Dataset Information

Plasmonic photosynthesis of C1-C3 hydrocarbons from carbon dioxide assisted by an ionic liquid.

ABSTRACT: Photochemical conversion of CO2 into fuels has promise as a strategy for storage of intermittent solar energy in the form of chemical bonds. However, higher-energy-value hydrocarbons are rarely produced by this strategy, because of kinetic challenges. Here we demonstrate a strategy for green-light-driven synthesis of C1-C3 hydrocarbons from CO2 and H2O. In this approach, plasmonic excitation of Au nanoparticles produces a charge-rich environment at the nanoparticle/solution interface conducive for CO2 activation, while an ionic liquid stabilizes charged intermediates formed at this interface, facilitating multi-step reduction and C-C coupling. Methane, ethylene, acetylene, propane, and propene are photosynthesized with a C2+ selectivity of ~50% under the most optimal conditions. Hydrocarbon turnover exhibits a volcano relationship as a function of the ionic liquid concentration, the kinetic analysis of which coupled with density functional theory simulations provides mechanistic insights into the synergy between plasmonic excitation and the ionic liquid.

SUBMITTER: Yu S

PROVIDER: S-EPMC6494896 | biostudies-other | 2019 May

REPOSITORIES: biostudies-other

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Plasmonic photosynthesis of C1-C3 hydrocarbons from carbon dioxide assisted by an ionic liquid.

Yu Sungju S Jain Prashant K PK

Nature communications 20190501 1

Photochemical conversion of CO2 into fuels has promise as a strategy for storage of intermittent solar energy in the form of chemical bonds. However, higher-energy-value hydrocarbons are rarely produced by this strategy, because of kinetic challenges. Here we demonstrate a strategy for green-light-driven synthesis of C1-C3 hydrocarbons from CO2 and H2O. In this approach, plasmonic excitation of Au nanoparticles produces a charge-rich environ ...[more]

PMID: 31043604

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Project description:Heteroatom-doped porous carbon membranes (HPCMMs) with a tailor-made pore architecture, chemical composition, atomic structural order, and surface state represent an exciting family of porous carbon materials for diverse potential applications in catalysis, water treatment, biofiltration, energy conversion/storage, and so forth. Conventional porous carbon membranes possess intrinsic structural integrity, interconnectivity, and chemical purity across the atomic-to-macro world and have been popularly incorporated into devices as separators or chemically inert conductive supports, circumventing otherwise the inevitable complicated processing and structure weakness of their fine powderous counterpart. Motivated by the distinguished heteroatom-doping effect that revolutionizes the chemical and physical nature of carbon materials, the HPCMM research surges very recently, and focuses not only on the eminent conductive supports or separators but also on electro(co)catalysts in energy devices. Synergy of the porous nature, incorporation of heteroatoms, and the membrane state creates a vivid profile pattern and new task-specific usage. It is also noteworthy that the inherent structural merits of HPCMMs plus a high electron conductivity imbue them as a reliable binder-free model electrode to derive the intrinsic structure-property relationship of porous carbons in electrochemical environments, excluding the complex and adverse factors in association with polymer binders in carbon powder-based electrodes. HPCMMs are of both intense academic interest and practical value because of their well-defined properties endowed by controllable structure and porosity at both atomic and macroscopic scales in a membrane form. The sole aim of this article is to bring this group of porous carbon materials to the forefront so their comprehensive properties and functions can be better understood to serve the carbon community to address pressing materials challenges in our society. In this Account, we highlight the latest discovery and proceedings of HPCMMs, particularly the advancements in how to tailor structures and properties of HPCMMs by rational structure design of porous polymer membranes as sacrificial template built up especially from heteroatom-rich poly(ionic liquid)s (PILs). We will also stress the carbonization craft and the state-of-the-art electrochemical applications for HPCMMs. Key factors and thoughts in heteroatom doping and porous systems in HPCMMs are discussed. A future perspective of the challenges and promising potential of HPCMMs is cast on the basis of these achievements.

Dataset Information

Plasmonic photosynthesis of C1-C3 hydrocarbons from carbon dioxide assisted by an ionic liquid.

Publications

Plasmonic photosynthesis of C<sub>1</sub>-C<sub>3</sub> hydrocarbons from carbon dioxide assisted by an ionic liquid.

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