NDLI: Photocatalytic proton reduction with ruthenium and cobalt complexes immobilized on fumed reversed-phase silica† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c5sc02124c

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Photocatalytic proton reduction with ruthenium and cobalt complexes immobilized on fumed reversed-phase silica† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c5sc02124c

Content Provider	Semantic Scholar
Author	Bachmann, Cyril Probst, Benjamin Oberholzer, Miriam Fox, Thomas Alberto, Roger
Copyright Year	2016
Abstract	Heterogeneous photocatalytic hydrogen production with a non-covalently immobilized molecular ruthenium based photosensitizer (PS) and a cobalt polypyridyl based water reducing catalyst (WRC) is reported. PS and WRC were derivatized with C18-alkyl chains and immobilized by adsorption on hydrophobic fumed silica. The resulting loaded support was suspended in water with anionic or cationic surfactants and subjected to heterogeneous photocatalytic H2 production with ascorbate as sacrificial electron donor (SED). No leaching was observed under catalytic conditions, thus catalysis was truly heterogeneous. The catalytic performance of immobilized PS and WRC clearly exceeded that of homogeneous catalysis at low concentrations. At high concentration, diffusion and light limitation lead to lower reaction rates, but the same stability as for homogeneous reactions was still achieved. WRC concentration variations indicated a relatively high stability (up to 1300 H2/Co) and mobility of amphiphilic catalysts on the hydrophobic silica surface. Comparison of fumed silica with porous and non-porous silica showed, that a high BET surface area along with a good accessibility from the reaction media are crucial for catalytic performance. Mechanistic investigations by transient absorption spectroscopy displayed reductive quenching of excited PS by ascorbate followed by on particle electron transfer to WRC as reaction pathway. Particles with additional cationic surfactants exhibited a significantly higher catalytic performance as compared to anionic surfactants. Non-covalent anchoring of correspondingly derivatized WRCs or PSs to reversed-phase silica offers a rapid and versatile transition from homogeneous to heterogeneous molecular proton reduction.
Starting Page	436
Ending Page	445
Page Count	10
File Format	PDF HTM / HTML
DOI	10.1039/c5sc02124c
PubMed reference number	29861992
Journal	Medline
Volume Number	7
Alternate Webpage(s)	http://pubs.rsc.org/en/content/articlepdf/2016/sc/c5sc02124c
Alternate Webpage(s)	https://pubs.rsc.org/en/content/articlepdf/2016/sc/c5sc02124c
Alternate Webpage(s)	https://doi.org/10.1039/c5sc02124c
Journal	Chemical science
Language	English
Access Restriction	Open
Content Type	Text
Resource Type	Article

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