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Author |
Barreca, D.; Carraro, G.; Gasparotto, A.; Maccato, C.; Warwick, M.E.A.; Kaunisto, K.; Sada, C.; Turner, S.; Gönüllü, Y.; Ruoko, T.-P.; Borgese, L.; Bontempi, E.; Van Tendeloo, G.; Lemmetyinen, H.; Mathur, S. |
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Title |
Fe2O3-TiO2Nano-heterostructure Photoanodes for Highly Efficient Solar Water Oxidation |
Type |
A1 Journal article |
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Year  |
2015 |
Publication |
Advanced Materials Interfaces |
Abbreviated Journal |
Adv Mater Interfaces |
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Volume |
2 |
Issue |
2 |
Pages |
1500313 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Harnessing solar energy for the production of clean hydrogen by photoelectrochemical water splitting represents a very attractive, but challenging approach for sustainable energy generation. In this regard, the fabrication of Fe2O3–TiO2 photoanodes is reported, showing attractive performances [≈2.0 mA cm−2 at 1.23 V vs. the reversible hydrogen electrode in 1 M NaOH] under simulated one-sun illumination. This goal, corresponding to a tenfold photoactivity enhancement with respect to bare Fe2O3, is achieved by atomic layer deposition of TiO2 over hematite (α-Fe2O3) nanostructures fabricated by plasma enhanced-chemical vapor deposition and final annealing at 650 °C. The adopted approach enables an intimate Fe2O3–TiO2 coupling, resulting in an electronic interplay at the Fe2O3/TiO2 interface. The reasons for the photocurrent enhancement determined by TiO2 overlayers with increasing thickness are unraveled by a detailed chemico-physical investigation, as well as by the study of photogenerated charge carrier dynamics. Transient absorption spectroscopy shows that the increased photoelectrochemical response of heterostructured photoanodes compared to bare hematite is due to an enhanced separation of photogenerated charge carriers and more favorable hole dynamics for water oxidation. The stable responses obtained even in simulated seawater provides a feasible route in view of the eventual large-scale generation of renewable energy. |
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Wos |
000368914700011 |
Publication Date |
2015-09-03 |
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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 |
2196-7350; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
4.279 |
Times cited |
56 |
Open Access |
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Notes |
The authors kindly acknowledge the fi nancial support under the FP7 project “SOLAROGENIX” (NMP4-SL-2012-310333), as well as Padova University ex-60% 2012–2014 projects, Grant No. CPDR132937/13 (SOLLEONE), and Regione Lombardia-INSTM ATLANTE projects. S.T. acknowledges the FWO Flanders for a postdoctoral scholarship. |
Approved |
Most recent IF: 4.279; 2015 IF: NA |
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Call Number |
c:irua:129201 |
Serial |
3957 |
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Author |
Warwick, M.E.A.; Kaunisto, K.; Barreca, D.; Carraro, G.; Gasparotto, A.; Maccato, C.; Bontempi, E.; Sada, C.; Ruoko, T.P.; Turner, S.; Van Tendeloo, G.; |
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Title |
Vapor phase processing of \alpha-Fe2O3 photoelectrodes for water splitting : an insight into the structure/property interplay |
Type |
A1 Journal article |
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Year |
2015 |
Publication |
ACS applied materials and interfaces |
Abbreviated Journal |
Acs Appl Mater Inter |
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Volume |
7 |
Issue |
7 |
Pages |
8667-8676 |
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Keywords |
A1 Journal article; Engineering sciences. Technology; Electron microscopy for materials research (EMAT) |
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Abstract |
Harvesting radiant energy to trigger water photoelectrolysis and produce clean hydrogen is receiving increasing attention in the search of alternative energy resources. In this regard, hematite (alpha-Fe2O3) nanostructures with controlled nano-organization have been fabricated and investigated for use as anodes in photoelectrochemical (PEC) cells. The target systems have been grown on conductive substrates by plasma enhanced-chemical vapor deposition (PE-CVD) and subjected to eventual ex situ annealing in air to further tailor their structure and properties. A detailed multitechnique approach has enabled to elucidate between system characteristics and the generated photocurrent. The present alpha-Fe2O3 systems are characterized by a high purity and hierarchical morphologies consisting of nanopyramids/organized dendrites, offering a high contact area with the electrolyte. PEC data reveal a dramatic response enhancement upon thermal treatment, related to a more efficient electron transfer. The reasons underlying such a phenomenon are elucidated and discussed by transient absorption spectroscopy (TAS) studies of photogenerated charge carrier kinetics, investigated on different time scales for the first time on PE-CVD Fe2O3 nanostructures. |
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Wos |
000353931300037 |
Publication Date |
2015-04-08 |
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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 |
1944-8244;1944-8252; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
