Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 46, Pages 16660-16667Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201909934
Keywords
dopant activation; ion implantation; orbital modulation; photoelectrochemical water splitting; TiO2 model
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Funding
- National Natural Science Foundation of China [51571153, 11722543, 11705129, U1867215, 11875211, U1932134]
- Fundamental Research Funds for the Central Universities [2042019kf0312]
- Suzhou key industrial technology innovation project [SYG201828]
- China Postdoctoral Science Foundation [2016M602346]
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An N-doped TiO2 model reveals a conceptually different mechanism for activating the N dopant based on delocalized orbital hybridization through O vacancy incorporation. Synchrotron-based X-ray absorption spectroscopy, time-resolved fluorescence, and DFT studies revealed that O vacancy incorporation can effectively stimulate the delocalization of N impurity states through p-band orbital modulation, which leads to a significant enhancement in photocarrier lifetime. Consequently, this effect also results in a remarkable increase in the incident photon-to-electron conversion efficiency in the range of 400-550nm compared to that of conventional N-incorporated TiO2 (15% versus 1% at 450nm). This work reveals the fundamental necessity of orbital modulation in the band engineering of metal oxides for driving solar water splitting and beyond.
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