Electron Sponge Effect by Dynamic-Regulated Electron Self-Flow toward Coupled Electrochemical Ammonia Synthesis.
basic_science · Level V
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- Record sourced from PubMed, PMID 39294859.
- Also identified by DOI 10.1021/acsnano.4c11702.
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Abstract
A dynamic-regulated Pd-Fe-N electrocatalyst was effectively constructed with electron-donating and back-donating effects, which serves as an efficient engineering strategy to optimize the electrocatalytic activity. The designed PdFe<sub>3</sub>/FeN features a comprehensive electrocatalytic performance toward the nitrogen reduction reaction (NRR, yield rate of 29.94 μg h<sup>-1</sup> mg<sub>cat</sub><sup>-1</sup> and FE of 38.43% at -0.2 V vs RHE) and oxygen evolution reaction (OER, 308 mV at 100 mA cm<sup>-2</sup>). Combining <i>in situ</i> ATR-FTIR, XAS, and DFT results, the role of the interstitial-N-dopant-induced electron sponge effect has been significantly elucidated in strengthening the electrocatalytic NRR process. Specifically, the introduction of a N dopant, an electron acceptor, initiates the generation of robust Lewis-acidic Fe sites, facilitating free N<sub>2</sub> capture and bonding. Simultaneously, after NH<sub>3</sub> adsorption, the N dopant can back-donate electrons to Fe sites, strengthening the NH<sub>3</sub> deportation through weakening the Lewis acidity of Fe centers. Besides, the electron-deficient Fe sites contribute to the reconstruction of FeOOH, the real active species during the OER, which accelerates the four-electron reaction kinetics. This research offers a perspective on electrocatalyst design, potentially facilitating the evolution of advanced material engineering for efficient electrocatalytic synthesis and energy storage.