Boosting Efficiency in Light‐Driven Water Splitting by Dynamic Irradiation through Synchronizing Reaction and Transport Processes **

ORCID
0000-0003-4853-5488
Affiliation
Institute of Chemical Engineering Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Sender, Maximilian;
ORCID
0000-0003-1150-0257
Affiliation
Institute of Inorganic Chemistry I Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Huber, Fabian L.;
Affiliation
Institute of Chemical Engineering Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Moersch, Maximilian C. G.;
ORCID
0000-0002-3603-5980
Affiliation
Institute of Chemical Engineering Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Kowalczyk, Daniel;
ORCID
0000-0002-8652-8812
Affiliation
Department Spectroscopy & Imaging Leibniz Institute of Photonic Technology Albert-Einstein-Str. 9 07745 Jena Germany
Hniopek, Julian;
ORCID
0000-0002-7919-093X
Affiliation
Institute of Analytical and Bioanalytical Chemistry Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Klingler, Sarah;
GND
120748193
ORCID
0000-0002-3807-3630
Affiliation
Institute of Physical Chemistry & Abbe Center of Photonics Friedrich Schiller University Jena Helmholtzweg 4 07743 Jena Germany
Schmitt, Michael;
ORCID
0000-0002-0698-1378
Affiliation
Institute of Inorganic Chemistry I Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Kaufhold, Simon;
Affiliation
Institute of Inorganic Chemistry I Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Siewerth, Kevin;
Affiliation
Department Spectroscopy & Imaging Leibniz Institute of Photonic Technology Albert-Einstein-Str. 9 07745 Jena Germany
Popp, Jürgen;
ORCID
0000-0002-5583-7962
Affiliation
Institute of Analytical and Bioanalytical Chemistry Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Mizaikoff, Boris;
ORCID
0000-0001-6104-4953
Affiliation
Institute of Chemical Engineering Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Ziegenbalg, Dirk;
ORCID
0000-0001-9635-6009
Affiliation
Institute of Inorganic Chemistry I Ulm University Albert-Einstein-Allee 11 89081 Ulm Germany
Rau, Sven

Abstract This work elaborates the effect of dynamic irradiation on light‐driven molecular water oxidation to counteract deactivation. It highlights the importance of overall reaction engineering to overcome limiting factors in artificial photosynthesis reactions. Systematic investigation of a homogeneous three‐component ruthenium‐based water oxidation system revealed significant potential to enhance the overall catalytic efficiency by synchronizing the timescales of photoreaction and mass transport in a capillary flow reactor. The overall activity could be improved by a factor of more than 10 with respect to the turnover number and a factor of 31 referring to the external energy efficiency by controlling the local availability of photons. Detailed insights into the mechanism of light driven water oxidation could be obtained using complementary methods of investigation like Raman, IR, and UV/Vis/emission spectroscopy, unraveling the importance of avoiding high concentrations of excited photosensitizers.

Water splitting : Dynamic irradiation enables a significant increase in catalytic performance of a homogeneous three‐component system for light‐driven water oxidation. Lower irradiation intensities and higher flowrates in a flow‐through reactor minimize photosensitizer degradation and thus improve catalyst lifetime, yield, and overall efficiency of a catalytic system for artificial photosynthesis. image

Cite

Citation style:
Could not load citation form.

Rights

License Holder: © 2022 Wiley‐VCH GmbH

Use and reproduction:
This publication is with permission of the rights owner freely accessible due to an Alliance licence and a national licence (funded by the DFG, German Research Foundation) respectively.