SPP 1613:
Regeneratively Produced Fuels by Light Driven Water Splitting: Investigation of Involved Elementary Processes and Perspectives of Technologic Implementation
Subject Area
Chemistry
Materials Science and Engineering
Physics
Thermal Engineering/Process Engineering
Term
from 2012 to 2020
Project identifier
Deutsche Forschungsgemeinschaft (DFG) - Project number 198634447
Final Report Year
2020
Final Report Abstract
The efficient and economic competitive production of fuels e.g. H2 through light driven water splitting is widely considered to be the most favourable future renewable energy technology and is intensively investigated all over the world. Consequently, the proposal for the priority program (SPP) „SolarH2” was accepted by the German Science foundation (DFG) in early 2012 as SPP1613, and the program started at the kick-off meeting in November 2012. The aim of the SPP SolarH2 was to merge distinct research approaches for advanced photoelectrochemical cells involving different disciplines and expertise as e.g. the preparation of photoactive semiconductors and adapted device structures, the synthesis and characterization of electrocatalysts as well as the fundamental analysis of the involved elementary processes and their theoretical simulation. The objective of the SPP was to investigate artificial photosynthesis based on inorganic semiconductors from a fundamental scientific perspective as well as the material science engineering improvements required for its technological implementation. New basic approaches were required that merge scientific innovation with advanced engineering strategies.
In the first funding period the priority was on the development and analysis of defined model systems for understanding of those (photo)electrochemical reactions which are involved in H2O splitting at interfaces. Four different but related project areas were defined and studied in close relation to each other to reach the needed and essential synergy effects in the priority program: Photoelectrochemical, Photocatalytic, Electrocatalytic, and Model systems. Based on the obtained results and the approved projects the central research topics were shifted in the second funding period to identify the scientific material preconditions for further investigations of technologically promising systems, which may serve as basis for the subsequent necessary technological developments. Therefore, the SPP was adapted to three complimentary project areas to be studied in close relation to each other to reach the needed and essential synergy effects: Novel photoabsorbers, Advanced electrocatalysts, and Device development.
The main results of the PP are i) Multijunction devices are needed as semiconductor absorber layers. Ii) The contact to the electrolyte for hydrogen and oxygen evolution must be engineered with a buried junction and adapted catalysts. Iii) With optimized systems, efficiencies and stability issues can be solved and approach PV-electrolyzer combinations. The basic understanding of the needs and future research goals for realizing an efficient synthetic artificial leaf approach to solar fuel (H2) generation has strongly improved internationally within the last years, most probably also due to the results obtained within the SPP 1613. We are convinced that its funding by the DFG was an important step forward for the reestablishment of the research on artificial fuels in Germany, its international visibility and competitiveness. We do expect a number of further efforts in this decisive research field in the next future.
Publications
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Anodic Formation of Self-Organized Cobalt Oxide Nanoporous Layers, Angew. Chemie Int. Ed. 52 (2013) 2077–2081
C.-Y. Lee, K. Lee, P. Schmuki
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Efficient and Stable TiO2:Pt-Cu(In,Ga)Se2 Composite Photoelectrodes for Visible –Light Driven Hydrogen Evolution, Advanced Energy Materials 2015, 1402148-1402157
A. Azarpira, M. Lublow, A. Steigert, P. Bogdanoff, D. Greiner, C.A. Kaufmann, M. Krüger, U. Gernert, R. van de Krol, A. Fischer, T. Schedel-Niedrig
