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

• Published in: Advanced functional materials Vol. 30; no. 39
• Main Authors: Yuan, Menglei, Li, Qiongguang, Zhang, Jingxian, Wu, Jiawen, Zhao, Tongkun, Liu, Zhanjun, Zhou, Le, He, Hongyan, Li, Bin, Zhang, Guangjin
• Format: Journal Article
• Language: English
• Published: Hoboken Wiley Subscription Services, Inc 01.09.2020
• Subjects: Ammonia; Architecture; Catalysts; Charge transfer; Chemical reduction; Computer simulation; crystal facets; Electrocatalysts; Exposure; Hydrogen evolution reactions; Materials science; Nanocrystals; Nickel; nickel telluride; nitrogen reduction reaction; Nitrogenation; Reaction kinetics; surface atomic architecture; Tellurides
• ISSN: 1616-301X; 1616-3028
• DOI: 10.1002/adfm.202004208

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. Although Ni (nickel) sites display desirable electrochemical nitrogen reduction reaction activity (NRR), realizing the manipulation of catalysts, surface chemistry at the atomic level to expose Ni sites to maximize catalytic performance is rarely reported. Herein, a simple strategy is reported for engineering the surface atomic architecture of nickel telluride nanocrystals to expose Ni sites at the surface toward efficient NRR.