期刊
ACS APPLIED MATERIALS & INTERFACES
卷 7, 期 35, 页码 19635-19642出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.5b04020
关键词
phosphonite-coordinated ruthenium(II) sensitizers; carboxylate anchor; hydrogen evolution; DFT studies; high TON
资金
- TAPSUN-NWP-54 project
- DST Fast Track Young Scientist Project [CS-83/2012]
For the first time we report the design and syntheses of phosphonite coordinated ruthenium(II) sensitizers bearing (C) over cap(N) over capN ligand and/or terpyridine derivatives carboxylate anchor (GS11, GS12. and GS13) and its application for hydrogen production over Pt-TiO2 system. These heteroleptic complexes exhibit broad metal-to-ligand charge transfer transition band over the whole visible regime extending up to 900 nm. DFT calculations of these complexes show that the HOMO is distributed over the Ru and Cl atom whereas; LUMO is localized on the polypyridile ligand, which are anchored on TiO2 surface. Among the sensitizers tested for photocatalytic hydrogen evolution, GS12 exhibited a maximum turnover number (TON) 8605 (for 8h), which is very high compared to the reference sensitizer (N719) with TON 163 under similar evaluation condition. The dependence of the hydrogen evolution rate at different pH using GS11, GS12, GS13, and DX-1-sensitized Pt-TiO2 has been studied and the maximum H-2 production yield was obtained at pH 7 for all sensitizers.
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