Functional nanocomposites as water splitting photoelectrodes  Page description

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Details of project

  
Identifier
128841
Type NN
Principal investigator Pap, József Sándor
Title in Hungarian Funkcionális nanokompozitok, mint vízbontó fotoelektródák
Title in English Functional nanocomposites as water splitting photoelectrodes
Keywords in Hungarian molekuláris ko-katalizátor, nanostruktúra, félvezető, fotoelektrokatalízis, vízbontás
Keywords in English molecular co-catalyst, nanostructure, semiconductor, photoelectrocatalysis, water splitting
Discipline
Inorganic Chemistry (Council of Physical Sciences)40 %
Ortelius classification: Organometallic Chemistry
Material Science and Technology (chemistry) (Council of Physical Sciences)40 %
Structural Determination Methods (Council of Physical Sciences)20 %
Panel Chemistry 1
Department or equivalent Institute for Energy Security and Environmental Safety (Centre for Energy Research)
Participants Benkó, Tímea
Frey, Krisztina
Kerner, Zsolt Gábor
Ollár, Tamás
Srankó, Dávid Ferenc
Starting date 2018-12-01
Closing date 2023-11-30
Funding (in million HUF) 35.388
FTE (full time equivalent) 11.02
state running project





 

Final report

  
Results in Hungarian
A vizsgált egymagvú, Fe- és Cu-tartalmú komplexek oxigénfejlesztő anódkatalizátorként működhetnek félvezetőkön. Az elektródfelületen ilyen komplexek egycentrumú katalízisben vesznek részt, amelynek során a vízmolekula nukleofil támadása a kulcslépés. A működés feltétele, hogy az aromás ligandum erős donorként stabilizálja a kétszer egyelektronos oxidációban részt vevő és így reaktívvá váló fémcentrumot, vagy redoxaktivitása révén megkerülje a fémcentrumú oxidációt, ezzel nyitva új reakcióutat. Késői átmenetifém esetén (Cu) így elkerülhető a komplex korai bomlása. Mindkét stratégia segíti a katalitikus működést, növeli a stabilitást. A vízoldhatatlan aromás ligandumokat tartalmazó komplexek egyszerű és átméretezhető módszerekkel rögzíthetők (foto)elektród felületén (felcseppentés-rászárítás, bemártás, elektrodepozíció). A felületi komplexréteg fizikai stabilitását korlátozza a visszaoldódás, amelynek révén dinamikus egyensúlyi rendszer jön létre, de számolni kell a fémionok kioldódásával is. Számos komplex alkalmazható prekurzorként, aminek előnye, hogy in situ mineralizációval, szabályozható módon hozható létre belőlük aktív katalizátorfilm kis fémtartalmú, hosszú ideig stabil pufferoldatból. Fotoelektrokatalízisben a komplexek a fémcentrum oxidációs állapotától függően, fotolízissel mineralizálódhatnak. A hidrofób ligandumok befolyásolják a tényleges ko-katalizátor regioszelektív kialakulását, és ezzel a végső rendszer hatékonyságát.
Results in English
The studied mononuclear Fe- and Cu-complexes can act as oxygen-evolving anode catalysts on semiconductors. On surfaces, such complexes take part in single-site catalysis, during which the water nucleophilic attack is the key step. The condition is that the aromatic ligand stabilizes the metal center as a strong donor that participates in two, single-electron oxidations and thus becomes reactive, or bypasses the metal-centered oxidation via ligand redox activity, opening a new reaction path. For a late transition metal (Cu), the early decomposition can thus be avoided. Both strategies help catalytic operation and increase stability. Complexes with water-insoluble aromatic ligands can be immobilized on (photo)electrode surfaces using simple methods suitable for scale-over (drop-casting, dip-coating, electrodeposition). The physical stability of the surface layer is limited by re-dissolution, which creates a dynamic equilibrium system, but metal ion dissolution must also be taken into account. Many complexes can be used as precursors; the advantage is that an active catalyst film can be created in a controllable manner by in situ mineralization from a buffer solution with low metal content and long-time stability. In photoelectrocatalysis, the complexes can be mineralized by photolysis, depending on the oxidation state of the metal. The hydrophobic ligands influence the regioselective formation of the actual co-catalyst and thus the efficiency of the eventual system.
Full text https://www.otka-palyazat.hu/download.php?type=zarobeszamolo&projektid=128841
Decision
Yes





 

