TY - JOUR
T1 - Enabling circular economy by N-recovery
T2 - Electrocatalytic reduction of nitrate with cobalt hydroxide nanocomposites on copper foam treating low conductivity groundwater effluents
AU - Cerrón-Calle, Gabriel Antonio
AU - Fajardo, Ana S.
AU - Liu, Jingyue
AU - Sánchez-Sánchez, Carlos M.
AU - Garcia-Segura, Sergi
N1 - Publisher Copyright: © 2023 Elsevier B.V.
PY - 2023/8/20
Y1 - 2023/8/20
N2 - Fertilizers play a vital role in the food-energy-water nexus. The traditional method of artificial nitrogen fixation to produce ammonia is a high-energy intensive centralized process that has caused an imbalance of the N-cycle due to the release of N-species to water. Electrocatalytic nitrate reduction (ENR) to ammonia is a promising N-resource recovery alternative that can enable the circular reuse of ammonia in decentralized settings. However, the primary challenge is identifying selective and affordable electrocatalysts. Identifying electrodes that rely on something other than platinum-group metals is required to surpass barriers associated with using expensive and endangered elements. In this study, an earth-abundant bimetallic catalyst, Cu/Co(OH)x, prepared and optimized by electrodeposition, demonstrates superior ammonia production. Under environmentally relevant conditions of 30 mg NO3−-N L−1, Cu/Co(OH)x showed higher ammonia production than pristine Cu foam with 0.7 and 0.3 mmol NH3 gcat−1 h−1, respectively. The experimental evaluation demonstrated direct reduction and catalytic hydrogenation mechanisms in Cu/Co(OH)x sites. Leaching analyses suggest that Cu/Co(OH)x has outstanding stability with negligible metal concentration below the maximum contaminant level for both Cu and Co. These results provide a framework for using earth-abundant materials in ENR with comparable efficiency and energy consumption to platinum-group materials.
AB - Fertilizers play a vital role in the food-energy-water nexus. The traditional method of artificial nitrogen fixation to produce ammonia is a high-energy intensive centralized process that has caused an imbalance of the N-cycle due to the release of N-species to water. Electrocatalytic nitrate reduction (ENR) to ammonia is a promising N-resource recovery alternative that can enable the circular reuse of ammonia in decentralized settings. However, the primary challenge is identifying selective and affordable electrocatalysts. Identifying electrodes that rely on something other than platinum-group metals is required to surpass barriers associated with using expensive and endangered elements. In this study, an earth-abundant bimetallic catalyst, Cu/Co(OH)x, prepared and optimized by electrodeposition, demonstrates superior ammonia production. Under environmentally relevant conditions of 30 mg NO3−-N L−1, Cu/Co(OH)x showed higher ammonia production than pristine Cu foam with 0.7 and 0.3 mmol NH3 gcat−1 h−1, respectively. The experimental evaluation demonstrated direct reduction and catalytic hydrogenation mechanisms in Cu/Co(OH)x sites. Leaching analyses suggest that Cu/Co(OH)x has outstanding stability with negligible metal concentration below the maximum contaminant level for both Cu and Co. These results provide a framework for using earth-abundant materials in ENR with comparable efficiency and energy consumption to platinum-group materials.
KW - Bimetallic catalysts
KW - Electrochemical water treatment
KW - Green chemistry
KW - Hydrogenation
KW - Nitrogen cycle
KW - Non‑platinum group metals (non-PGMs)
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U2 - 10.1016/j.scitotenv.2023.163938
DO - 10.1016/j.scitotenv.2023.163938
M3 - Article
C2 - 37149180
SN - 0048-9697
VL - 887
JO - Science of the Total Environment
JF - Science of the Total Environment
M1 - 163938
ER -