Fundamental Insights into Photoelectrocatalytic Hydrogen Production with a Hole-Transport Bismuth Metal–Organic Framework
| Autor: | Ignacio J. Villar-Garcia, Miguel Gomez-Mendoza, Alba García-Sánchez, Víctor A. de la Peña O’Shea, Marta Liras, Mariam Barawi, Felipe Gándara |
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| Přispěvatelé: | European Research Council, Ministerio de Ciencia, Innovación y Universidades (España), Ministerio de Economía y Competitividad (España), Comunidad de Madrid, Barawi, Mariam [0000-0001-5719-9872], Liras, Marta [0000-0002-1724-1586], Gándara Barragán, Felipe [0000-0002-1671-6260], Peña O'Shea, Víctor A. de la [0000-0001-5762-4787], Barawi, Mariam, Liras, Marta, Gándara Barragán, Felipe, Peña O'Shea, Víctor A. de la |
| Rok vydání: | 2019 |
| Předmět: |
Metal-organic framework
Photoelectrochemistry chemistry.chemical_element Nanotechnology General Chemistry Renewable fuels Reaction intermediate 010402 general chemistry Solar fuel 7. Clean energy 01 natural sciences Biochemistry Catalysis 3. Good health 0104 chemical sciences Bismuth Colloid and Surface Chemistry Charge transfer chemistry 13. Climate action Hydrogen production Flash photolysis |
| Zdroj: | Digital.CSIC. Repositorio Institucional del CSIC instname |
| Popis: | [EN] Solar fuels production is a cornerstone in the development of emerging sustainable energy conversion and storage technologies. Light-induced H2 production from water represents one of the most crucial challenges to produce renewable fuel. Metalorganic frameworks (MOFs) are being investigated in this process, due to the ability to assemble new structures with the use of suitable photoactive building blocks. However, the identification of the reaction intermediates remains elusive, having negative impacts in the design of more efficient materials. Here, we report the synthesis and characterization of a new MOF prepared with the use of bismuth and dithieno[3,2-b:2',3'-d]thiophene-2,6-dicarboxylic acid (DTTDC), an electron-rich linker with hole transport ability. By combining theoretical studies and time-resolved spectroscopies, such as core hole clock and laser flash photolysis measurements, we have completed a comprehensive study at different time scales (fs to-ms) to determine the effect of competitive reactions on the overall H2 production. We detect the formation of an intermediate radical anion upon reaction of photogenerated holes withan electron donor, which plays a key role in the photoelectrocatalytic processes. These results shed new light on the use of MOFs for solar fuel production. This work was supported by the EU (ERC CoG HyMAP 648319) and Spanish MCIU, Ra-Phuel (ENE2016-79608-C2-1-R), SOLPAC (ENE2017-89170-R) FOTOFUEL (ENE2016-82025-REDT) and CTQ2017-87262-R (MCIU/AEI/FEDER, UE). We thank "Comunidad de Madrid" and European Structural Funds for their financial support to FotoArt-CM project (S2018/NMT-4367). F.G., M. L and M. B thank to MINECO and European Social Fund for a Ramón y Cajal contract (RyC-2015-18384, RyC-2015-18677) and Juan de la Cierva Formación contract (FJCI-2016-30567), respectively. We thank Diamond Facilities for the access to synchrotron radiation and CESCA for computational resources. |
| Databáze: | OpenAIRE |
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