期刊
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
卷 343, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2023.123474
关键词
D-band center modulation; Spin orbital; B-mediation; Nitrogen activation; Electrocatalytic nitrogen fixation
This study develops a nonmetal boron mediated FeS2 material for electrocatalytic nitrogen fixation and enhances the ammonia synthesis performance by tuning the d-band center of the catalyst.
Electrocatalytic nitrogen fixation is a promising approach for ambient ammonia synthesis. The key that limits the improvement of ammonia evolution performance is the N---N bond cleavage of molecular nitrogen. One effective route to break this bottleneck is the d-band center modulation of catalysts. Herein, a nonmetal boron mediated FeS2 (B-FeS2) is developed for electrocatalytic nitrogen fixation. The B-mediation alters the spin-orbits of Fe site and upshifts the d-band center of FeS2, thus inducing a strong d-pi* interaction between the Fe site and nitrogen to activate N---N bond. Besides, the experimental and theoretical calculations indicate the B-mediation reduces the energy barrier for *NNH intermediate, thus significantly accelerating ammonia production. As a result, B-FeS2 displays high ammonia yield (1.56 mmol & sdot;g- 1 & sdot;h- 1) with 12.6 % Faradaic efficiency. This strategy of d-band center tuning induced by the B-mediation provides a distinctive insight for the design of high-efficiency electrocatalysts.
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