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, Chizoba Ignatius, Ghosh, Srabanti, Faraldos Izquierdo, María Soledad, González Mosquera, Marta Elena|||0000-0003-2248-3050, Rosal García, Roberto|||0000-0003-0816-8775
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universidad de Alcalá (UAH)
Repositorio:e_Buah Biblioteca Digital Universidad de Alcalá
Idioma:inglés
OAI Identifier:oai:ebuah.uah.es:10017/62309
Acceso en línea:http://hdl.handle.net/10017/62309
https://dx.doi.org/10.1016/j.seppur.2022.122868
Access Level:acceso abierto
Palabra clave:Bimetallic metal-organic frameworks
De novo synthesis
Visible-light photocatalysis
Carbon dioxide reduction
Hydrogen generation
Chemistry
Química
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 ?mol 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.