Chiral Nanostructured\nAg Films for Multicarbon Products\nfrom CO<sub>2</sub> Electroreduction

The formation of multicarbon products from CO<sub>2</sub> electroreduction\nis challenging on materials other than Cu-based catalysts. Ag has\nbeen known to be a typical metal catalyst, producing CO in CO<sub>2</sub> electroreduction. The formation of C<sub>2+</sub> products\nby Ag has never been reported because the carbon–carbon (C–C)\ncoupling is an unfavorable process due to the high reaction barrier\nenergy of *OCCO. Here, we propose that the chirality-induced spin\npolarization of chiral nanostructured Ag films (CNAFs) can promote\nthe formation of triplet OCCO by regulating its parallel electron\nspin alignment, and the helical lattice distortion of nanostructures\ncan decrease the reaction energy of *OCCO, which triggers C–C\ncoupling and promotes subsequent *OCCO hydrogenation to facilitate\nthe generation of C<sub>2+</sub> products. The CNAFs with helically\nlattice-distorted nanoflakes were fabricated via electrodeposition\nusing phenylalanine as the symmetry-breaking agent. C<sub>2+</sub> products (C<sub>2</sub>H<sub>4</sub>, C<sub>2</sub>H<sub>6</sub>, C<sub>3</sub>H<sub>8</sub>, C<sub>2</sub>H<sub>5</sub>OH, and CH<sub>3</sub>COOH) with a Faradaic efficiency of ∼4.7% and a current\ndensity of ∼22 mA/cm<sup>2</sup> were generated in KHCO<sub>3</sub> electrolytes under 12.5 atm of CO<sub>2</sub> (g). Our findings\npropose that the chiral nanostructured materials can regulate the\nmultifunctionality of catalytic performance in the catalytic reactions\nwith triplet intermediates and products.

Publication Details

Journal
Figshare
Published
2024-10-02
DOI
https://doi.org/10.1021/jacs.4c08445.s001
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
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article

Chiral Nanostructured\nAg Films for Multicarbon Products\nfrom CO2 Electroreduction

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CO2 Reduction Techniques and Catalysts
article

Chiral Nanostructured\nAg Films for Multicarbon Products\nfrom CO2 Electroreduction

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Abstract

The formation of multicarbon products from CO<sub>2</sub> electroreduction\nis challenging on materials other than Cu-based catalysts. Ag has\nbeen known to be a typical metal catalyst, producing CO in CO<sub>2</sub> electroreduction. The formation of C<sub>2+</sub> products\nby Ag has never been reported because the carbon–carbon (C–C)\ncoupling is an unfavorable process due to the high reaction barrier\nenergy of *OCCO. Here, we propose that the chirality-induced spin\npolarization of chiral nanostructured Ag films (CNAFs) can promote\nthe formation of triplet OCCO by regulating its parallel electron\nspin alignment, and the helical lattice distortion of nanostructures\ncan decrease the reaction energy of *OCCO, which triggers C–C\ncoupling and promotes subsequent *OCCO hydrogenation to facilitate\nthe generation of C<sub>2+</sub> products. The CNAFs with helically\nlattice-distorted nanoflakes were fabricated via electrodeposition\nusing phenylalanine as the symmetry-breaking agent. C<sub>2+</sub> products (C<sub>2</sub>H<sub>4</sub>, C<sub>2</sub>H<sub>6</sub>, C<sub>3</sub>H<sub>8</sub>, C<sub>2</sub>H<sub>5</sub>OH, and CH<sub>3</sub>COOH) with a Faradaic efficiency of ∼4.7% and a current\ndensity of ∼22 mA/cm<sup>2</sup> were generated in KHCO<sub>3</sub> electrolytes under 12.5 atm of CO<sub>2</sub> (g). Our findings\npropose that the chiral nanostructured materials can regulate the\nmultifunctionality of catalytic performance in the catalytic reactions\nwith triplet intermediates and products.

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CO2 Reduction Techniques and Catalysts
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