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Enhanced Charge Transport in Tantalum Nitride Nanotube Photoanodes for Solar Water Splitting, ChemSusChem. 8 (2015) 2615–2620
L. Wang, N.T. Nguyen, X. Zhou, I. Hwang, M.S. Killian, P. Schmuki
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Oxide-Supported IrNiOx Core–Shell Particles as Efficient, Cost-Effective, and Stable Catalysts for Electrochemical Water Splitting, Angew. Chemie, 127, 10, 3018-3022, (2015)
H. Nhan Nong, H.-S. Oh, T. Reier, E. Willinger, M.-G. Willinger, V.Petkov, D. Teschner, P. Strasser
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Approaching Compositional Limits of Perovskite – type Oxides and Oxynitrides by Synthesis of Mg0.25Ca0.65Y0.1Ti(O,N)3, Ca1–xYxZr(O,N)3 (0.1 ≤ x ≤ 0.4), and Sr1– xLaxZr(O,N)3 (0.1 ≤ x ≤ 0.4), Solid State Sci. 2016, 54, 7–16
M. Widenmeyer, C. Peng, A. Baki, R. Niewa, A. Weidenkaff
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Band engineering for efficient catalyst-substrate coupling for photoelectrochemical water splitting, Phys. Chem. Chem. Phys. 16, 10751 (2016)
J. Klett, J. Ziegler, A. Radetinac, B. Kaiser, R. Schäfer, W. Jaegermann, F. Urbain, J. Becker, V. Smirnov, F. Finger
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Metal chalcogenide thin film electrode, method for the production thereof and use. 2016/10/20, Patentamt: US, Anmeldenummer: 15101639
Michael Lublow, Anna Fischer, Matthias Driess, Thomas Schedel-Niedrig, Marcel-Philip Luecke
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Multijunction Si photocathodes with tunable photovoltages from 2.0 V to 2.8 V for light induced water splitting, EnergyEnviron. Sci. 9 (2016) 145
F. Urbain, V. Smirnov, J.-P. Becker, A. Lambertz, F. Yang, J. Ziegler, B. Kaiser, W. Jaegermann, U. Rau, F. Finger
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Photoelectrochemical and theoretical investigations of spinel type ferrites (MXFe3-XO4) for water splitting: a mini-review, J. Photon. Energy 2016, 7, 012009
D.H. Taffa, R. Dillert, A.C. Ulpe, K.C.L. Bauerfeind, T. Bredow, D.W. Bahnemann, M. Wark
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Zinc Ferrite Photoanode Nanomorphologies with Favorable Kinetics for Water-Splitting. Advanced Functional Materials 2016, 26 (25), 4435-4443
A.G. Hufnagel, K. Peters, A. Müller, C. Scheu, D. Fattakhova-Rohlfing, T. Bein
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(2017) Unraveling Compositional Effects on the Light-Induced Oxygen Evolution in Bi(V-Mo-X)O4 Material Libraries, Energy & Environmental Science, 10, 1213 – 1221
R. Gutkowski, C. Khare, F. Conzuelo, Y.U. Kayran, A. Ludwig, W. Schuhmann
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Decoupling the effects of high crystallinity and surface area on the photocatalytic overall water splitting over b-Ga2O3 nanoparticles by chemical vapor synthesis, ChemSusChem 2017,10, 4190-4197
S. Lukic, J. Menze, P. Weide, G.W. Busser, M. Winterer, M. Muhler
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Low-Temperature Atomic Layer Deposition of Cobalt Oxide as an Effective Catalyst for Photoelectrochemical Water-Splitting Devices, Chem. Mater. 2017, 29, 5796
J. Kim, T. Iivonen, J. Hämäläinen, M. Kemell, K. Meinander, K. Mizohata, J. Räisänen, L. Wang, R. Beranek, M. Leskelä, A. Devi
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Rock Salt Ni/Co Oxides with Unusual Nanoscale-Stabilized Composition as Water Splitting Electrocatalysts. Advanced Functional Materials 2017, 27, 1605121
K. Fominykh, G.C. Tok, P. Zeller, H. Hajiyani, T. Miller, M. Döblinger, R. Pentcheva, T. Bein, D. Fattakhova-Rohlfing
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A Unique Oxygen Ligand Environment Facilitates Water Oxidation in Hole-doped IrNiOx Core-Shell Electrocatalysts, Nature Catalysis, 1, 841-851 (2018)
H. Nhan Nong, T. Reier, H.-S. Oh, M. Gliech, P. Paciok, Thu Ha Thi Vu, D. Teschner, M. Heggen, V. Petkov, R. Schlögl, T. Jones, P. Strasser
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CVD-grown copper tungstate thin films for solar water splitting, J. Mater. Chem. A 2018, 6, 10206
D. Peeters, O. Mendoza Reyes, L. Mai, A. Sadlo, S. Cwik, D. Rogalla, H.- W. Becker, H.M. Schütz, J. Hirst, S. Müller, D. Friedrich, D. Mitoraj, M. Nagli, M. CasparyToroker, R. Eichberger, R. Beranek, A. Devi