7.504 |
Times cited |
51 |
Open Access |
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Notes |
246791 Countatoms; Fwo |
Approved |
Most recent IF: 7.504; 2015 IF: 6.723 |
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Call Number |
c:irua:126059 |
Serial |
3836 |
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Author |
Carraro, G.; Gasparotto, A.; Maccato, C.; Bontempi, E.; Lebedev, O.I.; Sada, C.; Turner, S.; Van Tendeloo, G.; Barreca, D. |
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Title |
Rational synthesis of F-doped iron oxides on Al2O3(0001) single crystals |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
RSC advances |
Abbreviated Journal |
Rsc Adv |
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Volume |
4 |
Issue |
94 |
Pages |
52140-52146 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
A plasma enhanced-chemical vapor deposition (PE-CVD) route to Fe2O3-based materials on Al2O3(0001) single crystals at moderate growth temperatures (200-400 degrees C) is reported. The use of the fluorinated Fe(hfa)(2)TMEDA (hfa = 1,1,1,5,5,5-hexafluoro-2,4-pentanedionate; TMEDA = N,N,N',N'-tetramethylethylenediamine) molecular precursor in Ar/O-2 plasmas enabled an in situ F-doping of iron oxide matrices, with a fluorine content tunable as a function of the adopted preparative conditions. Variations of the thermal energy supply enabled control of the system phase composition, resulting in gamma-Fe2O3 at 200 degrees C and alpha-Fe2O3 nanostructures at higher deposition temperatures. Notably, at 400 degrees C the formation of highly oriented alpha-Fe2O3 nanocolumns characterized by an epitaxial relation with the Al2O3(0001) substrate was observed. Beside fluorine content, phase composition and nano-organization, even the system optical properties and, in particular, energy gap values, could be tailored by proper modifications of processing parameters. |
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Wos |
000344389000041 |
Publication Date |
2014-10-02 |
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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 |
2046-2069; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.108 |
Times cited |
4 |
Open Access |
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Notes |
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Approved |
Most recent IF: 3.108; 2014 IF: 3.840 |
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Call Number |
UA @ lucian @ c:irua:121239 |
Serial |
2813 |
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Author |
Carraro, G.; Gasparotto, A.; Maccato, C.; Bontempi, E.; Lebedev, O.I.; Sada, C.; Turner, S.; Van Tendeloo, G.; Barreca, D. |
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Title |
Rational synthesis of F-doped iron oxides on Al2O3(0001) single crystals |
Type |
A1 Journal article |
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Year |
2014 |
Publication |
Rsc Advances |
Abbreviated Journal |
Rsc Adv |
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Volume |
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Issue |
94 |
Pages |
52140-52146 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
A plasma enhanced-chemical vapor deposition (PE-CVD) route to Fe2O3-based materials on Al2O3(0001) single crystals at moderate growth temperatures (200400 °C) is reported. The use of the fluorinated Fe(hfa)2TMEDA (hfa = 1,1,1,5,5,5-hexafluoro-2,4-pentanedionate; TMEDA = N,N,N′,N′-tetramethylethylenediamine) molecular precursor in Ar/O2 plasmas enabled an in situ F-doping of iron oxide matrices, with a fluorine content tunable as a function of the adopted preparative conditions. Variations of the thermal energy supply enabled control of the system phase composition, resulting in γ-Fe2O3 at 200 °C and α-Fe2O3 nanostructures at higher deposition temperatures. Notably, at 400 °C the formation of highly oriented α-Fe2O3 nanocolumns characterized by an epitaxial relation with the Al2O3(0001) substrate was observed. Beside fluorine content, phase composition and nano-organization, even the system optical properties and, in particular, energy gap values, could be tailored by proper modifications of processing parameters. |
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Corporate Author |
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Wos |
000344389000041 |
Publication Date |
2014-10-02 |
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Series Editor |
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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 |
2046-2069; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.108 |
Times cited |
4 |
Open Access |
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Notes |
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Approved |
Most recent IF: 3.108; 2014 IF: 3.840 |
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Call Number |
UA @ lucian @ c:irua:119529 |
Serial |
2814 |
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Author |
Carraro, G.; Maccato, C.; Bontempi, E.; Gasparotto, A.; Lebedev, O.I.; Turner, S.; Depero, L.E.; Van Tendeloo, G.; Barreca, D. |
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Title |
Insights on growth and nanoscopic investigation of uncommon iron oxide polymorphs |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
European journal of inorganic chemistry |
Abbreviated Journal |
Eur J Inorg Chem |
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Volume |
