Journal
SCIENCE CHINA-MATERIALS
Volume 65, Issue 5, Pages 1237-1244Publisher
SCIENCE PRESS
DOI: 10.1007/s40843-021-1898-6
Keywords
high-valence state; metal-organic frameworks; metal-to-cluster charge transfer; photocatalytic hydrogen production
Categories
Funding
- National Natural Science Funds for Distinguished Young Scholars [51725201]
- International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China [51920105003]
- Innovation Program of Shanghai Municipal Education Commission [E00014]
- China Postdoctoral Science Foundation [2020M681201]
- Shanghai Engineering Research Center of Hierarchical Nanomaterials [18DZ2252400]
- Fundamental Research Funds for the Central Universities [JKD01211519]
- Shanghai Rising-star Program [20QA1402400]
- Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning
- Feringa Nobel Prize Scientist Joint Research Center
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By installing high-valence W6+ ions onto the Ti-oxo clusters of MIL-125(Ti), a W-O-Ti structure is formed, triggering metal-to-cluster charge transfer and enhancing light absorption. This optimized charge transfer process efficiently separates photogenerated electron-hole spatially, leading to an enhanced photocatalytic hydrogen evolution performance.
Metal-organic frameworks (MOFs) possess the features of highly porosity-tunable and electronic-tunable structures, . Taking advantages of these merits, we successfully installed high-valence W6+ ions onto the Ti-oxo clusters of MIL-125(Ti) (W-MIL-125). The installed W6+ ions which form a W-O-Ti structure trigger the metal-to-cluster charge transfer (MCCT), together with an enhanced light absorption. Structural and spectroscopic characterizations reveal that the MCCT process optimizes the charge transfer process and efficiently separates the photogenerated electron-hole spatially. The as-obtained sample of 3.45 W-MIL-125 with optimized electronic structure demonstrates an enhanced photocatalytic hydrogen evolution performance of 1110.7 +/- 63.7 mu mol g(-1)h(-1) under light irradiation, which is 4.0 times that of the pristine MIL-125(Ti). This work will open up a new avenue for local structural modification of MOFs to boost photocatalytic performance.
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