4.8 Article

Electrochemical Nitrogen Reduction Kinetics on a Copper Sulfide Catalyst for NH3 Synthesis at Low Temperature and Atmospheric Pressure

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 21, Pages 24593-24603

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c00850

Keywords

ammonia; electrocatalyst; nitrogen reduction; copper sulfide; Tafel analysis

Funding

  1. Creative Materials Discovery Program through the National Research Foundation of Korea [NRF-2016M3D1A1021140]
  2. New & Renewable Energy Core Technology Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) - Ministry of Trade, Industry Energy (MOTIE) [20173010032210]
  3. Korea Institute of Science and Technology [2V07940, 2E30201, 2E30380]
  4. Korea Evaluation Institute of Industrial Technology (KEIT) [20173010032210] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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The Fe-CuS/C catalyst exhibits a high NH3 production rate in the nitrogen reduction reaction, but rapid degradation of the catalyst hinders precise investigation in longer measurements. However, when the degradation effect is mitigated, the NH3 production rate is enhanced with increased overpotentials.
We studied the electrochemical synthesis of NH3 on Fe-CuS/C catalysts in an alkaline aqueous solution under ambient conditions. The metal chalcogenide catalyst is active in the nitrogen reduction reaction (NRR) for approximately 45 min with an NH3 production yield of 16 mu g h(-1) cm(-2) at -0.4 V-RHE, while it decomposes to CuO. The rapid degradation of the catalyst hinders the precise investigation of the NH3 production activity in longer time measurements. Herein, the electrochemical NH3 production rate is enhanced with increased overpotentials when the degradation effect is mitigated in the measurement, which was difficult to observe in the NRR reports. In the Tafel analysis, the exchange current density, heterogeneous rate constant, and transfer coefficient of the Fe-CuS/C catalyst on the NRR were estimated. When the electrode degradation is mitigated, one of the best NH3 production activities among the reported metal sulfide electrochemical NRR catalysts is obtained, which is 42 mu g h(-1) cm(-2) at -0.6 V-RHE.

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