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Atomically Dispersed Uranium Enables an Unprecedentedly High NH3 Yield Rate

机译：Atomically Dispersed Uranium Enables an Unprecedentedly High NH3 Yield Rate

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摘要

The low NH3 yield rate is a grand challenge for electrocatalytic N-2 reduction to NH3. Herein, we report the first uranium single-atom catalyst (SAC) capable of catalyzing the electrochemical N-2 reduction reaction (NRR). The uranium SAC features a low limiting potential (<0.5 V) and near-zero free energy changes for N-2 adsorption and NH3 desorption. The integration of these merits enables the uranium SAC to afford an unprecedentedly high NH3 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-2 reduction catalyzed by the uranium SAC is synergistically regulated by the d and f electrons of atomic uranium. This work proposes a promising solution (that is, atomically dispersed uranium) to the daunting challenge associated with the low NH3 yield rate, thus enabling the scalable production of NH3 via electrochemical N-2 reduction.

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