Embedding a Dinuclear Ru─Pt Photocatalyst Into Polyampholytic Graft Copolymer Matrix Enables Prolonged Hydrogen Evolution While Allowing Catalyst Repair
7 affiliations
- 1Institute of Organic Chemistry and Macromolecular Chemistry Friedrich Schiller University Jena Jena Germany
- 2Institute of Inorganic Chemistry I Ulm University Ulm Germany
- 3Institute of Physical Chemistry Friedrich Schiller University Jena Jena Germany
- 4Jena Center for Soft Matter (JCSM) Friedrich Schiller University Jena Jena Germany
- 5Center For Energy and Environmental Chemistry (CEEC) Friedrich Schiller University Jena Jena Germany
- 6Leibniz Institute of Surface Engineering Leipzig Germany
- 7Helmholtz Institute for Polymers in Energy Applications Jena (HIPOLE Jena) Jena Germany
Abstract
There are few molecular catalysts where active repair has been demonstrated, and one prominent example is a tetrapyridophenazine‐bridged heterodinuclear Ru‐Pt hydrogen‐evolving photocatalyst, where hydrogenation of the pyrazine ring in the bridging ligand has been shown to lead to an end of photocatalytic activity. Subsequent in situ repair by persulfate enabled catalyst reactivation, but so far at the cost of decreasing catalytic activity over several repair cycles. We now show that tailored polyampholytic graft copolymers enable electrostatic immobilization of the photocatalyst in a unimolecular soft matter matrix, thereby prolonging (photo)catalytic activity due to slower photocatalyst degradation kinetics. We attribute this to a decreased propensity for hydrogenation of the pyrazine ring and, with that, slower degradation of the bridge and improved long‐term HER activity, as evidenced by a holistic spectroscopic characterization of the molecular and electronic structure of the photocatalyst. At the same time, the graft copolymer matrix does not hinder oxidative repair of the photocatalyst, thus enabling multiple repair cycles without noticeable loss of catalytic activity. We therefore regard this as a novel blueprint for a synergistic molecule‐in‐matrix combination for sustainable light‐driven catalysis.
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BibTeX
@article{utievskyi2026embedding,
title = {{Embedding a Dinuclear Ru─Pt Photocatalyst Into Polyampholytic Graft Copolymer Matrix Enables Prolonged Hydrogen Evolution While Allowing Catalyst Repair}},
author = {Yurii Utievskyi and Alexander K. Mengele and Mariet Puthanagady and Nikita Vashistha and Linda Zedler and Christof Neumann and Marius Müßler and Andrey Turchanin and Benjamin Dietzek‐Ivanšić and Sven Rau and Felix H. Schacher},
journal = {Chemistry (Weinheim an Der Bergstrasse, Germany)},
year = {2026},
month = aug,
doi = {10.1002/chem.71568},
url = {https://doi.org/10.1002/chem.71568},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Embedding a Dinuclear Ru─Pt Photocatalyst Into Polyampholytic Graft Copolymer Matrix Enables Prolonged Hydrogen Evolution While Allowing Catalyst Repair
AU - Yurii Utievskyi
AU - Alexander K. Mengele
AU - Mariet Puthanagady
AU - Nikita Vashistha
AU - Linda Zedler
AU - Christof Neumann
AU - Marius Müßler
AU - Andrey Turchanin
AU - Benjamin Dietzek‐Ivanšić
AU - Sven Rau
AU - Felix H. Schacher
PY - 2026
DA - 2026/08/14
JO - Chemistry (Weinheim an Der Bergstrasse, Germany)
DO - 10.1002/chem.71568
UR - https://doi.org/10.1002/chem.71568
AB - There are few molecular catalysts where active repair has been demonstrated, and one prominent example is a tetrapyridophenazine‐bridged heterodinuclear Ru‐Pt hydrogen‐evolving photocatalyst, where hydrogenation of the pyrazine ring in the bridging ligand has been shown to lead to an end of photocatalytic activity. Subsequent in situ repair by persulfate enabled catalyst reactivation, but so far at the cost of decreasing catalytic activity over several repair cycles. We now show that tailored polyampholytic graft copolymers enable electrostatic immobilization of the photocatalyst in a unimolecular soft matter matrix, thereby prolonging (photo)catalytic activity due to slower photocatalyst degradation kinetics. We attribute this to a decreased propensity for hydrogenation of the pyrazine ring and, with that, slower degradation of the bridge and improved long‐term HER activity, as evidenced by a holistic spectroscopic characterization of the molecular and electronic structure of the photocatalyst. At the same time, the graft copolymer matrix does not hinder oxidative repair of the photocatalyst, thus enabling multiple repair cycles without noticeable loss of catalytic activity. We therefore regard this as a novel blueprint for a synergistic molecule‐in‐matrix combination for sustainable light‐driven catalysis.
SN - 0947-6539
SN - 1521-3765
ER -