Oxygen-deficient SnO2 nanoparticles with ultrathin carbon shell for efficient electrocatalytic N2 reduction

Abstract

For high-efficiency NH3 synthesis via ambient-condition electrohydrogenation of inert N2, it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency, good conductivity and large surface area. Here, oxygen-deficient SnO2 nanoparticles encapsulated by ultrathin carbon layer (d-SnO2@C) are developed by hydrothermal deposition coupled with annealing process, as promising catalysts for ambient electrocatalytic N2 reduction. d-SnO2@C exhibits high activity and excellent selectivity for electrocatalytic conversion of N2 to NH3 in acidic electrolytes, with Faradic efficiency as high as 12.7% at −0.15 V versus the reversible hydrogen electrode (RHE) and large NH3 yield rate of 16.68 μg h−1 mgcat−1 at −0.25 V vs. RHE in 0.1 mol L−1 HCl. Benefiting from the structural superiority of enhanced charge transfer efficiency and optimized surface states, d-SnO2@C also achieves excellent long-term stability.