Engineering Surface Atomic Architecture of NiTe Nanocrystals Toward Efficient Electrochemical N₂ Fixation

Abstract Efficient N₂ fixation at ambient condition through electrochemical processes has been regarded as a promising alternative to traditional Haber–Bosch technology. Engineering surface atomic architecture of the catalysts to generate desirable active sites is important to facilitate electrochemical nitrogen reduction reaction (NRR) while suppressing the competitive hydrogen evolution reaction. Herein, nickel telluride nanocrystals with selectively exposed {001} and {010} facets are synthesized by a simple process, realizing the manipulation of surface chemistry at the atomic level. It is found that the catalysts expose the {001} facets coupled with desirable Ni sites, which possess high Faraday efficiency of 17.38 ± 0.36% and NH₃ yield rate of 33.34 ± 0.70 μg h⁻¹ mg⁻¹ at ‐0.1 V vs RHE, outperforming other samples enclosed by {010} facets (8.56 ± 0.22%, 12.78 ± 0.43 μg h⁻¹ mg⁻¹). Both experimental results and computational simulations reveal that {001} facets, with selectively exposed Ni sites, guarantee the adsorption and activation of N₂ and weaken the binding for *H species. Moreover, the enhanced reduction capacity and accelerated charge transfer kinetics also contribute the superior NRR performance of {001} facets. This work presents a novel strategy in designing nonprecious NRR electrocatalyst with exposed favorable active sites.