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^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

67 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_C up to 288 mA/cm₂₊²). 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. © 2023 Elsevier Inc.

Original language	English
Pages (from-to)	211-233
Journal	Chem
Volume	10
Issue number	1
Online published	21 Sept 2023
DOIs	https://doi.org/10.1016/j.chempr.2023.08.027
Publication status	Published - 11 Jan 2024
Externally published	Yes

Funding

This work is supported by the National Natural Science Foundation of China (21972006, U2001217, and 22261160370), Shenzhen Peacock Plan (KQTD2016053015544057), Shenzhen Science and Technology Innovation Commission (KCXFZ20201221173604012), National Key Research and Development Project (2022YFA1503900), Shenzhen Fundamental Research Funding (JCYJ20220818100212027), National Key R&D Program of China (2021YFA1501101), and Research Grant Council of Hong Kong (N_PolyU502/21 and CRS_PolyU504_22). B.H. gratefully acknowledges the support from Research Centre for Carbon-Strategic Catalysis (RC-CSC) of the Hong Kong Polytechnic University.

Research Keywords

asymmetric C-C coupling
copper electronic structure gradient
electrocatalytic CO2 reduction
ethanol
interface
SDG7: Affordable and clean energy
SDG9: Industry, innovation, and infrastructure

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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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 (jC up to 288 mA/cm2+2). 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. {\textcopyright} 2023 Elsevier Inc.",

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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

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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 (jC up to 288 mA/cm2+2). 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. © 2023 Elsevier Inc.

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 (jC up to 288 mA/cm2+2). 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. © 2023 Elsevier Inc.

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KW - interface

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

Abstract

Funding

Research Keywords

UN SDGs

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NSFC-CRS-ExtU-Lead: Long-cycle and High-energy-density Flexible Li Batteries Using Hollow Multishelled Structure and Hierarchical Composite Electrode

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

Abstract

Funding

Research Keywords

UN SDGs

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

NSFC-CRS-ExtU-Lead: Long-cycle and High-energy-density Flexible Li Batteries Using Hollow Multishelled Structure and Hierarchical Composite Electrode

Cite this

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