TY - JOUR
T1 - Laser-Induced Pd-PdO/rGO Catalysts for Enhanced Electrocatalytic Conversion of Nitrate into Ammonia
AU - Ebenezer, James
AU - Lal, Aneena
AU - Velayudham, Parthiban
AU - Borenstein, Arie
AU - Schechter, Alex
N1 - Publisher Copyright:
© 2024 The Authors. Published by American Chemical Society.
PY - 2024/7/17
Y1 - 2024/7/17
N2 - Electrochemical reduction of nitrate to ammonia (eNO3RR) is proposed as a sustainable solution for high-rate ammonia synthesis under ambient conditions. The complex, multistep eNO3RR mechanism necessitates the use of a catalyst for the complete conversion of nitrate to ammonia. Our research focuses on developing a novel Pd-PdO doped in a reduced graphene oxide (rGO) composite catalyst synthesized via a laser-assisted one-step technique. This catalyst demonstrates dual functionality: palladium (Pd) boosts hydrogen adsorption, while its oxide (PdO) demonstrates considerable nitrogen adsorption affinity and exhibits a maximum ammonia yield of 5456.4 ± 453.4 μg/h/cm2 at −0.6 V vs reversible hydrogen electrode (RHE), with significant yields for nitrite and hydroxylamine under ambient conditions in a nitrate-containing alkaline electrolyte. At a lower potential of −0.1 V, the catalyst exhibited a minimal hydrogen evolution reaction of 3.1 ± 2.2% while achieving high ammonia selectivity (74.9 ± 4.4%), with the balance for nitrite and hydroxylamine. Additionally, the catalyst’s stability and activity can be regenerated through the electrooxidation of Pd.
AB - Electrochemical reduction of nitrate to ammonia (eNO3RR) is proposed as a sustainable solution for high-rate ammonia synthesis under ambient conditions. The complex, multistep eNO3RR mechanism necessitates the use of a catalyst for the complete conversion of nitrate to ammonia. Our research focuses on developing a novel Pd-PdO doped in a reduced graphene oxide (rGO) composite catalyst synthesized via a laser-assisted one-step technique. This catalyst demonstrates dual functionality: palladium (Pd) boosts hydrogen adsorption, while its oxide (PdO) demonstrates considerable nitrogen adsorption affinity and exhibits a maximum ammonia yield of 5456.4 ± 453.4 μg/h/cm2 at −0.6 V vs reversible hydrogen electrode (RHE), with significant yields for nitrite and hydroxylamine under ambient conditions in a nitrate-containing alkaline electrolyte. At a lower potential of −0.1 V, the catalyst exhibited a minimal hydrogen evolution reaction of 3.1 ± 2.2% while achieving high ammonia selectivity (74.9 ± 4.4%), with the balance for nitrite and hydroxylamine. Additionally, the catalyst’s stability and activity can be regenerated through the electrooxidation of Pd.
KW - bifunctionality
KW - environmental remediation
KW - hydroxylamine
KW - laser processing
KW - nitrate reduction
KW - nitrite
UR - http://www.scopus.com/inward/record.url?scp=85199084292&partnerID=8YFLogxK
U2 - 10.1021/acsami.4c06378
DO - 10.1021/acsami.4c06378
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C2 - 38961637
AN - SCOPUS:85199084292
SN - 1944-8244
VL - 16
SP - 36433
EP - 36443
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 28
ER -