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Title: Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
 [1];  [2];  [3];  [4];  [5];  [6];  [6];  [7];  [8];  [8];  [9];  [4];  [10];  [11];  [6]
  1. Shandong Univ. of Science and Technology, Qingdao (China). College of Electrical Engineering and Automation; Stanford Univ., Stanford, CA (United States). Dept. of Chemistry
  2. Stanford Univ., Stanford, CA (United States). Dept. of Chemistry; South Univ. of Science and Technology of China, Shenzhen (China). Dept. of Materials Science and Engineering
  3. Stanford Univ., Stanford, CA (United States). Dept. of Chemistry; National Central Univ., Taoyuan (Taiwan). Inst. of Materials Science and Engineering
  4. Univ. of Connecticut, Storrs, CT (United States). Inst. of Materials Science
  5. National Central Univ., Taoyuan (Taiwan). Inst. of Materials Science and Engineering
  6. Stanford Univ., Stanford, CA (United States). Dept. of Chemistry
  7. Academia Sinica, Taipei (Taiwan)
  8. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  9. Stanford Univ., CA (United States)
  10. Shandong Univ. of Science and Technology, Qingdao (China). College of Electrical Engineering and Automation
  11. South Univ. of Science and Technology of China, Shenzhen (China). Dept. of Materials Science and Engineering
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Electrochemical reduction of CO2to useful chemicals has been actively pursued for closing the carbon cycle and preventing further deterioration of the environment/climate. Since CO2reduction 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 KHCO3solution 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 KHCO3exhibited 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 CO2 RR 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.

Research Organization:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
AC02-76SF00515; MOST-106-2918-I-035-002; FG02-86ER13622
OSTI ID:
1596288
Alternate ID(s):
OSTI ID: 1598226
Journal Information:
Proceedings of the National Academy of Sciences of the United States of America, Vol. 116, Issue 48; ISSN 0027-8424
Publisher:
National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 33 works
Citation information provided by
Web of Science

References (35)

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Highly selective and active CO2 reduction electrocatalysts based on cobalt phthalocyanine/carbon nanotube hybrid structures journal March 2017
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Degree of Geometric Tilting Determines the Activity of FeO 6 Octahedra for Water Oxidation journal June 2018
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Importance of Ag–Cu Biphasic Boundaries for Selective Electrochemical Reduction of CO 2 to Ethanol journal November 2017
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Non-3d Metal Modulation of a Cobalt Imidazolate Framework for Excellent Electrocatalytic Oxygen Evolution in Neutral Media journal December 2018

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
oxygen evolution
CO2 reduction
CO2 electrolyzer
electrocatalysis
pH-neutral electrolyte