biostudies-literatureZhao ZNatural Science Foundation of Beijing MunicipalityState Key Laboratory of Organic–Inorganic CompositesNational Natural Science Foundation of ChinaBeijing University of Chemical Technology100190https://www.ebi.ac.uk/biostudies/studies/S-EPMC8693264biostudies-literatureUnknown3(1)Demand for ammonia continues to increase to sustain the growing global population. The direct electrochemical N₂ reduction reaction (NRR) powered by renewable electricity offers a promising carbon-neutral and sustainable strategy for manufacturing NH₃, 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 TaTe₂ nanosheets. Remarkable NH₃ 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 NH₄ ⁺ originate from N<sub>Innovation (Cambridge (Mass.))Engineering vacancy and hydrophobicity of two-dimensional TaTe₂ for efficient and stable electrocatalytic N₂ reduction.PMC8693264219203921972010NRF-2016M3D1A1021147XK180301201901001Choi CLv ZPark JRobertson AWBenedict Lo TWZhang HJung YHui XZhao ZSun ZHong SfalseEngineering 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 N₂ reduction reaction (NRR) powered by renewable electricity offers a promising carbon-neutral and sustainable strategy for manufacturing NH₃, 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 TaTe₂ nanosheets. Remarkable NH₃ 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 NH₄ ⁺ originate from N<sub>2022-01-01T00:00:00Z2022 Jan2025-04-18T22:14:20.442Z2022-02-11T14:48:38.642ZS-EPMC86932643498440910.1016/j.xinn.2021.100190