Selective CO2 Reduction on Zinc Electrocatalyst: The Effect of Zinc Oxidation State Induced by Pretreatment Environment

Dang Le Tri Nguyen, Michael Shincheon Jee, Da Hye Won, Hyejin Jung, Hyung Suk Oh, Byoung Koun Min, Yun Jeong Hwang

Research output: Contribution to journalArticle

18 Citations (Scopus)

Abstract

Here, we have developed porous nanostructured Zn electrocatalysts for CO2 reduction reaction (CO2RR), fabricated by reducing electrodeposited ZnO (RE-Zn) to activate the CO2RR electrocatalytic performance. We discovered that the electrochemical activation environment using CO2-bubbled electrolyte during reducing ZnO in a pretreatment step is important for highly selective CO production over H2 production, while using Ar gas bubbling instead can lead to less CO product of the Zn-based catalyst in CO2RR later. The RE-Zn activated in CO2-bubbled electrolyte condition achieves a Faradaic efficiency of CO production (FECO) of 78.5%, which is about 10% higher than that of RE-Zn activated in Ar-bubbled electrolyte. The partial current density of CO product had more 10-fold increase with RE-Zn electrodes than that of bulk Zn foil at -0.95 V vs RHE in KHCO3. In addition, a very high FECO of 95.3% can be reached using the CO2-pretreated catalyst in KCl electrolyte. The higher amount of oxidized zinc states has been found in the high performing Zn electrode surface by high-resolution X-ray photoelectron spectroscopy studies, which suggest that oxidized zinc states induce the active sites for electrochemical CO2RR. Additionally, in pre- and post-CO2RR performance tests, the carbon deposition is also significantly suppressed on RE-Zn surfaces having a higher ratio of oxidized Zn state.

Original languageEnglish
Pages (from-to)11377-11386
Number of pages10
JournalACS Sustainable Chemistry and Engineering
Volume5
Issue number12
DOIs
Publication statusPublished - 2017 Dec 4

Fingerprint

Electrocatalysts
Carbon Monoxide
Zinc
zinc
electrolyte
Electrolytes
oxidation
Oxidation
electrode
catalyst
Electrodes
Catalysts
density current
Metal foil
X-ray spectroscopy
Current density
Carbon
X ray photoelectron spectroscopy
Gases
Chemical activation

Keywords

  • CO production
  • CO reduction reaction
  • Electrocatalysis
  • Pretreatment
  • Zinc catalyst

ASJC Scopus subject areas

  • Chemistry(all)
  • Environmental Chemistry
  • Chemical Engineering(all)
  • Renewable Energy, Sustainability and the Environment

Cite this

Selective CO2 Reduction on Zinc Electrocatalyst : The Effect of Zinc Oxidation State Induced by Pretreatment Environment. / Nguyen, Dang Le Tri; Jee, Michael Shincheon; Won, Da Hye; Jung, Hyejin; Oh, Hyung Suk; Min, Byoung Koun; Hwang, Yun Jeong.

In: ACS Sustainable Chemistry and Engineering, Vol. 5, No. 12, 04.12.2017, p. 11377-11386.

Research output: Contribution to journalArticle

Nguyen, Dang Le Tri ; Jee, Michael Shincheon ; Won, Da Hye ; Jung, Hyejin ; Oh, Hyung Suk ; Min, Byoung Koun ; Hwang, Yun Jeong. / Selective CO2 Reduction on Zinc Electrocatalyst : The Effect of Zinc Oxidation State Induced by Pretreatment Environment. In: ACS Sustainable Chemistry and Engineering. 2017 ; Vol. 5, No. 12. pp. 11377-11386.
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AB - Here, we have developed porous nanostructured Zn electrocatalysts for CO2 reduction reaction (CO2RR), fabricated by reducing electrodeposited ZnO (RE-Zn) to activate the CO2RR electrocatalytic performance. We discovered that the electrochemical activation environment using CO2-bubbled electrolyte during reducing ZnO in a pretreatment step is important for highly selective CO production over H2 production, while using Ar gas bubbling instead can lead to less CO product of the Zn-based catalyst in CO2RR later. The RE-Zn activated in CO2-bubbled electrolyte condition achieves a Faradaic efficiency of CO production (FECO) of 78.5%, which is about 10% higher than that of RE-Zn activated in Ar-bubbled electrolyte. The partial current density of CO product had more 10-fold increase with RE-Zn electrodes than that of bulk Zn foil at -0.95 V vs RHE in KHCO3. In addition, a very high FECO of 95.3% can be reached using the CO2-pretreated catalyst in KCl electrolyte. The higher amount of oxidized zinc states has been found in the high performing Zn electrode surface by high-resolution X-ray photoelectron spectroscopy studies, which suggest that oxidized zinc states induce the active sites for electrochemical CO2RR. Additionally, in pre- and post-CO2RR performance tests, the carbon deposition is also significantly suppressed on RE-Zn surfaces having a higher ratio of oxidized Zn state.

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