journal article·2023-02Open access

Photocatalytic CO2‐to‐Syngas Evolution with Molecular Catalyst Metal‐Organic Framework Nanozymes

Philip M. Stanley, Alice Y. Su, Vanessa Ramm, Pascal Fink, Ceren Kimna, Oliver Lieleg, Martin Elsner, Johannes A. Lercher, Bernhard Rieger, Julien Warnan, Roland A. Fischer

Advanced Materials· Volume 35· Issue 6

Abstract

Abstract Syngas, a mixture of CO and H2, is a high‐priority intermediate for producing several commodity chemicals, e.g., ammonia, methanol, and synthetic hydrocarbon fuels. Accordingly, parallel sunlight‐driven catalytic conversion of CO2 and protons to syngas is a key step toward a sustainable energy cycle. State‐of‐the‐art catalytic systems and materials often fall short as application‐oriented concurrent CO and H2 evolution requires challenging reaction conditions which can hamper stability, selectivity, and efficiency. Here a light‐harvesting metal‐organic framework hosting two molecular catalysts is engineered to yield colloidal, water‐stable, versatile nanoreactors for photocatalytic syngas generation with highly controllable product ratios. In‐depth fluorescence, X‐ray, and microscopic studies paired with kinetic analysis show that the host delivers energy efficiently to active sites, conceptually yielding nanozymes. This unlocked sustained CO2 reduction and H2 evolution with benchmark turnover numbers and record incident photon conversions up to 36%, showcasing a highly active and durable all‐in‐one material toward application in solar energy‐driven syngas generation.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: Metal-Organic Frameworks: Synthesis and Applications · Advanced Photocatalysis Techniques · Catalytic Processes in Materials Science

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Chair of Inorganic and Metal‐Organic Chemistry Department of Chemistry and Catalysis Research Center (CRC) TUM School of Natural Sciences Technical University of Munich 85748 Garching Germany

WACKER‐Chair of Macromolecular Chemistry Department of Chemistry TUM School of Natural Sciences Technical University of Munich 85748 Garching Germany

School of Engineering and Design Department of Materials Engineering and Center for Protein Assemblies (CPA) Technical University of Munich 85748 Garching Germany

Chair of Analytical Chemistry and Water Chemistry Department of Chemistry TUM School of Natural Sciences Technical University of Munich 85748 Garching Germany

Chair of Chemical Technology II Department of Chemistry TUM School of Natural Sciences Technical University of Munich 85748 Garching Germany

Institute for Integrated Catalysis Pacific Northwest National Laboratory 902 Battelle Blvd Richland WA 99354 USA

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