Atomically Dispersed Uranium Enables an Unprecedentedly High NH<sub>3</sub> Yield Rate.
basic_science · Level V
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- Record sourced from PubMed, PMID 35604434.
- Also identified by DOI 10.1021/acs.nanolett.2c01185.
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Abstract
The low NH<sub>3</sub> yield rate is a grand challenge for electrocatalytic N<sub>2</sub> reduction to NH<sub>3</sub>. Herein, we report the first uranium single-atom catalyst (SAC) capable of catalyzing the electrochemical N<sub>2</sub> reduction reaction (NRR). The uranium SAC features a low limiting potential (<0.5 V) and near-zero free energy changes for N<sub>2</sub> adsorption and NH<sub>3</sub> desorption. The integration of these merits enables the uranium SAC to afford an unprecedentedly high NH<sub>3</sub> yield rate, 3-4 orders of magnitude higher than that of the Ru(0001) surface, which is widely recognized as an excellent NRR electrocatalyst. Further theoretical analysis reveals that the N<sub>2</sub> reduction catalyzed by the uranium SAC is synergistically regulated by the <i>d</i> and <i>f</i> electrons of atomic uranium. This work proposes a promising solution (that is, atomically dispersed uranium) to the daunting challenge associated with the low NH<sub>3</sub> yield rate, thus enabling the scalable production of NH<sub>3</sub> via electrochemical N<sub>2</sub> reduction.