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- Title
Semiconductive Copper(I)-Organic Frameworks for Efficient Light-Driven Hydrogen Generation Without Additional Photosensitizers and Cocatalysts.
- Authors
Shi, Dongying; Zheng, Rui; Sun, Ming ‐ Jun; Cao, Xinrui; Sun, Chun ‐ Xiao; Cui, Chao ‐ Jie; Liu, Chun ‐ Sen; Zhao, Junwei; Du, Miao
- Abstract
As the first example of a photocatalytic system for splitting water without additional cocatalysts and photosensitizers, the comparatively cost-effective Cu2I2-based MOF, Cu-I-bpy (bpy=4,4′-bipyridine) exhibited highly efficient photocatalytic hydrogen production (7.09 mmol g−1 h−1). Density functional theory (DFT) calculations established the electronic structures of Cu-I-bpy with a narrow band gap of 2.05 eV, indicating its semiconductive behavior, which is consistent with the experimental value of 2.00 eV. The proposed mechanism demonstrates that Cu2I2 clusters of Cu-I-bpy serve as photoelectron generators to accelerate the copper(I) hydride interaction, providing redox reaction sites for hydrogen evolution. The highly stable cocatalyst-free and self-sensitized Cu-I-bpy provides new insights into the future design of cost-effective d10-based MOFs for highly efficient and long-term solar fuels production.
- Subjects
COPPER catalysts; SEMICONDUCTORS; PHOTOCATALYSIS; PHOTOSENSITIZERS; INTERSTITIAL hydrogen generation; WATER electrolysis
- Publication
Angewandte Chemie, 2017, Vol 129, Issue 46, p14829
- ISSN
0044-8249
- Publication type
Article
- DOI
10.1002/ange.201709869