Size-induced d band center upshift of copper for efficient nitrate reduction to ammonia

JOURNAL OF COLLOID AND INTERFACE SCIENCE(2024)

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Abstract
Electrocatalytic nitrate reduction (NO3RR) technique has emerged as a hotspot in NH3 production, for its practicability, and a series of advanced electrocatalysts with high activity and robust stability needed to be constructed in today's era. In this work, size-tunable Cu nanoparticles on porous nitrogen-doped hexagonal carbon nanorods (Cu@NHC) were reasonably designed and served for catalyzing NO3RR in neutral media. Especially, Cu30%@NHC demonstrated a remarkable electroactivity for NH3 production as it showed a suitable grain size with massive catalytic centers and favorable d band structure with faster *NO3--to-*NO2- catalytic dynamics. As expected, Cu30%@NHC (3628.28 mu g h-1 mgcat.- 1) had a much higher NH3 yield than those for Cu20%@NHC (1268.42 mu g h-1 mgcat.-1) and Cu40%@NHC (725.03 mu g h-1 mgcat.-1). And those collected NH3 products indeed derived from NO3RR process revealed by 15N isotope-labeling and systemic control tests. Moreover, Cu30%@NHC was also durable for NO3RR bulk electrolysis with minor loss in activity. This work offered an effective modifying tactics to boost NO3RR catalysis and could guide the design of other advanced electro-catalysts via size-induced surface engineering.
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Key words
Size -tunable Cu,N -doped hexagonal carbon nanorod,d band structure,NH 3 electrosynthesis
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