Governing Interlayer Strain in Bismuth Nanocrystals for Efficient Ammonia Electrosynthesis from Nitrate Reduction.
basic_science · Level V
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- Also identified by DOI 10.1021/acsnano.2c00101.
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Abstract
Electrochemical ammonia (NH<sub>3</sub>) synthesis from nitrate (NO<sub>3</sub><sup>-</sup>) reduction offers an intriguing approach for both sustainable ammonia synthesis and environmental denitrification, yet it remains hindered by a complicated reaction pathway with various intermediates. Here we present that the interlayer strain compression in bismuth (Bi) nanocrystals can contribute to both activity and selectivity improvement toward NH<sub>3</sub> electrosynthesis from NO<sub>3</sub><sup>-</sup> reduction. By virtue of comprehensive spectroscopic studies and theoretical calculations, we untangle that the interlayer lattice compression shortens Bi-Bi bond to broaden the 6<i>p</i> bandwidth for electron delocalization, promoting the chemical affinities of nitrogen intermediates. Such a manipulation facilitates NO<sub>3</sub><sup>-</sup> activation to reduce the energy barrier for activity improvement, and also alleviates *NO<sub>2</sub> desorption to suppress nitrite generation. As a result, a strain-compressive Bi electrocatalyst yields a maximal Faradaic efficiency of 90.6% and high generation rate of 46.5 g h<sup>-1</sup> g<sub>cat</sub><sup>-1</sup> with industrially scalable partial current density up to 300 mA cm<sup>-2</sup> for NH<sub>3</sub> product at the optimized conditions, respectively.