Engineering vacancy and hydrophobicity of two-dimensional TaTe2 for efficient and stable electrocatalytic N2 reduction

Demand for ammonia continues to increase to sustain the growing global population. The direct electrochemical N 2 reduction reaction (NRR) powered by renewable electricity offers a promising carbon-neutral and sustainable strategy for manufacturing NH 3 , yet achieving this remains a grand challenge. Here, we report a synergistic strategy to promote ambient NRR for ammonia production by tuning the Te vacancies (V Te ) and surface hydrophobicity of two-dimensional TaTe 2 nanosheets. Remarkable NH 3 faradic efficiency of up to 32.2% is attained at a mild overpotential, which is largely maintained even after 100 h of consecutive electrolysis. Isotopic labeling validates that the N atoms of formed NH 4 + originate from N 2 . In situ X-ray diffraction indicates preservation of the crystalline structure of TaTe 2 during NRR. Further density functional theory calculations reveal that the potent…