Salt-Free Glycine Electrosynthesis via Carbon-Nitrogen Coupling Boosted by the Lattice Strain in Atomically Thin <i>p</i>-Block Bismuthene.
basic_science · Level V
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- Also identified by DOI 10.1021/acsnano.5c19472.
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Abstract
Electrochemical carbon-nitrogen (C-N) coupling using simple inorganic feedstocks offers a sustainable route to valuable organonitrogen compounds such as amino acids. Herein, we present an atomically thin and acid-resistant <i>p</i>-block bismuthene (Bi-ene) derived via the reconstruction of a Bi-based metal-organic framework, where the enriched atomic misarrangement induces significant lattice strain that modulates the local electronic structure of the resultant Bi-ene, significantly boosting its electrocatalytic activity. Such defective Bi-ene exhibits an exceptional electrocatalytic performance for reductive C-N coupling in a salt-free acidic system, achieving a Faradaic efficiency (FE) of 95.7% and an ultrahigh yield rate of 1161 μmol cm<sup>-2</sup> h<sup>-1</sup> for NH<sub>2</sub>OH generation via the nitrate reduction reaction (NtrRR). Further, the efficient coreduction of HNO<sub>3</sub> and oxalic acid (OA) over Bi-ene simultaneously generates NH<sub>2</sub>OH and glyoxylic acid (GX) respectively, which undergo effective C-N coupling to produce glycine with a high yield of 455.4 μmol cm<sup>-2</sup> h<sup>-1</sup>. Moreover, the Bi-ene demonstrates stable performance for over 120 h at an industrial-relevant current density of 200 mA cm<sup>-2</sup>. Operando spectroscopy and calculations reveal that the strain in lattice-distorted Bi-ene optimizes the intermediate adsorption through modulating local electronic structure and thus enhances the efficacy for glycine electrosynthesis.