Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO2 to Methanol on Cu3P@C

Haoming Yu; Xinxin Han; Zhengyu Hua; Weiqiang Yang; Xiaopeng Wu; Yuzhen Wu; Shixia Chen; Wei Hong; Shuguang Deng; Jie Zhang; Jun Wang

doi:10.1021/acscatal.4c02465

Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO₂ to Methanol on Cu₃P@C

Haoming Yu
, Xinxin Han
, Zhengyu Hua
, Weiqiang Yang
, Xiaopeng Wu
, Yuzhen Wu
, Shixia Chen
, Wei Hong
, Shuguang Deng
, Jie Zhang
, Jun Wang

School of Chemistry

Research output: Contribution to journal › Article › Research › peer-review

28 Citations (Scopus)

Abstract

Carbon layer-coated CuX (CuX@C, X = P, S, Se) with different electron densities on the carbon coating layers have been successfully prepared. Among them, Cu₃P@C, which has a high-electron-density carbon coating layer, delivers a high faradaic efficiency for methanol of 61.2% at −0.36 V versus reversible hydrogen electrode (RHE), and a record partial current density for methanol of 130 mA cm^-2 at −0.76 V versus RHE when it is assembled on a gas diffusion electrode in a flow cell setup using 1 M KOH electrolyte, outperforming most of the state-of-the-art electrocatalysts. In contrast, Cu₂Se@C and Cu_1.8S@C, which have low-electron-density carbon coating layers, predominately produce formate. In situ Raman spectroscopy analysis and computational density functional theory calculations reveal the influence of Cu₃P on the electronic properties of carbon binding sites and the underlying mechanisms for methanol production.

Original language	English
Pages (from-to)	12783-12791
Number of pages	9
Journal	ACS Catalysis
Volume	14
Issue number	17
DOIs	https://doi.org/10.1021/acscatal.4c02465
Publication status	Published - 9 Aug 2024

Keywords

electrochemical CO reduction
electronic effect
intermediate binding
methanol production
product selectivity

Access to Document

10.1021/acscatal.4c02465

618104347-oaAccepted author manuscript, 2.96 MB

Cite this

@article{ebe12ffc2a904777aa860a02610f8bc1,

title = "Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO2 to Methanol on Cu3P@C",

abstract = "Carbon layer-coated CuX (CuX@C, X = P, S, Se) with different electron densities on the carbon coating layers have been successfully prepared. Among them, Cu3P@C, which has a high-electron-density carbon coating layer, delivers a high faradaic efficiency for methanol of 61.2\% at −0.36 V versus reversible hydrogen electrode (RHE), and a record partial current density for methanol of 130 mA cm-2 at −0.76 V versus RHE when it is assembled on a gas diffusion electrode in a flow cell setup using 1 M KOH electrolyte, outperforming most of the state-of-the-art electrocatalysts. In contrast, Cu2Se@C and Cu1.8S@C, which have low-electron-density carbon coating layers, predominately produce formate. In situ Raman spectroscopy analysis and computational density functional theory calculations reveal the influence of Cu3P on the electronic properties of carbon binding sites and the underlying mechanisms for methanol production.",

keywords = "electrochemical CO reduction, electronic effect, intermediate binding, methanol production, product selectivity",

author = "Haoming Yu and Xinxin Han and Zhengyu Hua and Weiqiang Yang and Xiaopeng Wu and Yuzhen Wu and Shixia Chen and Wei Hong and Shuguang Deng and Jie Zhang and Jun Wang",

note = "Publisher Copyright: {\textcopyright} 2024 American Chemical Society.",

year = "2024",

month = aug,

day = "9",

doi = "10.1021/acscatal.4c02465",

language = "English",

volume = "14",

pages = "12783--12791",

journal = "ACS Catalysis",

issn = "2155-5435",

publisher = "American Chemical Society",

number = "17",

}

TY - JOUR

T1 - Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO2 to Methanol on Cu3P@C

AU - Yu, Haoming

AU - Han, Xinxin

AU - Hua, Zhengyu

AU - Yang, Weiqiang

AU - Wu, Xiaopeng

AU - Wu, Yuzhen

AU - Chen, Shixia

AU - Hong, Wei

AU - Deng, Shuguang

AU - Zhang, Jie

AU - Wang, Jun

PY - 2024/8/9

Y1 - 2024/8/9

N2 - Carbon layer-coated CuX (CuX@C, X = P, S, Se) with different electron densities on the carbon coating layers have been successfully prepared. Among them, Cu3P@C, which has a high-electron-density carbon coating layer, delivers a high faradaic efficiency for methanol of 61.2% at −0.36 V versus reversible hydrogen electrode (RHE), and a record partial current density for methanol of 130 mA cm-2 at −0.76 V versus RHE when it is assembled on a gas diffusion electrode in a flow cell setup using 1 M KOH electrolyte, outperforming most of the state-of-the-art electrocatalysts. In contrast, Cu2Se@C and Cu1.8S@C, which have low-electron-density carbon coating layers, predominately produce formate. In situ Raman spectroscopy analysis and computational density functional theory calculations reveal the influence of Cu3P on the electronic properties of carbon binding sites and the underlying mechanisms for methanol production.

AB - Carbon layer-coated CuX (CuX@C, X = P, S, Se) with different electron densities on the carbon coating layers have been successfully prepared. Among them, Cu3P@C, which has a high-electron-density carbon coating layer, delivers a high faradaic efficiency for methanol of 61.2% at −0.36 V versus reversible hydrogen electrode (RHE), and a record partial current density for methanol of 130 mA cm-2 at −0.76 V versus RHE when it is assembled on a gas diffusion electrode in a flow cell setup using 1 M KOH electrolyte, outperforming most of the state-of-the-art electrocatalysts. In contrast, Cu2Se@C and Cu1.8S@C, which have low-electron-density carbon coating layers, predominately produce formate. In situ Raman spectroscopy analysis and computational density functional theory calculations reveal the influence of Cu3P on the electronic properties of carbon binding sites and the underlying mechanisms for methanol production.

KW - electrochemical CO reduction

KW - electronic effect

KW - intermediate binding

KW - methanol production

KW - product selectivity

UR - https://www.scopus.com/pages/publications/85200891346

U2 - 10.1021/acscatal.4c02465

DO - 10.1021/acscatal.4c02465

M3 - Article

AN - SCOPUS:85200891346

SN - 2155-5435

VL - 14

SP - 12783

EP - 12791

JO - ACS Catalysis

JF - ACS Catalysis

IS - 17

ER -

Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO₂ to Methanol on Cu₃P@C

Abstract

Keywords

Access to Document

Other files and links

ARC Centre of Excellence for Green Electrochemical Transformation of Carbon Dioxide

Cite this

Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO2 to Methanol on Cu3P@C

Abstract

Keywords

Access to Document

Other files and links

Projects

ARC Centre of Excellence for Green Electrochemical Transformation of Carbon Dioxide

Cite this

Modulating Electronic Properties of Carbon for Selective Electrochemical Reduction of CO₂ to Methanol on Cu₃P@C