Unveiling the competitive behavior by the orientated regulation of S-vacancy over MoS2 for highly effective N2 fixation

摘要

The electrochemical N-2 reduction reaction (NRR) renders great potential for sustainable ammonia generation but still suffers from serious challenges, which limit the effective enhancement of catalytic performances. Herein, we skillfully utilize the asynchronous NRR and hydrogen evolution reaction (HER) activities as a function of S-vacancy (V-s) concentrations to enhance the NRR activity but sacrifice the HER activity, thus achieving the tradeoff between activity and selectivity towards the NRR. Inspired by the theoretical guidance, the optimized catalyst (FL-MoS2-20) with a suitable Vs concentration (16.30 %) renders a high NH3 yield rate of 92.95 +/- 2.10 mu g h(-1) mg(-1) and a Faradic efficiency (FE) of 20.80 +/- 0.18 %, exceeding virtually all previously published MoS2-based NRR catalysts and the overwhelming majority of state-of-the-art NRR catalysts. This work broadens the potential of vacancy engineering to manage the competitive reaction on a single active site and enlightens the catalyst design in the NRR field and beyond.

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