Electrochemical Synthesis of NH3 at Low Temperature and Atmospheric Pressure Using a γ-Fe2O3 Catalyst

Jimin Kong, Ahyoun Lim, Changwon Yoon, Jong Hyun Jang, Hyung Chul Ham, Jonghee Han, SukWoo Nam, Dokyoon Kim, Yung Eun Sung, Jungkyu Choi, Hyun S. Park

Research output: Contribution to journalArticle

88 Citations (Scopus)

Abstract

The electrochemical synthesis of NH3 by the nitrogen reduction reaction (NRR) at low temperature (<65 °C) and atmospheric pressure using nanosized γ-Fe2O3 electrocatalysts were demonstrated. The activity and selectivity of the catalyst was investigated both in a 0.1 M KOH electrolyte and when incorporated into an anion-exchange membrane electrode assembly (MEA). In a half-reaction experiment conducted in a KOH electrolyte, the γ-Fe2O3 electrode presented a faradaic efficiency of 1.9% and a weight-normalized activity of 12.5 nmol h-1 mg-1 at 0.0 VRHE. However, the selectivity toward N2 reduction decreased at more negative potentials owing to the competing proton reduction reaction. When the γ-Fe2O3 nanoparticles were coated onto porous carbon paper to form an electrode for a MEA, their weight-normalized activity for N2 reduction was found to increase dramatically to 55.9 nmol h-1 mg-1. However, the weight- and area-normalized N2 reduction activities of γ-Fe2O3 decreased progressively from 35.9 to 14.8 nmol h-1 mg-1 and from 0.105 to 0.043 nmol h-1 cm-2 act, respectively, during a 25 h MEA durability test. In summary, a study of the fundamental behavior and catalytic activity of γ-Fe2O3 nanoparticles in the electrochemical synthesis of NH3 under low temperature and pressure is presented.

Original languageEnglish
Pages (from-to)10986-10995
Number of pages10
JournalACS Sustainable Chemistry and Engineering
Volume5
Issue number11
DOIs
Publication statusPublished - 2017 Nov 6

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atmospheric pressure
Atmospheric pressure
electrode
catalyst
Electrodes
Catalysts
membrane
Membranes
electrolyte
Electrolytes
Catalyst activity
Temperature
Nanoparticles
Catalyst selectivity
Electrocatalysts
durability
Anions
Protons
low pressure
ion exchange

Keywords

  • Electrocatalyst
  • Electrochemical ammonia synthesis
  • Iron oxide
  • Membrane electrode assembly

ASJC Scopus subject areas

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

Cite this

Electrochemical Synthesis of NH3 at Low Temperature and Atmospheric Pressure Using a γ-Fe2O3 Catalyst. / Kong, Jimin; Lim, Ahyoun; Yoon, Changwon; Jang, Jong Hyun; Ham, Hyung Chul; Han, Jonghee; Nam, SukWoo; Kim, Dokyoon; Sung, Yung Eun; Choi, Jungkyu; Park, Hyun S.

In: ACS Sustainable Chemistry and Engineering, Vol. 5, No. 11, 06.11.2017, p. 10986-10995.

Research output: Contribution to journalArticle

Kong, Jimin ; Lim, Ahyoun ; Yoon, Changwon ; Jang, Jong Hyun ; Ham, Hyung Chul ; Han, Jonghee ; Nam, SukWoo ; Kim, Dokyoon ; Sung, Yung Eun ; Choi, Jungkyu ; Park, Hyun S. / Electrochemical Synthesis of NH3 at Low Temperature and Atmospheric Pressure Using a γ-Fe2O3 Catalyst. In: ACS Sustainable Chemistry and Engineering. 2017 ; Vol. 5, No. 11. pp. 10986-10995.
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AU - Han, Jonghee

AU - Nam, SukWoo

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AB - The electrochemical synthesis of NH3 by the nitrogen reduction reaction (NRR) at low temperature (<65 °C) and atmospheric pressure using nanosized γ-Fe2O3 electrocatalysts were demonstrated. The activity and selectivity of the catalyst was investigated both in a 0.1 M KOH electrolyte and when incorporated into an anion-exchange membrane electrode assembly (MEA). In a half-reaction experiment conducted in a KOH electrolyte, the γ-Fe2O3 electrode presented a faradaic efficiency of 1.9% and a weight-normalized activity of 12.5 nmol h-1 mg-1 at 0.0 VRHE. However, the selectivity toward N2 reduction decreased at more negative potentials owing to the competing proton reduction reaction. When the γ-Fe2O3 nanoparticles were coated onto porous carbon paper to form an electrode for a MEA, their weight-normalized activity for N2 reduction was found to increase dramatically to 55.9 nmol h-1 mg-1. However, the weight- and area-normalized N2 reduction activities of γ-Fe2O3 decreased progressively from 35.9 to 14.8 nmol h-1 mg-1 and from 0.105 to 0.043 nmol h-1 cm-2 act, respectively, during a 25 h MEA durability test. In summary, a study of the fundamental behavior and catalytic activity of γ-Fe2O3 nanoparticles in the electrochemical synthesis of NH3 under low temperature and pressure is presented.

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