Regenerative Electrocatalytic Redox Cycle of Copper Sulfide for Sustainable NH3 Production under Ambient Conditions

Authors
Kim, Hee SooChoi, JihyunKong, JiminKim, HansungYoo, Sung JongPark, Hyun S.
Issue Date
2021-01-01
Publisher
AMER CHEMICAL SOC
Citation
ACS CATALYSIS, v.11, no.1, pp.435 - 445
Abstract
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.
Keywords
CARBON SPHERES; UNS N08800; NITROGEN; CUS; REDUCTION; TEMPERATURE; NANOSHEETS; AMMONIA; N-2; NANOPARTICLES; CARBON SPHERES; UNS N08800; NITROGEN; CUS; REDUCTION; TEMPERATURE; NANOSHEETS; AMMONIA; N-2; NANOPARTICLES; electrochemical nitrogen reduction reaction; NH3 production; copper sulfide; catalyst degradation; electrochemical regeneration
ISSN
2155-5435
URI
https://pubs.kist.re.kr/handle/201004/117550
DOI
10.1021/acscatal.0c03985
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KIST Article > 2021
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