PdNi nanosheets boost nitrate electroreduction to ammonia. Issue 5 (October 2022)

• Record Type: Journal Article
• Authors: Zhang, Guike; Li, Xingchuan; Shen, Peng; Luo, Yaojing; Li, Xiaotian; Chu, Ke
• Is Part Of: Journal of environmental chemical engineering. Volume 10:Issue 5(2022)
• Publication Date: 2022-10
• Subjects: Electrochemical nitrate reduction -- PdNi nanosheets -- Density functional theory -- Molecular dynamics simulations; Chemical engineering -- Environmental aspects -- Periodicals; Environmental engineering -- Periodicals; Chemical engineering -- Environmental aspects; Environmental engineering; Periodicals; 660.0286
• DOI: 10.1016/j.jece.2022.108362
• Languages: English
• ISSNs: 2213-2929

Abstract

Abstract: Electrochemical NO3 − -to-NH3 reduction reaction (NO3 RR) represents an environmentally-friendly way to not only degrade NO3 − in contaminated water, but also produce value-added NH3 with a high efficiency. Herein, we first demonstrate Ni-alloyed PdNi nanosheets as a high-performing NO3 RR catalyst, which presents the maximum NH3 yield rate of 16.7 mg h −1 mg −1 at − 1.2 V (RHE) and the highest FE of 87.9% at − 0.6 V (RHE), together with the good catalytic durability. Combined density functional theory and molecular dynamics simulations reveal that Ni alloying can effectively modulate the electronic configuration of Pd to enable the favorable desorption of produced NH3, resulting in decreased hydrogenation energy barrier and boosted NO3 RR energetics. Graphical Abstract: ga1 Highlights: PdNi nanosheets are explored as an effective nitrate electroreduction (NO3 RR) catalyst for NH3 electrosynthesis. PdNi nanosheets exhibit a maximum NH3 yield rate of 16.7 mg h -1 cm -2 at −1.2 V and a highest FE of 87.9% at − 0.6 V. Theoretical calculations reveal that Ni alloying decreases the hydrogenation energy barrier for boosted NO 3 RR energetics.