Synergistic bimetallic CuPd oxide alloy electrocatalyst for ammonia production from the electrochemical nitrate reaction

The electrochemical nitrate reduction reaction (eNO 3 RRs) can produce value-added chemicals such as ammonia (NH 3 ) via multiple steps. Here, we demonstrate that bimetallic Cu-Pd-O x alloy electrocatalysts can promote selective NH 3 production from the eNO 3 RR, especially at low overpotential, by...

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Published in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2022-11, Vol.1 (44), p.2376-23769
Main Authors: Jung, Wonsang, Jeong, Jaewoo, Chae, Younghyun, Lee, Woong Hee, Ko, Young-Jin, Chae, Keun Hwa, Oh, Hyung-suk, Lee, Ung, Lee, Dong Ki, Min, Byoung Koun, Shin, Hyeyoung, Hwang, Yun Jeong, Won, Da Hye
Format: Article
Language:English
Subjects:
Ammonia
Bimetals
Catalysts
Chemical reduction
Copper
Electrocatalysts
Electrochemistry
Fine structure
Hydrogenation
Nitrate reduction
Nitrogen dioxide
Palladium
Selectivity
Synergistic effect
Ultrastructure
X ray absorption
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Summary:The electrochemical nitrate reduction reaction (eNO 3 RRs) can produce value-added chemicals such as ammonia (NH 3 ) via multiple steps. Here, we demonstrate that bimetallic Cu-Pd-O x alloy electrocatalysts can promote selective NH 3 production from the eNO 3 RR, especially at low overpotential, by accelerating the rate-determining hydrogenation of NO 2 − , a critical intermediate, on the Cu catalyst. The synergistic effect of Cu and Pd affords 14 times higher NH 3 yield (1.41 mg h −1 cm −2 ) at −0.2 V RHE with an optimum composition (Cu 0.65 Pd 0.35 O x ) than that obtained using bare CuO x . The operando near edge X-ray absorption fine structure (NEXAFS) and simulation results support that the high hydrogen affinity of Pd facilitates sequential hydrogenation on metallic Cu active sites, consequently increasing the NH 3 selectivity and production rate. Our study sheds light on the mechanism of the catalytic eNO 3 RR and presents a design strategy for more advanced eNO 3 RR electrocatalysts. Bimetallic CuPd oxide alloy electrocatalysts can promote selective ammonia production from the nitrate reduction reaction by accelerating the rate-determining hydrogenation of nitrite, which is a critical intermediate.
ISSN:2050-7488
2050-7496
DOI:10.1039/d2ta06316f