期刊
CHEMSUSCHEM
卷 14, 期 3, 页码 961-970出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202002761
关键词
porphyrinoids; photocatalysis; hydrogen evolution; self-assembly; nanoparticles
资金
- General Secretariat for Research and Technology (GSRT)
- Hellenic Foundation for Research and Innovation (HFRI) [508]
- European Union
- Greek national funds through the Operational Program Competitiveness, Entrepreneurship, and Innovation, under the call RESEARCH-CREATE-INNOVATE [T1EDK-01504]
- Regional Operational Program Crete 2014-2020 [OPS:5029187]
- European Commission [229927]
- University of Crete
- Technologies Go Hybrid (SolTech) initiative of the Bavarian State Government
In this study, a highly efficient photocatalytic system for H-2 production is developed using porphyrins as photocatalysts. Self-organization of PdTCP and PtTCP into H- and J-aggregates on TiO2 NPs is crucial for H-2 evolution, with J-aggregated PtTCPs showing higher efficiency than H-aggregated PdTCPs. The simultaneous adsorption of PdTCP and PtTCP onto TiO2 NPs results in the most efficient catalytic system, achieving high turnover numbers.
In this study, a highly efficient photocatalytic H-2 production system is developed by employing porphyrins as photocatalysts. Palladium and platinum tetracarboxyporphyrins (PdTCP and PtTCP) are adsorbed or coadsorbed onto TiO2 nanoparticles (NPs), which act as the electron transport medium and as a scaffold that promotes the self-organization of the porphyrinoids. The self-organization of PdTCP and PtTCP, forming H- and J-aggregates, respectively, is the key element for H-2 evolution, as in the absence of TiO2 NPs no catalytic activity is detected. Notably, J-aggregated PtTCPs are more efficient for H-2 production than H-aggregated PdTCPs. In this approach, a single porphyrin, which self-organizes onto TiO2 NPs, acts as the light harvester and simultaneously as the catalyst, whereas TiO2 serves as the electron transport medium. Importantly, the concurrent adsorption of PdTCP and PtTCP onto TiO2 NPs results in the most efficient catalytic system, giving a turnover number of 22,733 and 30.2 mmol(H-2) g(cat)(-1).
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