List of publications

  
Tímea Benkó, Dávid Lukács, Mingtao Li, József S. Pap: Redox-active ligands in artificial photosynthesis: a review, Environmental Chemistry Letters 20, 3657-3695, 2022
Tímea Benkó, Shaohua Shen, Miklós Németh, Jinzhan Su, Ákos Szamosvölgyi, Zoltán Kovács, György Sáfrán, Sahir M. Al-Zuraiji, Endre Zsolt Horváth, András Sápi, Zoltán Kónya, József Sándor Pap: BiVO4 charge transfer control by a water-insoluble iron complex for solar water oxidation, Appl. Catal. A: Gen. 652, 119035, 2023
Lukács Dávid: Molekuláris és heterogén vízoxidációs katalízis réz-peptid komplexekkel, Pannon Egyetem, Kémiai és Környezettudományi DI, 2023
J. S. Pap, S. Keszei, T. Ollár, L. Tapasztó: The role of ligand heteroatoms in electrocatalytic hydrogen evolution by iron(II) N-heterocyclic complexes, 15th European Congress on Catalysis (EuropaCat 2023) Prague, Czech Republic, Aug 27 - Sep 1, 2023
J. S. Pap, T. Benkó, M. Li, S. Shen, L. Vayssieres: Hydrophobic, redox-active, percursory - ancillary ligand choices for electrode surface immobilization of molecular water splitting electrocatalysts, The 4th International Workshop on Graphene and C3N4-Based Photocatalysts and Others (IWGCP4), October 13-16, Xi'an, China, 2023
T. Benkó, S. Shen, M. Németh, D. Lukács, J. S. Pap: α-Fe2O3-CuO nano-heterostructure for efficient photoelectrocatalytic water oxidation using a Cu-complex, 15th European Congress on Catalysis (EuropaCat 2023) Prague, Czech Republic, Aug 27 - Sep 1, 2023
T. Benkó, S. Shen, M. Nemeth, Á. Szamosvölgyi, A. Sápi, G. Sáfrán, S. M. Al-Zuraiji, L. Illés, J. S. Pap: Enhanced photoelectrochemical water oxidation activity of BiVO4 using a hydrophobic iron complex, 15th Pannonian International Symposium on Catalysis, September 4-8, 2022, Jastrzebia Gora, Poland, oral lecture, book of abstracts p. 75, ISBN 978-83-965789-0-7, 2022
T. Benkó, S. Shen, M. Németh, D. Lukács, Zs. Czigány, J. S. Pap: Gentle electrodeposition of ’CuO’ on α-Fe2O3 nanoarrays using Cu-peptides for efficient photoelectrocatalytic water oxidation, E-MRS Fall Meeting, September 18-21, Warsaw, Poland, 2023
D. Lukács, J. S. Pap, T. Benkó, M. Li, N. V. May, L. Vayssieres: „Problems with solutions" – in the search of the role of copper(II)-bis-aryliminoisondoline complexes in water oxidation, 15th Pannonian International Symposium on Catalysis September 4-8, 2022, Jastrzebia Gora, Poland, oral, book of abstracts p. 47, ISBN 978-83-965789-0-7, 2022
J. S. Pap, M. Li, S. Shen, L. Vayssieres: From hydrophobic to redox-active – evolution of ligands in molecular water splitting electrocatalysts, 15th Pannonian International Symposium on Catalysis September 4-8, 2022, Jastrzebia Gora, Poland, oral, book of abstracts p. 65, ISBN 978-83-965789-0-7, 2022
T. Benkó, S. Shen, M. Németh, Á. Szamosvölgyi, A. Sápi, S. M. Al-Zuraiji, J. S. Pap: Enhanced photoelectrochemical water oxidation activity of BiVO4 using a hydrophobic iron complex, XXVIII. International Conference on Coordination and Bioinorganic Chemistry, June 5-10, 2022, Smolenice, Slovakia, oral, book of abstracts p. 20, ISBN 978-80-8208-080-6, 2022
D. Lukács, J. S. Pap, T. Benkó, M. Li, N. V. May, L. Vayssieres: Condemned to function - water oxidation catalysis with Cu(II)-bis-aryliminoisoindoline complexes sans Cu(III) intermediates, XXVIII. International Conference on Coordination and Bioinorganic Chemistry, June 5-10, 2022, Smolenice, Slovakia, oral, book of abstracts p. 62, ISBN 978-80-8208-080-6, 2022
T. Benkó, S. Shen, M. Németh, D. Lukács, Zs. Czigány, J. S. Pap: Soft electrodeposition of ’CuO’ on α-Fe2O3 nanoarrays using Cu-peptides for photoelectrocatalytic water oxidation, The 4th International Workshop on Graphene and C3N4-Based Photocatalysts and Others (IWGCP4), October 13-16, Xi'an, China, 2023
