Proceedings of nanoGe Spring Meeting 2022 (NSM22)
DOI: https://doi.org/10.29363/nanoge.nsm.2022.051
Publication date: 7th February 2022
Syngas, an industrially relevant mixture of CO and H2, is a high-priority intermediate resource for producing several commodity chemicals, e.g., ammonia, methanol, and synthetic hydrocarbon fuels. Accordingly, parallel photocatalytic conversion of CO2 and protons to syngas is a key step in fostering a sustainable energy cycle. State-of-the-art catalytic systems often fall short as concurrent CO and H2 evolution requires challenging reaction conditions which can hamper stability, selectivity, and efficiency under application-oriented conditions. Here a light-harvesting metal-organic framework and two molecular catalysts are associated to design colloidal, water-stable, versatile nanoreactors for photocatalytic syngas generation with highly controllable product ratios. The host provides efficient directional light-harvested energy transport to the active sites, yielding sustained CO2 reduction and H2 evolution with incident photon conversions up to 36% and turnover numbers setting a benchmark, thus paving the way for application in solar energy-driven syngas generation. System bottlenecks, such as limited light absorption and kinetics, were identified, and proven addressable upon modularly co-hosting molecular additives owing to the system’s intrinsic versatility. Based on our findings, we highlight the uniqueness of MOF materials’ coordination space for rational designing and directing of such multicomponent supramolecular assemblies including antenna chromophores, auxiliary photosensitizers, and several catalysts of orthogonal photo-physical and chemical properties to minimize energy loss. This opens perspectives to tackle scalability, synthesize value-added products from the full redox cycle, harness the full solar spectrum energy, and precisely implement active sites with co-factors to mimic natural enzyme functionalities.[1-3]
Deutsche Forschungsgemeinschaft, PP 1329 "COORNETs"
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