Engineering Cu(I)/Cu(0) interfaces for efficient ethanol production from CO2 electroreduction

Rongming Cai; Mingzi Sun; Fei Yang; Min Ju; Yanpeng Chen; M. Danny Gu; Bolong Huang; Shihe Yang

doi:10.1016/j.chempr.2023.08.027

Engineering Cu(I)/Cu(0) interfaces for efficient ethanol production from CO₂ electroreduction

Rongming Cai, Mingzi Sun, Fei Yang, Min Ju, Yanpeng Chen, M. Danny Gu, Bolong Huang, Shihe Yang

Research output: Journal article publication › Journal article › Academic research › peer-review

38 Citations (Scopus)

Abstract

By leveraging a Cu(OH)F precursor, we construct a disk-like Cu(I)/Cu(0) interface model (P-Cu_x/Cu₂OF) composed of F-stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C₂₊) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5-fold over pure P-Cu, with the corresponding partial current density (j_ethanol) reaching up to 128 mA/cm². This is enabled by a 3.6-fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8-fold boost in activity (j_C₂₊ up to 288 mA/cm²). The interactions between P-Cu and Cu₂OF upshift the d-band center of Cu sites on the interface region, which is critical to asymmetrical C-C coupling to form OCCOH∗, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene-forming symmetrical C-C coupling occurs primarily on P-Cu away from the Cu(I)/Cu(0) interface.

Original language	English
Pages (from-to)	211-233
Number of pages	23
Journal	Chem
Volume	10
Issue number	1
DOIs	https://doi.org/10.1016/j.chempr.2023.08.027
Publication status	Published - 11 Jan 2024

Keywords

asymmetric C-C coupling
copper electronic structure gradient
electrocatalytic CO reduction
ethanol
interface
SDG7: Affordable and clean energy
SDG9: Industry, innovation, and infrastructure

ASJC Scopus subject areas

General Chemistry
Biochemistry
Environmental Chemistry
General Chemical Engineering
Biochemistry, medical
Materials Chemistry

More information

10.1016/j.chempr.2023.08.027

Cite this

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title = "Engineering Cu(I)/Cu(0) interfaces for efficient ethanol production from CO2 electroreduction",

abstract = "By leveraging a Cu(OH)F precursor, we construct a disk-like Cu(I)/Cu(0) interface model (P-Cux/Cu2OF) composed of F-stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C2+) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5-fold over pure P-Cu, with the corresponding partial current density (jethanol) reaching up to 128 mA/cm2. This is enabled by a 3.6-fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8-fold boost in activity (jC2+ up to 288 mA/cm2). The interactions between P-Cu and Cu2OF upshift the d-band center of Cu sites on the interface region, which is critical to asymmetrical C-C coupling to form OCCOH∗, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene-forming symmetrical C-C coupling occurs primarily on P-Cu away from the Cu(I)/Cu(0) interface.",

keywords = "asymmetric C-C coupling, copper electronic structure gradient, electrocatalytic CO reduction, ethanol, interface, SDG7: Affordable and clean energy, SDG9: Industry, innovation, and infrastructure",

author = "Rongming Cai and Mingzi Sun and Fei Yang and Min Ju and Yanpeng Chen and Gu, {M. Danny} and Bolong Huang and Shihe Yang",

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AU - Cai, Rongming

AU - Sun, Mingzi

AU - Yang, Fei

AU - Ju, Min

AU - Chen, Yanpeng

AU - Gu, M. Danny

AU - Huang, Bolong

AU - Yang, Shihe

PY - 2024/1/11

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N2 - By leveraging a Cu(OH)F precursor, we construct a disk-like Cu(I)/Cu(0) interface model (P-Cux/Cu2OF) composed of F-stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C2+) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5-fold over pure P-Cu, with the corresponding partial current density (jethanol) reaching up to 128 mA/cm2. This is enabled by a 3.6-fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8-fold boost in activity (jC2+ up to 288 mA/cm2). The interactions between P-Cu and Cu2OF upshift the d-band center of Cu sites on the interface region, which is critical to asymmetrical C-C coupling to form OCCOH∗, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene-forming symmetrical C-C coupling occurs primarily on P-Cu away from the Cu(I)/Cu(0) interface.

AB - By leveraging a Cu(OH)F precursor, we construct a disk-like Cu(I)/Cu(0) interface model (P-Cux/Cu2OF) composed of F-stabilized Cu(I) shell and Cu(0) core by one-step pulsed potential conversion. The interfacial region is shown to facilitate ethanol formation, guaranteeing a high FE(C2+) of up to 80.2%. Tuning the Cu(I)/Cu(0) ratio enhances the ethanol yield by 18.5-fold over pure P-Cu, with the corresponding partial current density (jethanol) reaching up to 128 mA/cm2. This is enabled by a 3.6-fold boost in selectivity for the ethanol product (35.4%) and an overall 7.8-fold boost in activity (jC2+ up to 288 mA/cm2). The interactions between P-Cu and Cu2OF upshift the d-band center of Cu sites on the interface region, which is critical to asymmetrical C-C coupling to form OCCOH∗, concurrent with a lowered energy barrier for ethanol formation. On the other hand, the ethylene-forming symmetrical C-C coupling occurs primarily on P-Cu away from the Cu(I)/Cu(0) interface.

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