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High-dimensional wave packet dynamics: photodissociation of water on rutile (110), J. Photochem. And Photobiol. A: Chemistry 366 (2018), 3-11
T. Petersen, J. Mitschker, T. Klüner
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Mesoporous ZnFe2O4 photoanodes with template-tailored mesopores and temperature-dependent photocurrents, Chem. Phys. Chem. 19 (2018) 2313-2320
K. Kirchberg, S. Wang, L. Wang, R. Marschall
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ZnO Nanowire Networks as Photoanode Model Systems for Photoelectrochemical Applications, Nanomaterials (2018) 8, 693
L. Movsesyan, A.W. Maijenburg, N. Goethals, W. Sigle, A. Spende, F. Yang, B. Kaiser, W. Jaegermann, S.-Y. Park, G. Mul, C. Trautmann, M.E. Toimil-Molares
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Electronically Coupled Uranium and Iron Oxide Heterojunctions as Efficient Water Oxidation Catalysts, Advanced Functional Materials 2019, 1905005
J. Leduc, Y. Gönüllü, T. Ruoko, T. Fischer, L. Mayrhofer, N.V. Tkachenko, C. Dong, A. Held, M. Moseler, S. Mathur
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Electronically-Coupled Phase Boundaries in alpha-Fe2O3/Fe3O4 Nanocomposite Photoanodes for Enhanced Water Oxidation, ACS Applied Nano Materials 2019, 2, 334-342
J. Leduc, Y. Gönüllü, P. Ghamgosar, S. You, J. Mouzon, H. Choi, A. Vomiero, M. Grosch, S. Mathur
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Enhanced Photoelectrochemical Water Oxidation Performance by Fluorine Incorporation in BiVO 4 and Mo:BiVO 4 Thin Film Photoanodes, ACS Appl. Mater. Interfaces 2019, 11 (18), 16430–16442
M. Rohloff, B. Anke, O. Kasian, S. Zhang, M. Lerch, C. Scheu, A. Fischer
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Photoelectrochemistry of Ferrites: Theoretical Predictions vs. Experimental Results. Z. Phys. Chem.
A.C. Ulpe, K.C.L. Bauerfeind, L.I. Granone, A. Arimi, L. Megatif, R. Dillert, S. Warfsmann, D.H. Taffa, M. Wark, D.W. Bahnemann, T. Bredow
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Sol-gel synthesis of mesoporous CaFe2O4 photocathodes with hierarchical pore morphology, Sustainable Energy Fuels 3 (2019) 1150-1153
K. Kirchberg, R. Marschall
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Stability and Degradation Mechanismof Si-based Photocathodes for Water Splitting with Ultrathin TiO2 Protection Layer, Z. Phys. Chem., 20191481
E. Ronge, T. Cottre, K. Welter, V. Smirnov, N. J. Ottinger, F. Finger, B. Kaiser, W. Jaegermann, and C. Jooss
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Structural Transformation Identification of Sputtered Amorphous MoSx as an Efficient Hydrogen-Evolving Catalyst during Electrochemical Activation, ACS Catalysis 2019, 9, 2368−2380
F. Xi, P. Bogdanoff, K. Harbauer, P. Plate, C. Höhn, J. Rappich, B. Wang, X. Han, R. van de Krol, S. Fiechter
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Tuning the Size and Shape of NanoMOFs via Templated Electrodeposition and Subsequent Electrochemical Oxidation, ACS Appl. Mater. Interfaces (2019) 11, 25378
F. Caddeo, R. Vogt, D. Weil, W. Sigle, M.E. Toimil-Molares, W. Maijenburg
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Water-Oxidation Electrocatalysis by Manganese Oxides: Syntheses, Electrode Preparations, Electrolytes and Two Fundamental Questions, 2020
J. Melder, P. Bogdanoff, I. Zaharieva, S. Fiechter, H. Dau, P. Kurz
DFG Programme
Priority Programmes
International Connection
Denmark
Projects
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A monolithic all-silicon multi-junction photovoltaic electrolysis device for solar hydrogen production by direct water splitting
(Applicant
Berghoff, Birger
)
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Coordination Funds
(Applicant
Jaegermann, Wolfram
)
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Development of catalysts, namely manganese oxides and molybdenum sulphides, for an implementation in a light-driven water-splitting device using a multi-junction solar cell
(Applicants
Dau, Holger
;
Fiechter, Sebastian
;
Kurz, Philipp
)
