Abstract
Water oxidation is still one of the most important challenges to develop efficient artificial photosynthetic devices. In recent decades, the development and study of molecular complexes for water oxidation have allowed insight into the principles governing catalytic activity and the mechanism as well as establish ligand design guidelines to improve performance. However, their durability and long-term stability compromise the performance of molecular-based artificial photosynthetic devices. In this context, heterogenization of molecular water oxidation catalysts on electrode surfaces has emerged as a promising approach for efficient long-lasting water oxidation for artificial photosynthetic devices. This review covers the state of the art of strategies for the heterogenization of molecular water oxidation catalysts onto electrodes for (photo)electrochemical water oxidation. An overview and description of the main binding strategies are provided explaining the advantages of each strategy and their scope. Moreover, selected examples are discussed together with the the differences in activity and stability between the homogeneous and the heterogenized system when reported. Finally, the common design principles for efficient (photo)electrocatalytic performance summarized.
Highlights
IntroductionThe need to mitigate the increasing CO2 emissions and transition to a sustainable society has increased in importance due to the high anthropogenic CO2 emissions that have caused 1.1 ◦ C of global warming
Light excitation of the chlorophyll pigments present in photosystem II (PSII) triggers the oxidation of a tetranuclear manganese cluster which is the active center of the oxygen evolving complex (OEC), which upon four electron oxidations is able to oxidize the molecule of water to generate O2 while releasing protons and electrons
Wang and coworkers reported a Co-based water oxidation catalysts (WOCs) (WOC-25, Figure 5d) that consisted of a metal organic frameworks (MOFs) where the redox function of the embedded cobalt active centers was modified by introducing imidazolate ligands as linkers to facilitate the proton transfer process involved in WO, generating a Co-containing zeolitic imidazolate framework (CoZIF) that was supported onto an fluorine doped tin oxide (FTO) electrode to explore its electrochemical WO capability
Summary
The need to mitigate the increasing CO2 emissions and transition to a sustainable society has increased in importance due to the high anthropogenic CO2 emissions that have caused 1.1 ◦ C of global warming. Light excitation of the chlorophyll pigments present in PSII triggers the oxidation of a tetranuclear manganese cluster which is the active center of the oxygen evolving complex (OEC), which upon four electron oxidations is able to oxidize the molecule of water to generate O2 while releasing protons and electrons. These reductive equivalents are transferred to the reductive site by cytochrome b6f to PSI (electron transport chain or Z scheme), where they are separated to generate the reduced molecule NADPH by a ferredoxin-NADP+ reductase (FNR), and the proton gradient triggers the APT production by the ATP synthase. Selected examples for each strategy are explained and compared to their homogeneous counterparts in terms of stability or catalytic activity
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