Long-chain hydrocarbons by CO2 electroreduction using polarized nickel catalysts
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Date
2022-06
Publication Type
Journal Article
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yes
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Abstract
The electroreduction of CO2, driven by renewable electricity, can be used to sustainably generate synthetic fuels. So far, only copper-based materials have been used to catalyse the formation of multicarbon products, albeit limited to C2 or C3 molecules. Herein, we disclose that inorganic nickel oxygenate-derived electrocatalysts can generate linear and branched C3 to C6 hydrocarbons with sustained Faradaic efficiencies of up to 6.5%, contrasting with metallic nickel, which is practically inactive. Operando X-ray absorption spectroscopy, electrochemical CO stripping and density functional theory pinpoint the presence of stable, polarized Niδ+ active sites associated with Ni–O bonds, which bind CO moderately. The reduction of selected C1 molecules and density functional theory simulations suggest that the Niδ+ sites promote a mechanism reminiscent of the Fischer–Tropsch synthesis: COOH + CHx coupling followed by successive CHx insertions. Our results disclose atom polarization to be the key that prevents the CO poisoning of nickel and enables CO2 reduction to a wider pool of valuable products.
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published
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Volume
5
Pages / Article No.
545 - 554
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Nature
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03871 - Pérez-Ramírez, Javier / Pérez-Ramírez, Javier
02291 - NCCR Catalysis / NCCR Catalysis
Notes
Funding
ETH-47 19-1 - Microstructured electrocatalysts as a design platform for decentralized ammonia synthesis and carbon dioxide fixation in artificial leaves (ETHZ)
180544 - NCCR Catalysis (phase I) (SNF)
180544 - NCCR Catalysis (phase I) (SNF)