Accelerating Tandem Electroreduction of Nitrate to Ammonia via Multi-Site Synergy in Mesoporous Carbon-Supported High-Entropy Intermetallics.
basic_science · Level V
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- Record sourced from PubMed, PMID 39648538.
- Also identified by DOI 10.1002/adma.202413560.
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Abstract
The electrochemical nitrate reduction reaction (NO<sub>3</sub> <sup>-</sup>RR) for ammonia (NH<sub>3</sub>) synthesis represents a significant technological advancement, yet it involves a cascade of elementary reactions alongside various intermediates. Thus, the development of multi-site catalysts for enhancing NO<sub>3</sub> <sup>-</sup>RR and understanding the associated reaction mechanisms for NH<sub>3</sub> synthesis is vital. Herein, a versatile approach is presented to construct platinum based high-entropy intermetallic (HEI) library for NH<sub>3</sub> synthesis. The HEI nanoparticles (NPs) are uniformly supported on a 2D nitrogen doped mesoporous carbon (N-mC) framework, featured with adjustable compositions (up to eight elements) and a high degree of atomic order (over 90%). Guided by the density functional theory (DFT) calculations and atomic structural analysis, a quinary Pt<sub>0.8</sub>Fe<sub>0.2</sub>Co<sub>0.2</sub>Ni<sub>0.2</sub>Cu<sub>0.2</sub> HEI NPs based N-mC catalyst is designed, which demonstrates a large ammonia Faradaic efffciency (>97%) and a remarkable recyclability (>20 cycles) under both acidic and basic conditions. The combined in situ experimental analysis and further DFT calculation suggests that the well-defined multi-sites nature of the HEI NPs cooperate for a tandem reduction mechanism, in which the Pt-X (X represents the other four transition elements) bridging sites offer optimal adsorption for key nitrogen-oxygen species while the Pt sites facilitate the generation and adsorption of *H species.