Ruthenium Complex-Incorporated Two-Dimensional Metal–Organic Frameworks for Cocatalyst-Free Photocatalytic Proton Reduction from Water
Autor: | Yongfei Ji, Debiao Huo, Feifei Lin, Yueran Ni, Shani Chen, Lianpeng Tong, Aiju Zhou, Lele Duan, Ranhao Wang, Hong Chen |
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Rok vydání: | 2020 |
Předmět: |
010405 organic chemistry
chemistry.chemical_element 010402 general chemistry Photochemistry 01 natural sciences Exfoliation joint 0104 chemical sciences Ruthenium Catalysis Inorganic Chemistry Adsorption chemistry Photocatalysis Density functional theory Metal-organic framework Physical and Theoretical Chemistry Nanosheet |
Zdroj: | Inorganic Chemistry. 59:2379-2386 |
ISSN: | 1520-510X 0020-1669 |
Popis: | Ultrathin two-dimensional (2D) nanosheets with efficient light-driven proton reduction activity were obtained through the exfoliation of novel metal-organic frameworks (MOF), which were synthesized by using a bis(4'-carboxy-2,2':6',2″-terpyridine) ruthenium complex as a linker and 3d transition-metal (Mn, Co, Ni, and Zn) anions as nodes. The nanosheet of the Ni2+ node exhibits a photocatalytic hydrogen evolution rate of 923 ± 40 μmol g-1 h-1 at pH = 4.0, without the presence of any cocatalyst or cosensitizer. A combined experimental and theoretical study suggests a reductive quenched pathway for the photocatalytic hydrogen evolution by the nanosheet. The transition-metal nodes at the edge of the nanosheets are proposed as the active sites. Density functional theory (DFT) calculations attributed the different catalytic activities of the nanosheets to the discrepancy of H adsorption free energy at various transition-metal nodes. |
Databáze: | OpenAIRE |
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