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Development of optimum bandgap photoanodes for tandem water-splitting cells based on doped complex metal oxides and III-V semiconductors coupled to water oxidation electrocatalysts
(Applicants
Beránek, Radim
;
Devi, Anjana
;
Eichberger, Rainer
)
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Elementary Steps in the photocatalytic Water Splitting over TiO2-based Model Electrode Systems
(Applicants
Jacob, Timo
;
Over, Herbert
)
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Enhanced water splitting activity through flame made heterojunctions of doped and functionalized mixed metal oxide nanoparticles predicted by combinatorial computational materials design
(Applicants
Heine, Thomas
;
Mädler, Lutz
)
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Ferrites for photoelectrochemical water splitting
(Applicants
Bahnemann, Detlef
;
Bredow, Thomas
;
Wark, Michael
)
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High-throughput characterization of multinary transition metal oxide and oxynitride libraries. New materials for solar water splitting with improved properties
(Applicants
Fiechter, Sebastian
;
Ludwig, Alfred
;
Schuhmann, Wolfgang
)
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Highly Robust and Efficient Water Oxidation Catalysts based on Nanoscopic Metal Oxide Species (Polyoxometalates): from Fundamental Science to Devices
(Applicants
Kortz, Ph.D., Ulrich
;
Vankova, Nina
)
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In-situ environmental TEM studies of electro- and photo-electrochemical systems for water splitting
(Applicant
Jooss, Christian
)
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Iron oxides with highly ordered mesoporosity for photoelectrochemical oxygen formation from water
(Applicants
Bahnemann, Detlef
;
Wark, Michael
)
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Metal oxide nanostructures for electrochemical and photoelectrochemical water splitting
(Applicants
Bein, Thomas
;
Fattakhova-Rohlfing, Dina
;
Pentcheva, Rossitza
;
Scheu, Christina
)
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Nanostructured mixed metal oxides for the electrocatalytic oxidation of water
(Applicants
Strasser, Peter
;
Teschner, Detre
)
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Novel thin film composites and co-catalysts for visible light-induced water splitting
(Applicants
Behrens, Malte
;
Fischer, Anna
;
Lerch, Martin
;
Schedel-Niedrig, Thomas
)
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Photoelectrocatalytic Anion Substituted Perovskites PAP
(Applicant
Weidenkaff, Anke
)
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PhotoElectroChemical applicCation of Uranium oxides for enhanced LIght AbsoRption (PECULIAR)
(Applicant
Mathur, Sanjay
)
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Photoelectrochemical water splitting using adapted silicon based semiconductor multi-junction cell structures
(Applicants
Finger, Friedhelm
;
Jaegermann, Wolfram
;
Schäfer, Rolf
)
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Quantum chemical and quantum dynamical studies of the photocatalytic water splitting on titanium dioxide surfaces
(Applicant
Klüner, Thorsten
)
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Sustainable solar energy conversion with defined ferrite nanostructures
(Applicant
Marschall, Roland
)
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Ta3N5 nanotubes and -rods: doping, band-gap engineering and stabilization (co-catalysis)
(Applicant
Schmuki, Patrik
)
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Three-dimensional semiconductor nanowire networks as model systems to study physical processes in nanostructured electrodes for light-driven water splitting
(Applicant
Toimil-Molares, Maria Eugenia
)
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Tuning the (magneto)optical properties of supported plasmonic metal catalysts towards high performance and stability in photo(electro)catalytic water splitting
(Applicants
Beller, Matthias
;
Brüser, Volker
;
Lochbrunner, Stefan
)
-
Zn-doped Gallium Oxynitride Nanoparticles as Efficient Photocatalyst for Water Splitting
(Applicants
Muhler, Martin
;
Winterer, Markus
)