechanism on TiO2 (001) and (101) surfaces: a combined theoratical and experimental study
Open this publication in new window or tab >>SO2 adsorption mechanism on TiO2 (001) and (101) surfaces: a combined theoratical and experimental study
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(English)Manuscript (preprint) (Other academic)
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-179353 (URN)
Funder
Swedish Research Council
Available from: 2012-08-13 Created: 2012-08-13 Last updated: 2013-12-05
12. Molecular simulation for gas adsorption at NiO (100) surface
Open this publication in new window or tab >>Molecular simulation for gas adsorption at NiO (100) surface
2012 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 4, no 10, p. 5691-5697Article in journal (Refereed) Published
Abstract [en]

Density functional theory (DFT) calculations have been employed to explore the gas-sensing mechanisms of NiO (100) surface on the basis of energetic and electronic properties. We have calculated the adsorption energies of NO 2, H 2S, and NH 3 molecules on NiO (100) surface using GGA+U method. The calculated results suggest that the interaction of NO 2 molecule with NiO surface becomes stronger and contributes more extra peaks within the band gap as the coverage increases. The band gap of H 2S-adsorbed systems decrease with the increase in coverage up to 0.5 ML and the band gap does not change at 1 ML because H 2S molecules are repelled from the surface. In case of NH 3 molecular adsorption, the adsorption energy has been increased with the increase in coverage and the band gap is directly related to the adsorption energy. Charge transfer mechanism between the gas molecule and the NiO surface has been illustrated by the Bader analysis and plotting isosurface charge distribution. It is also found that that work function of the surfaces shows different behavior with different adsorbed gases and their coverage. The work function of NO 2 gas adsorption has a hill-shaped behavior, whereas H 2S adsorption has a valley-shaped behavior. The work function of NH 3 adsorption decreases with the increase in coverage. On the basis of our calculations, we can have a better understanding of the gas-sensing mechanism of NiO (100) surface toward NO 2, H 2S, and NH 3 gases

Keyword
conductivity, density functional theory (DFT), gas sensing, NiO (100) surface
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-179340 (URN)10.1021/am3016894 (DOI)000310109000084 ()
Funder
Swedish Research Council
Available from: 2012-08-13 Created: 2012-08-13 Last updated: 2017-12-07Bibliographically approved
13. Optical gap and native point defects in kaolinite studied by the GGA-PBE, HSE functional, and GW approaches
Open this publication in new window or tab >>Optical gap and native point defects in kaolinite studied by the GGA-PBE, HSE functional, and GW approaches
2011 (English)In: Physical Review B. Condensed Matter and Materials Physics, ISSN 1098-0121, E-ISSN 1550-235X, Vol. 84, no 7, p. 075120-Article in journal (Refereed) Published
Abstract [en]

The electronic structure of kaolinite with and without intrinsic defects has been studied by the Perdew-Burke-Ernzerhof (PBE) and Heyd-Scuseria-Ernzerhof (HSE) functionals and by the G(0)W(0) approach. The band gap of defect-free kaolinite was estimated to between 6.2 and 8.2 eV. Analysis of the formation energy of native point defects in kaolinite was carried out under different growth conditions. When the PBE defect formation energy as a function of temperature is considered, the hydroxyl vacancy is compensated by a hydrogen vacancy at a formation energy of 0.45 eV at oxygen-rich and hydrogen-poor conditions. The hydroxyl vacancy acts as a donor whereas the hydrogen vacancy acts as an acceptor, both inducing states in the band gap. The HSE06 hybrid functional increases the defect formation energy and tends to localize and move these states away from the band edges, as compared to the other two methods. Our results imply that intrinsic defects will tune the band gap of kaolinite and influence properties related to its band structure such as the cation retention capability and drug release.

National Category
Physical Sciences Nano Technology
Research subject
Engineering Science with specialization in Nanotechnology and Functional Materials
Identifiers
urn:nbn:se:uu:diva-158167 (URN)10.1103/PhysRevB.84.075120 (DOI)000293618900007 ()
Available from: 2011-09-05 Created: 2011-09-01 Last updated: 2017-12-08Bibliographically approved
14. Kaolinite: defect states define material properties-a soft x-ray and first principles study of the band gap
Open this publication in new window or tab >>Kaolinite: defect states define material properties-a soft x-ray and first principles study of the band gap
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2015 (English)In: Journal of Electron Spectroscopy and Related Phenomena, ISSN 0368-2048, E-ISSN 1873-2526, Vol. 202, p. 11-15Article in journal (Refereed) Published
National Category
Condensed Matter Physics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
urn:nbn:se:uu:diva-179354 (URN)10.1016/j.elspec.2015.02.003 (DOI)000357904600003 ()
Funder
Swedish Research Council
Note

Funding: HEC of Pakistan, Sandvik AB 

Available from: 2012-08-13 Created: 2012-08-13 Last updated: 2017-12-07Bibliographically approved

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