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Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis.

ABSTRACT: Membrane electrode assembly (MEA) electrolyzers offer a means to scale up CO₂-to-ethylene electroconversion using renewable electricity and close the anthropogenic carbon cycle. To date, excessive CO₂ coverage at the catalyst surface with limited active sites in MEA systems interferes with the carbon-carbon coupling reaction, diminishing ethylene production. With the aid of density functional theory calculations and spectroscopic analysis, here we report an oxide modulation strategy in which we introduce silica on Cu to create active Cu-SiO_x interface sites, decreasing the formation energies of OCOH* and OCCOH*-key intermediates along the pathway to ethylene formation. We then synthesize the Cu-SiO_x catalysts using one-pot coprecipitation and integrate the catalyst in a MEA electrolyzer. By tuning the CO₂ concentration, the Cu-SiO_x catalyst based MEA electrolyzer shows high ethylene Faradaic efficiencies of up to 65% at high ethylene current densities of up to 215 mA cm^-2; and features sustained operation over 50 h.

SUBMITTER: Li J

PROVIDER: S-EPMC8121866 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:Development of heterogeneous catalysts from biomass-derived activated carbon is a challenging task. Biomass-derived activated carbon possesses a large specific surface area, highly porous structure, and good thermal/chemical stability. Magnetic copper catalysts based on biomass-derived activated carbon exhibited good catalytic activity in base-free Chan-Lam coupling and oxidations. Herein, biomass-derived activated carbon was prepared by the carbonization of neem dead leaves (abundant waste biomass) followed by chemical activation with KOH. Such a porous carbon material was used as a low cost and highly efficient support material for the preparation of inexpensive and environmentally benign magnetic catalysts [Cu@KF-C/MFe2O4, M = Co, Cu, Ni, and Zn]. In addition, KF modification was done to impart basic character to the catalyst that can perform C-N coupling under base-free conditions. Initially, Brunauer-Emmett-Teller (BET) analysis of the synthesized catalysts was carried out, which indicated that Cu@KF-C/CoFe2O4 possess more surface area as well as pore volume, and so accounting for the highest activity among the other synthesized catalysts. Further, X-ray photoelectron spectroscopy (XPS) analysis was performed, which inferred that Cu@KF-C/CoFe2O4 contains most of the copper in reduced form, i.e., Cu(0), which is the active species responsible for better catalytic activity toward Chan-Lam coupling reactions as well as oxidation of alcohols and hydrocarbons. The physiochemical properties of the most active catalyst, Cu@KF-C/CoFe2O4, was examined by BET, XPS, Fourier transform infrared Spectroscopy (FTIR), thermogravimetric analysis (TGA), field emission gun scanning electron microscopy (FEG-SEM), high-resolution transmission electron microscopy (HR-TEM), energy dispersive X-ray (EDX) mapping, energy dispersive X-ray (EDX), inductively coupled plasma atomic emission spectroscopy (ICP-AES), powder X-ray diffraction (XRD), and vibrating sample magnetometry (VSM). Moreover, Cu@KF-C/CoFe2O4 shows excellent stability as well as reusability and could be easily separated with the help of an external magnet.

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Silica-copper catalyst interfaces enable carbon-carbon coupling towards ethylene electrosynthesis.

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