Peripheral ligands as electron storage reservoirs and their role in enhancement of photocatalytic hydrogen generation

Qing Pan; Leon Freitag; Tanja Kowacs; Jane C. Falgenhauer; Jeroen P. Korterik; Derck Schlettwein; Wesley R. Browne; Mary T. Pryce; Sven Rau; Leticia González; Johannes G. Vos; Annemarie Huijser

doi:10.1039/C6CC05222C

Peripheral ligands as electron storage reservoirs and their role in enhancement of photocatalytic hydrogen generation†

Qing Pan,^a Leon Freitag,^b Tanja Kowacs,^c Jane C. Falgenhauer,^d Jeroen P. Korterik,^a Derck Schlettwein,^d Wesley R. Browne,^e Mary T. Pryce,^f Sven Rau,^c Leticia González,*^b Johannes G. Vos*^f and Annemarie Huijser*^a

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* Corresponding authors

^a MESA + Institute for Nanotechnology, University of Twente, P.O. Box 217, Enschede, The Netherlands
E-mail: j.m.huijser@utwente.nl

^b Institute of Theoretical Chemistry, University of Vienna, Währinger Str. 17, 1090 Vienna, Austria
E-mail: leticia.gonzalez@univie.ac.at

^c Institute of Inorganic Chemistry Materials and Catalysis, University of Ulm, Albert-Einstein-Allee 11, 89081 Ulm, Germany

^d Institute of Applied Physics, Justus-Liebig-University, Ludwigstraße 23, 35390 Gießen, Germany

^e Stratingh Institute for Chemistry, University of Groningen, Groningen, The Netherlands

^f SRC for Solar Energy Conversion, School of Chemical Sciences, Dublin City University, Glasnevin, Dublin 9, Ireland
E-mail: han.vos@dcu.ie

Abstract

The contrasting early-time photodynamics of two related Ru/Pt photocatalysts with very different photocatalytic H₂ generation capabilities are reported. Ultrafast equilibration (535 ± 17 fs) creates an electron reservoir on the peripheral ligands of the ester substituted complex, allowing a dramatic increase in photocatalytic performance. This insight opens the way towards a novel design strategy for H₂ generating molecular photocatalysts.

Chemical Communications

Peripheral ligands as electron storage reservoirs and their role in enhancement of photocatalytic hydrogen generation†

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Peripheral ligands as electron storage reservoirs and their role in enhancement of photocatalytic hydrogen generation

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