Engineering Surface Atomic Architecture of NiTe Nanocrystals Toward Efficient Electrochemical N2 Fixation. (5th August 2020)

• Record Type: Journal Article
• Authors: Yuan, Menglei; Li, Qiongguang; Zhang, Jingxian; Wu, Jiawen; Zhao, Tongkun; Liu, Zhanjun; Zhou, Le; He, Hongyan; Li, Bin; Zhang, Guangjin
• Is Part Of: Advanced functional materials. Volume 30:Number 39(2020)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2020-08-05
• Subjects: crystal facets -- nickel telluride -- nitrogen reduction reaction -- surface atomic architecture; Materials -- Periodicals; Chemical vapor deposition -- Periodicals; 620.11
• DOI: 10.1002/adfm.202004208
• Languages: English
• ISSNs: 1616-301X

Abstract

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. Abstract : 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.