Bimetallic metal-organic frameworks for efficient visible-light-driven photocatalytic CO2 reduction and H2 generation

A series of robust octahedral bimetallic metal-organic frameworks, NH2-UiO-66(Zr/M), denoted as Zr/M-ATA, (where M is Fe, Co, or Cu) were prepared by solvothermal de novo reaction of 2-aminoterephthalic acid (denoted as H2ATA) and mixed metal salts using benzoic acid as a modulator. Photocatalytic s...

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Detalles Bibliográficos
Autores: Ezugwu, C.I., Ghosh, S., Bera, S., Faraldos, Marisol, Mosquera, M.E.G., Rosal, R.
Tipo de recurso: artículo
Estado:Versión aceptada para publicación
Fecha de publicación:2022
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/358061
Acceso en línea:http://hdl.handle.net/10261/358061
https://www.scopus.com/inward/record.uri?eid=2-s2.0-85144380995&doi=10.1016%2fj.seppur.2022.122868&partnerID=40&md5=0f227e2e026ccd76383f57812da6dedf
Access Level:acceso abierto
Palabra clave:Bimetallic metal-organic frameworks
De novo synthesis
Visible-light photocatalysis
Carbon dioxide reduction
Hydrogen generation
Descripción
Sumario:A series of robust octahedral bimetallic metal-organic frameworks, NH2-UiO-66(Zr/M), denoted as Zr/M-ATA, (where M is Fe, Co, or Cu) were prepared by solvothermal de novo reaction of 2-aminoterephthalic acid (denoted as H2ATA) and mixed metal salts using benzoic acid as a modulator. Photocatalytic studies revealed that Zr/Fe-ATA, Zr/Cu-ATA and Zr/Co-ATA containing double metals outperformed that of the monometallic Zr-ATA. Zr/Cu-ATA displayed excellent performance for visible-light-driven CO2 reduction with a formate formation rate of 122 μmol h−1 mmolMOF-1, which is among the highest performance of NH2-UiO-66 based MOFs. Furthermore, Zr/Cu-ATA is an efficient catalyst that can generate 12.8 mmol of H2 in 2 h under visible light irradiation. The light absorption band of Zr/Cu-ATA shifted to the near-IR region and the presence of Cu-oxo clusters significantly narrowed the bandgap from 2.95 eV (Zr-ATA) to 1.93 eV (Zr/Cu-ATA). Other photoelectrochemical studies further confirmed that the high catalytic performance of Zr/Cu-ATA can be ascribed to optimized bandgap, facile charge transfer and availability of large number of active sites. © 2022 Elsevier B.V.