Journal
ACS CATALYSIS
Volume 11, Issue 1, Pages 435-445Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c03985
Keywords
electrochemical nitrogen reduction reaction; NH3 production; copper sulfide; catalyst degradation; electrochemical regeneration
Categories
Funding
- Creative Materials Discovery Program through the National Research Foundation of Korea [NRF-2016M3D1A1021140]
- Korea Institute of Science and Technology [2V07940, 2E30380]
- NRF - Korea government (MSIT) [2018M1A2A2061975, 2019R1A2B5B03004854]
- National Research Foundation of Korea [2018M1A2A2061975, 2019R1A2B5B03004854] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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The electrochemical nitrogen reduction reaction (NRR) is a promising method for energy-efficient and low-emission NH3 production. A copper sulfide-based electrocatalyst is used for electrochemical NH3 production, but the catalyst undergoes reductive degradation during the NRR process. A regenerative electrochemical sulfur cycle is introduced to revive the crystal structure and NRR activities of Cu9S5 for continuous electrochemical NH3 production.
Electrochemical nitrogen reduction reaction (NRR) is a promising method for energy-efficient and low-emission NH3 production. Herein, we report electrochemical NH3 production using a copper sulfide-based electrocatalyst. A solid-state synthesis is employed to prepare the Cu9S5 catalyst for artificial N-2 fixation in a neutral aqueous electrolyte. Despite an excellent NRR activity of 10.8 +/- 0.4 mu g/hcm(2) at -0.5 V-RHE, however, the catalyst itself is reductively degraded during the NRR. To achieve continuous electrochemical NH3 production, a regenerative electrochemical sulfur cycle is introduced that revives the Cu9S5 crystal structure and NRR activities. The electrochemical regeneration process reconstructing the metal-sulfur bond in between sequential NH3 production processes restores the NRR activity. Importantly, catalytic surfaces providing a labile sulfhydryl functional group attached to the N-2-adsorption metal center are required to achieve efficient NRR activity under ambient conditions.
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