Construction of Metal-N2O2 Sites on Poly(ionic liquid) for Highly Efficient Electrocatalytic CO2 Reduction

Shu Fan Lv; Xiao Qiang Li; Yi Ran Du; Rui Wang; Zhao Rong Yan; Jia Ni Li; Rui Zhang; Bao Hua Xu

doi:10.1021/acsami.5c06177

Construction of Metal-N₂O₂ Sites on Poly(ionic liquid) for Highly Efficient Electrocatalytic CO₂ Reduction

Shu Fan Lv, Xiao Qiang Li, Yi Ran Du^*, Rui Wang, Zhao Rong Yan, Jia Ni Li, Rui Zhang^*, Bao Hua Xu^*

^*Corresponding author for this work

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

Abstract

In this study, atomically dispersed metal catalysts of Salen-PIL(M) (M = Zn and Cu) for electrochemical CO₂-to-C₁ conversion were fabricated by polymerization of a vinyl-decorated ionic liquid (IL) monomer bearing a Salen-M moiety with para-diethylbenzene. The characterization results indicated that the Salen-Zn/Cu complex was atomically dispersed in the PIL skeleton. They differed significantly in the electron transfer speed to CO₂, CO affinity, and H₂O activation, which influenced both the activity and selectivity toward CO or CH₄. Besides, the formation of CO₂^•-* and H₂O activation were related to the tolerance of the pH range. Meanwhile, the adjustment of the interfacial H₂O content by introducing a hydrophobic IL benefited the competitive CO₂RR versus HER on Salen-PIL(Zn/Cu) catalysts. As a result, Salen-PIL(Zn) provided a CO faradaic efficiency (FE_CO) of 90.1% with a partial current density (j_CO) of 90.1 mA cm^-2 at −0.85 V, while a FE_CH4 of 54.5% with j_CH4 of 272.5 mA cm^-2 at −1.60 V was obtained on Salen-PIL(Cu).

Original language	English
Pages (from-to)	37927-37935
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	17
Issue number	26
DOIs	http://doi.org/10.1021/acsami.5c06177
Publication status	Published - 2 Jul 2025
Externally published	Yes

Keywords

CH production
CO electroreduction
CO production
metal−NO sites
poly(ionic liquids)

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10.1021/acsami.5c06177

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title = "Construction of Metal-N2O2 Sites on Poly(ionic liquid) for Highly Efficient Electrocatalytic CO2 Reduction",

abstract = "In this study, atomically dispersed metal catalysts of Salen-PIL(M) (M = Zn and Cu) for electrochemical CO2-to-C1 conversion were fabricated by polymerization of a vinyl-decorated ionic liquid (IL) monomer bearing a Salen-M moiety with para-diethylbenzene. The characterization results indicated that the Salen-Zn/Cu complex was atomically dispersed in the PIL skeleton. They differed significantly in the electron transfer speed to CO2, CO affinity, and H2O activation, which influenced both the activity and selectivity toward CO or CH4. Besides, the formation of CO2•-* and H2O activation were related to the tolerance of the pH range. Meanwhile, the adjustment of the interfacial H2O content by introducing a hydrophobic IL benefited the competitive CO2RR versus HER on Salen-PIL(Zn/Cu) catalysts. As a result, Salen-PIL(Zn) provided a CO faradaic efficiency (FECO) of 90.1\% with a partial current density (jCO) of 90.1 mA cm-2 at −0.85 V, while a FECH4 of 54.5\% with jCH4 of 272.5 mA cm-2 at −1.60 V was obtained on Salen-PIL(Cu).",

keywords = "CH production, CO electroreduction, CO production, metal−NO sites, poly(ionic liquids)",

author = "Lv, \{Shu Fan\} and Li, \{Xiao Qiang\} and Du, \{Yi Ran\} and Rui Wang and Yan, \{Zhao Rong\} and Li, \{Jia Ni\} and Rui Zhang and Xu, \{Bao Hua\}",

note = "Publisher Copyright: {\textcopyright} 2025 American Chemical Society.",

year = "2025",

month = jul,

day = "2",

doi = "10.1021/acsami.5c06177",

language = "English",

volume = "17",

pages = "37927--37935",

journal = "ACS Applied Materials and Interfaces",

issn = "1944-8244",

publisher = "American Chemical Society",

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TY - JOUR

T1 - Construction of Metal-N2O2 Sites on Poly(ionic liquid) for Highly Efficient Electrocatalytic CO2 Reduction

AU - Lv, Shu Fan

AU - Li, Xiao Qiang

AU - Du, Yi Ran

AU - Wang, Rui

AU - Yan, Zhao Rong

AU - Li, Jia Ni

AU - Zhang, Rui

AU - Xu, Bao Hua

PY - 2025/7/2

Y1 - 2025/7/2

N2 - In this study, atomically dispersed metal catalysts of Salen-PIL(M) (M = Zn and Cu) for electrochemical CO2-to-C1 conversion were fabricated by polymerization of a vinyl-decorated ionic liquid (IL) monomer bearing a Salen-M moiety with para-diethylbenzene. The characterization results indicated that the Salen-Zn/Cu complex was atomically dispersed in the PIL skeleton. They differed significantly in the electron transfer speed to CO2, CO affinity, and H2O activation, which influenced both the activity and selectivity toward CO or CH4. Besides, the formation of CO2•-* and H2O activation were related to the tolerance of the pH range. Meanwhile, the adjustment of the interfacial H2O content by introducing a hydrophobic IL benefited the competitive CO2RR versus HER on Salen-PIL(Zn/Cu) catalysts. As a result, Salen-PIL(Zn) provided a CO faradaic efficiency (FECO) of 90.1% with a partial current density (jCO) of 90.1 mA cm-2 at −0.85 V, while a FECH4 of 54.5% with jCH4 of 272.5 mA cm-2 at −1.60 V was obtained on Salen-PIL(Cu).

AB - In this study, atomically dispersed metal catalysts of Salen-PIL(M) (M = Zn and Cu) for electrochemical CO2-to-C1 conversion were fabricated by polymerization of a vinyl-decorated ionic liquid (IL) monomer bearing a Salen-M moiety with para-diethylbenzene. The characterization results indicated that the Salen-Zn/Cu complex was atomically dispersed in the PIL skeleton. They differed significantly in the electron transfer speed to CO2, CO affinity, and H2O activation, which influenced both the activity and selectivity toward CO or CH4. Besides, the formation of CO2•-* and H2O activation were related to the tolerance of the pH range. Meanwhile, the adjustment of the interfacial H2O content by introducing a hydrophobic IL benefited the competitive CO2RR versus HER on Salen-PIL(Zn/Cu) catalysts. As a result, Salen-PIL(Zn) provided a CO faradaic efficiency (FECO) of 90.1% with a partial current density (jCO) of 90.1 mA cm-2 at −0.85 V, while a FECH4 of 54.5% with jCH4 of 272.5 mA cm-2 at −1.60 V was obtained on Salen-PIL(Cu).

KW - CH production

KW - CO electroreduction

KW - CO production

KW - metal−NO sites

KW - poly(ionic liquids)

UR - http://www.scopus.com/pages/publications/105009038889

U2 - 10.1021/acsami.5c06177

DO - 10.1021/acsami.5c06177

M3 - Article

AN - SCOPUS:105009038889

SN - 1944-8244

VL - 17

SP - 37927

EP - 37935

JO - ACS Applied Materials and Interfaces

JF - ACS Applied Materials and Interfaces

IS - 26

ER -

Construction of Metal-N₂O₂ Sites on Poly(ionic liquid) for Highly Efficient Electrocatalytic CO₂ Reduction

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