T. Benkó, S. Shen, M. Németh, Á. Szamosvölgyi, A. Sápi, G. Sáfrán, S. M. Al-Zuraiji, J. S. Pap: Metallochaperone-like effect of a hydrophobic ligand in FeOx/BiVO4 nanohybrid formation for photoelectrochemical water oxidation, E-MRS 2022 Spring Meeting, online event, May 30th - June 3rd, Symposium 'Energy Materials' I.3.4. oral lecture, 2022
S. M. Alzuraiji, J. S. Pap: Utilization of iron complexes as molecular catalysts for water oxidation at low overpotential, XXVIII. International Conference on Coordination and Bioinorganic Chemistry, oral lecture, book of abstracts p. 18, 2022
Sahir Alzuraiji: Application of Water-Insoluble Iron Complexes in Water Oxidation, Doctoral School of Materials Sciences and Technologies, Óbuda University, Budapest, Hungary, 2022
J. S. Pap: Utilization of first-row transition metal complexes in (photo)electro-catalytic water splitting, XXVIII. International Conference on Coordination and Bioinorganic Chemistry, June 5-10, 2022, Smolenice, Slovakia, oral, book of abstracts p. 70, ISBN 978-80-8208-080-6, 2022
J. S. Pap, T. Benkó, S. Shen, L. Vayssieres: Exploiting immobilization, re-dissolution and degradation resulting from ancillary ligands of molecular complexes in water oxidation catalysis, E-MRS Fall Meeting, September 18-21, Warsaw, Poland, Symposium B - Advanced catalytic materials for (photo)electrochemical energy conversion, 2023
Tímea Benkó, Shaohua Shen, Miklós Németh, Jinzhan Su, Ákos Szamosvölgyi, Zoltán Kovács, György Sáfrán, Sahir M. Al-Zuraiji, Endre Zsolt Horváth, András Sápi, Zoltán Kónya, József Sándor Pap: BiVO4 charge transfer control by a water-insoluble iron complex for solar water oxidation, Appl. Catal. A: Gen. - submitted after revisions, 2023
J. S. Pap, D. Lukács, S. M. Al-Zuraiji, M. Németh, K. Frey, S. Shen, L. Vayssieres: Studying water oxidation catalysts on transparent conductive oxides, 8th TCM & 12th TOEO, Greece, Crete, October 17-25th, invited keynote lecture, 2022
Sahir M. Al-Zuraiji, Tímea Benkó, Krisztina Frey, Zsolt Kerner, József Sándor Pap: Electrodeposition of Fe-Complexes on Oxide Surfaces for Efficient OER Catalysis, Catalysts 11(5), 577, 2021
Tímea Benkó, Dávid Lukács, Mingtao Li, József S. Pap: Perspectives of Redox-Active Ligands in Artificial Photosynthesis, Environmental Chemistry Letters, submitted, 2022
József S. Pap, Tímea Benkó, Krisztina Frey, Sahir M. Al-Zuraiji, Márta M. Móricz, Shaohua Shen: How First Row Transition Metal Complexes Can Be Utilized to Improve Water Oxidation in (Photo)Electrocatalytic Hybrid Systems?, NPM-5/PAOT-6, May 24-27 Virtual Meeting, Proceedings Book p.70, ISBN: 978-963-306-789-5, 2021
József S. Pap: How First Row Transition Metal Complexes Utilized in Hybrid (Photo)Electrocatalytic Systems for Improved Water Oxidation?, Frontiers of Sustainable Technologies, virtual forum, September 18th, University of California, Berkeley, 2021
Tímea Benkó, Dávid Lukács, Krisztina Frey, Miklós Németh, Márta M Móricz, Dongyu Liu, Éva Kováts, Nóra May, Lionel Vayssieres, Mingtao Li, József S Pap: Redox-inactive metal single-site molecular complexes: A new generation of electrocatalysts for oxygen evolution?, Catalysis Science and Technology 11, 6411-6424, 2021
Sahir M. Al-Zuraiji, Tímea Benkó, Krisztina Frey, Zsolt Kerner, József Sándor Pap: Electrodeposition of Fe-Complexes on Oxide Surfaces for Efficient OER Catalysis, Catalysts 11(5), 577, 2021
Tímea Benkó, Dávid Lukács, Mingtao Li, József S. Pap: Redox-active ligands in artificial photosynthesis: a review, Environmental Chemistry Letters 20, 3657-3695, 2022
Sahir M Al-Zuraiji, Tímea Benkó, Levente Illés, Miklós Németh, Krisztina Frey, Attila Sulyok, József S. Pap: Utilization of Hydrophobic Ligands for Water-Insoluble Fe(II) Water Oxidation Catalysts - Immobilization and Characterization, Journal of Catalysis, 381, 615-625, 2020
