Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 132, Issue 33, Pages 11642-11648Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja103798k
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Funding
- Ministry of Science and Technology of China [2009CB220001]
- NSFC [50921004]
- Solar Energy Initiative of the Chinese Academy of Sciences (CAS), CAS [KJCX2-YW-H21-01]
- China Postdoctoral Science Foundation [20100471486]
- IMR SYNL
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Electronic structure intrinsically controls the light absorbance, redox potential, charge-carrier mobility, and consequently, photoreactivity of semiconductor photocatalysts. The conventional approach of modifying the electronic structure of a semiconductor photocatalyst for a wider absorption range by anion doping operates at the cost of reduced redox potentials and/or charge-carrier mobility, so that its photoreactivity is usually limited and some important reactions may not occur at all. Here, we report sulfur-doped graphitic C3N4 (C3N4-xSx) with a unique electronic structure that displays an increased valence bandwidth in combination with an elevated conduction band minimum and a slightly reduced absorbance. The C3N4-xSx shows a photoreactivity of H-2 evolution 7.2 and 8.0 times higher than C3N4 under lambda > 300 and 420 nm, respectively. More strikingly, the complete oxidation process of phenol under lambda > 400 nm can occur for sulfur-doped C3N4, which is impossible for C3N4 even under lambda > 300 nm. The homogeneous substitution of sulfur for lattice nitrogen and a concomitant quantum confinement effect are identified as the cause of this unique electronic structure and, consequently, the excellent photoreactivity of C3N4-xSx. The results acquired may shed light on general doping strategies for designing potentially efficient photocatalysts.
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