Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction

Yongtao Meng, Xiao Zhang, Wei Hsuan Hung, Junkai He, Yi Sheng Tsai, Yun Kuang, Michael J. Kenney, Jing Jong Shyue, Yijin Liu, Kevin H. Stone, Xueli Zheng, Steven L. Suib, Meng Chang Lin, Yongye Liang, Hongjie Dai

Research output: Contribution to journalArticlepeer-review

27 Citations (Scopus)

Abstract

Electrochemical reduction of CO2 to useful chemicals has been actively pursued for closing the carbon cycle and preventing further deterioration of the environment/climate. Since CO2 reduction reaction (CO2RR) at a cathode is always paired with the oxygen evolution reaction (OER) at an anode, the overall efficiency of electrical energy to chemical fuel conversion must consider the large energy barrier and sluggish kinetics of OER, especially in widely used electrolytes, such as the pH-neutral CO2-saturated 0.5 M KHCO3. OER in such electrolytes mostly relies on noble metal (Ir- and Ru-based) electrocatalysts in the anode. Here, we discover that by anodizing a metallic Ni–Fe composite foam under a harsh condition (in a low-concentration 0.1 M KHCO3 solution at 85 °C under a high-current ∼250 mA/cm2), OER on the NiFe foam is accompanied by anodic etching, and the surface layer evolves into a nickel–iron hydroxide carbonate (NiFe-HC) material composed of porous, poorly crystalline flakes of flower-like NiFe layer-double hydroxide (LDH) intercalated with carbonate anions. The resulting NiFe-HC electrode in CO2-saturated 0.5 M KHCO3 exhibited OER activity superior to IrO2, with an overpotential of 450 and 590 mV to reach 10 and 250 mA/cm2, respectively, and high stability for >120 h without decay. We paired NiFe-HC with a CO2RR catalyst of cobalt phthalocyanine/carbon nanotube (CoPc/CNT) in a CO2 electrolyzer, achieving selective cathodic conversion of CO2 to CO with >97% Faradaic efficiency and simultaneous anodic water oxidation to O2. The device showed a low cell voltage of 2.13 V and high electricity-to-chemical fuel efficiency of 59% at a current density of 10 mA/cm2

Original languageEnglish
Pages (from-to)23915-23922
Number of pages8
JournalProceedings of the National Academy of Sciences of the United States of America
Volume116
Issue number48
DOIs
Publication statusPublished - Nov 26 2019
Externally publishedYes

Keywords

  • CO electrolyzer
  • CO reduction
  • Electrocatalysis
  • Oxygen evolution
  • PH-neutral electrolyte

ASJC Scopus subject areas

  • General

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