Tímea Benkó, Dávid Lukács, Krisztina Frey, Miklós Németh, Márta M Móricz, Dongyu Liu, Éva Kováts, Nóra May, Lionel Vayssieres, Mingtao Li, József S Pap: Redox-inactive metal single-site molecular complexes: A new generation of electrocatalysts for oxygen evolution?, Catalysis Science and Technology 11, 6411-6424, 2021
Dávid Lukács, Łukasz Szyrwiel, József S. Pap: Copper Containing Molecular Systems in Electrocatalytic Water Oxidation—Trends and Perspectives, Catalysts 9(1), 83, 2019
Dávid Lukács, Miklós Németh, Łukasz Szyrwiel, Levente Illés, Béla Pécz, Shaohua Shen, József S. Pap: Behavior of a Cu-Peptide complex under water oxidation conditions – Molecular electrocatalyst or precursor to nanostructured CuO films?, Solar Energy Materials and Solar Cells 201, 110079, 2019
Sahir M Al-Zuraiji, Tímea Benkó, Levente Illés, Miklós Németh, Krisztina Frey, Attila Sulyok, József S. Pap: Utilization of Hydrophobic Ligands for Water-Insoluble Fe(II) Water Oxidation Catalysts - Immobilization and Characterization, Journal of Catalysis, accepted article, reference: YJCAT13559, 2020
József S. Pap, Dávid Lukács, Miklós Németh, Łukasz Szyrwiel, Levente Illés, Béla Pécz, Shaohua Shen, Lionel Vayssieres: Behavior of Cu-Peptides under Water Oxidation Conditions – Molecular Electrocatalysts or Precursors to Nanostructured CuO Films?, EMRS Spring Meeting, Nice, France, May 27-31, Symposium A: Latest advances on solar fuels, A.6.5 invited keynote lecture, 2019
József S. Pap: Functional First Row Transition Metal Complexes for the Promotion of Water Oxidation at Oxide Surfaces, 8th World Material Research Institute Forum, Budapest, Hungary, June 16-20, invited lecture, 2019
Tímea Benkó, Márta M. Móricz, József S. Pap: Electrocatalytic water oxidation by a water insoluble Cu(II) complex, EuropaCat, Aachen, Germany, August 18-23, B.2.185. Book of Abstracts pp 1003-1004. poster presentation, 2019
Sahir M. Al-Zuraiji, Tímea Benkó, József S. Pap: Application of water-insoluble Fe(II) complexes with hydrophobic bidentate N-donor ligands in electrocatalytic water oxidation, EMRS Spring Meeting, Nice, France, May 27-31, Symposium A: Latest advances on solar fuels, A.3.11 poster presentation, 2019
Dávid Lukács, József S. Pap, Miklós Németh, Levente Illés: Homogeneous or heterogeneous? – Exploring the dual role of copper-diglycyl-glycine in water oxidation, EMRS Spring Meeting, Nice, France, May 27-31, Symposium A: Latest advances on solar fuels, A.3.2 poster presentation (2nd AWARD), 2019
Dávid Lukács, Łukasz Szyrwiel, József S. Pap: Copper Containing Molecular Systems in Electrocatalytic Water Oxidation—Trends and Perspectives, Catalysts 9(1), 83, 2019
Dávid Lukács, Miklós Németh, Łukasz Szyrwiel, Levente Illés, Béla Pécz, Shaohua Shen, József S. Pap: Behavior of a Cu-Peptide complex under water oxidation conditions – Molecular electrocatalyst or precursor to nanostructured CuO films?, Solar Energy Materials and Solar Cells 201, 110079, 2019
Sahir M Al-Zuraiji, Tímea Benkó, Levente Illés, Miklós Németh, Krisztina Frey, Attila Sulyok, József S. Pap: Utilization of Hydrophobic Ligands for Water-Insoluble Fe(II) Water Oxidation Catalysts - Immobilization and Characterization, Journal of Catalysis, 381, 615-625, 2020
Sahir M. Al-Zuraiji, Dávid Lukács, Miklós Németh, Krisztina Frey, Tímea Benkó, Levente Illés, József S. Pap: An Iron(III) Complex with Pincer Ligand—Catalytic Water Oxidation through Controllable Ligand Exchange, Reactions, 1, 16-36, 2020
Benkó, Tímea; Lukács, Dávid; Frey, Krisztina; Németh, Miklós; Móricz, Márta; Liu, Dongyu; Vayssieres, Lionel; Li, Mingtao; Pap, József: Redox-Inactive Copper in a Molecular Water Oxidation Electrocatalyst, JACS Au, au-2020-00106j, submitted manuscript, 2021



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