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Issue |
31 |
Pages |
5454-5461 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
Si(100)-supported Fe2O3 nanomaterials were developed by a chemical vapor deposition (CVD) approach. The syntheses, which were performed at temperatures between 400 and 550 °C, selectively yielded the scarcely studied β- and ϵ-Fe2O3 polymorphs under O2 or O2 + H2O reaction environments, respectively. Correspondingly, the observed morphology underwent a progressive evolution from interconnected nanopyramids to vertically aligned nanorods. The present study aims to provide novel insights into Fe2O3 nano-organization by a systematic investigation of the system structure/morphology and of their interrelations with growth conditions. In particular, for the first time, the β- and ϵ-Fe2O3 preparation process has been accompanied by a thorough multitechnique investigation, which, beyond X-ray photoelectron spectroscopy (XPS) and field-emission scanning electron microscopy (FESEM), is carried out by X-ray diffraction (XRD), energy-dispersive X-ray spectroscopy (EDXS), atomic force microscopy (AFM), high-resolution transmission electron microscopy (HRTEM), electron diffraction (ED), scanning TEM electron energy-loss spectroscopy (STEM-EELS), and high-angle annular dark-field STEM (HAADF-STEM). Remarkably, the target materials showed a high structural and compositional homogeneity throughout the whole thickness of the nanodeposit. In particular, spatially resolved EELS chemical maps through the spectrum imaging (SI) technique enabled us to gain important information on the local Fe coordination, which is of crucial importance in determining the system reactivity. The described preparation method is in fact a powerful tool to simultaneously tailor phase composition and morphology of iron(III) oxide nanomaterials, the potential applications of which include photocatalysis, magnetic devices, gas sensors, and anodes for Li-ion batteries. |
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Place of Publication |
Weinheim |
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Wos |
000330567000009 |
Publication Date |
2013-10-08 |
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Series Volume |
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Series Issue |
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Edition |
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ISSN |
1434-1948; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
2.444 |
Times cited |
18 |
Open Access |
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Notes |
Fwo; Countatoms |
Approved |
Most recent IF: 2.444; 2013 IF: 2.965 |
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Call Number |
UA @ lucian @ c:irua:110946 |
Serial |
1676 |
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Author |
Carraro, G.; Gasparotto, A.; Maccato, C.; Bontempi, E.; Lebedev, O.I.; Turner, S.; Sada, C.; Depero, L.E.; Van Tendeloo, G.; Barreca, D. |
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Title |
Fluorine doped Fe2O3 nanostructures by a one-pot plasma-assisted strategy |
Type |
A1 Journal article |
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Year |
2013 |
Publication |
RSC advances |
Abbreviated Journal |
Rsc Adv |
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Volume |
3 |
Issue |
45 |
Pages |
23762-23768 |
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Keywords |
A1 Journal article; Electron microscopy for materials research (EMAT) |
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Abstract |
The present work reports on the synthesis of fluorine doped Fe2O3 nanomaterials by a single-step plasma enhanced-chemical vapor deposition (PE-CVD) strategy. In particular, Fe(hfa)2TMEDA (hfa = 1,1,1,5,5,5-hexafluoro-2,4-pentanedionate; TMEDA = N,N,N′,N′-tetramethylethylenediamine) was used as molecular source for both Fe and F in Ar/O2 plasmas. The structure, morphology and chemical composition of the synthesized nanosystems were thoroughly analyzed by two-dimensional X-ray diffraction (XRD2), field emission-scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), secondary ion mass spectrometry (SIMS) and transmission electron microscopy (TEM). A suitable choice of processing parameters enabled the selective formation of α-Fe2O3 nanomaterials, characterized by an homogeneous F doping, even at 100 °C. Interestingly, a simultaneous control of the system nanoscale organization and fluorine content could be achieved by varying the sole growth temperature. The tailored properties of the resulting materials can be favourably exploited for several technological applications, ranging from photocatalysis, to photoelectrochemical cells and gas sensing. |
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Wos |
000326395800141 |
Publication Date |
2013-10-03 |
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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 |
2046-2069; |
ISBN |
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Additional Links |
UA library record; WoS full record; WoS citing articles |
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Impact Factor |
3.108 |
Times cited |
23 |
Open Access |
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Notes |
Fwo |
Approved |
Most recent IF: 3.108; 2013 IF: 3.708 |
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Call Number |
UA @ lucian @ c:irua:111091 |
Serial |
1237 |
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