Chiral Nanostructured Ag Films for Multicarbon Products from CO<sub>2</sub> Electroreduction

The formation of multicarbon products from CO<sub>2</sub> electroreduction is challenging on materials other than Cu-based catalysts. Ag has been known to be a typical metal catalyst, producing CO in CO<sub>2</sub> electroreduction. The formation of C<sub>2+</sub> products by Ag has never been reported because the carbon-carbon (C-C) coupling is an unfavorable process due to the high reaction barrier energy of *OCCO. Here, we propose that the chirality-induced spin polarization of chiral nanostructured Ag films (CNAFs) can promote the formation of triplet OCCO by regulating its parallel electron spin alignment, and the helical lattice distortion of nanostructures can decrease the reaction energy of *OCCO, which triggers C-C coupling and promotes subsequent *OCCO hydrogenation to facilitate the generation of C<sub>2+</sub> products. The CNAFs with helically lattice-distorted nanoflakes were fabricated via electrodeposition using 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 density 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 propose that the chiral nanostructured materials can regulate the multifunctionality of catalytic performance in the catalytic reactions with triplet intermediates and products.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2024-10-02
DOI
https://doi.org/10.1021/jacs.4c08445
Citations
17
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
1.74

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article

Chiral Nanostructured Ag Films for Multicarbon Products from CO2 Electroreduction

Changlin Tian, Tianwei Ouyang, Shunai Che, Wanning Zhang et al.
17 citations
Journal of the American Chemical Society
CO2 Reduction Techniques and Catalysts
1.74
article

Chiral Nanostructured Ag Films for Multicarbon Products from CO2 Electroreduction

Changlin Tian, Tianwei Ouyang, Shunai Che, Wanning Zhang, Jing Ai, Yingying Duan, Yanhang Ma, Aokun Liu, Lu Han, Lu Yu, Yuxi Fang, Chaoyang Chu
article en
17 citations

Abstract

The formation of multicarbon products from CO<sub>2</sub> electroreduction is challenging on materials other than Cu-based catalysts. Ag has been known to be a typical metal catalyst, producing CO in CO<sub>2</sub> electroreduction. The formation of C<sub>2+</sub> products by Ag has never been reported because the carbon-carbon (C-C) coupling is an unfavorable process due to the high reaction barrier energy of *OCCO. Here, we propose that the chirality-induced spin polarization of chiral nanostructured Ag films (CNAFs) can promote the formation of triplet OCCO by regulating its parallel electron spin alignment, and the helical lattice distortion of nanostructures can decrease the reaction energy of *OCCO, which triggers C-C coupling and promotes subsequent *OCCO hydrogenation to facilitate the generation of C<sub>2+</sub> products. The CNAFs with helically lattice-distorted nanoflakes were fabricated via electrodeposition using 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 density 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 propose that the chiral nanostructured materials can regulate the multifunctionality of catalytic performance in the catalytic reactions with triplet intermediates and products.

Journal of the American Chemical Society
Sinopec (China) (CN), Tongji University (CN), University of Science and Technology of China (CN), Shanghai Jiao Tong University (CN), Chinese Academy of Sciences (CN), Hefei Institutes of Physical Science (CN), ShanghaiTech University (CN), High Magnetic Field Laboratory (CN)
National Natural Science Foundation of China
Openalex Percentile: Top 16%
CO2 Reduction Techniques and Catalysts
1.74
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