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      Noble Metal-Free Light-Driven Hydrogen Evolution Catalysis in Polyampholytic Hydrogel Networks

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          Abstract

          Future technologies to harness solar energy and to convert this into chemical energy strongly rely on straightforward approaches to prepare versatile soft matter scaffolds for the immobilization of catalysts and sensitizers in a defined environment. In addition, particularly for light-driven hydrogen evolution, a transition to noble metal-free photosensitizers and catalysts is urgently required. Herein, we report a fully organic light-harvesting soft matter network based on a polyampholyte hydrogel where both photosensitizer (a perylene monoimide derivative) and a H 2 evolution catalyst ([Mo 3S 13] 2–) are electrostatically incorporated. The resulting material exhibits sustained visible-light-driven H 2 evolution in aqueous ascorbic acid solution, even at rather low loadings of photosensitizer (0.4%) and catalyst (120 ppm). In addition, we provide initial insights into the long-term stability of the hybrid hydrogel. We believe that these results pave the way for a generalized route toward the incorporation of noble metal-free light-driven catalysis in soft matter networks.

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          Most cited references56

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          Artificial Photosynthesis for Sustainable Fuel and Chemical Production

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            Recent Advances in Noble Metal (Pt, Ru, and Ir)-Based Electrocatalysts for Efficient Hydrogen Evolution Reaction

            Noble metal (Pt, Ru, and Ir)-based electrocatalysts are currently considered the most active materials for the hydrogen evolution reaction (HER). Although they have been associated with high cost, easy agglomeration, and poor stability during the HER reaction, recent efforts to intentionally tailor noble-metal-based catalysts have led to promising improvements, with lower cost and superior activity, which are critical to achieving large-scale production of pure hydrogen. In this mini-review, we focus on the recent advances in noble-metal-based HER electrocatalysts. In particular, the synthesis strategies to enhance cost-effectiveness and the catalytic activity for HER are highlighted.
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              Metal oxide-based materials as an emerging family of hydrogen evolution electrocatalysts

              Metal oxide-based materials are emerging as a promising family of hydrogen evolution reaction (HER) electrocatalysts. Hydrogen production from electrochemical water splitting represents a highly promising technology for sustainable energy storage, but its widespread implementation heavily relies on the development of high-performance and cost-effective hydrogen evolution reaction (HER) electrocatalysts. Metal oxides, an important family of functional materials with diverse compositions and structures, were traditionally believed inactive towards HER. Encouragingly, the continuous breakthroughs and significant progress in recent years (mainly from 2015 onwards) make engineered metal oxides emerge as promising candidates for HER electrocatalysis. In this article, we present a comprehensive review of recent advances in metal oxide-based electrocatalysts for HER. We start with a brief description of some key fundamental concepts of HER, such as mechanisms, computational activity descriptors, and experimental parameters used to evaluate catalytic performance. This is followed by a overview of various types of metal oxide-based HER electrocatalysts reported so far, including single transition metal oxides, spinel oxides, perovskite oxides, metal (oxy)hydroxides, specially-structured metal oxides and oxide-containing hybrids, with special emphasis on designed strategies for promoting performance and property–activity correlation. Finally, some concluding remarks and perspectives about future opportunities of this exciting field are provided.
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                Author and article information

                Journal
                ACS Appl Mater Interfaces
                ACS Appl Mater Interfaces
                am
                aamick
                ACS Applied Materials & Interfaces
                American Chemical Society
                1944-8244
                1944-8252
                03 May 2024
                15 May 2024
                : 16
                : 19
                : 24796-24805
                Affiliations
                []Institute of Organic Chemistry and Macromolecular Chemistry, Friedrich Schiller University Jena , Humboldtstraße 10, D-07743 Jena, Germany
                []Jena Center for Soft Matter (JCSM), Friedrich Schiller University Jena , Philosophenweg 7, D-07743 Jena, Germany
                [§ ]Center for Energy and Environmental Chemistry Jena (CEEC), Friedrich Schiller University Jena , Philosophenweg 7a, 07743 Jena, Germany
                []Institute of Chemical Engineering, Ulm University , Albert-Einstein-Allee 11, 89081 Ulm, Germany
                Author notes
                Author information
                https://orcid.org/0000-0003-1859-839X
                https://orcid.org/0000-0001-5578-3266
                https://orcid.org/0000-0003-4685-6608
                Article
                10.1021/acsami.4c04045
                11103662
                38700504
                47863d98-0a39-4593-8c84-4ee6ed75e520
                © 2024 The Authors. Published by American Chemical Society

                Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained ( https://creativecommons.org/licenses/by/4.0/).

                History
                : 11 March 2024
                : 29 April 2024
                : 25 April 2024
                Funding
                Funded by: Deutscher Akademischer Austauschdienst, doi 10.13039/501100001655;
                Award ID: NA
                Funded by: Deutsche Forschungsgemeinschaft, doi 10.13039/501100001659;
                Award ID: TRR234 364549901
                Categories
                Research Article
                Custom metadata
                am4c04045
                am4c04045

                Materials technology
                hydrogen evolution catalysis,noble metal-free,polyampholyte,hydrogel,scaffold,immobilization

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