N2 electroreduction reaction (NRR) enables an eco‐friendly NH3 synthesis under mild conditions, which is regarded as a carbon‐neutral alternative technology to the traditional Haber–Bosch process. However, its practical applications are seriously impeded by the difficulty in N2 adsorption and activation over catalysts, as well as the competing hydrogen evolution reaction (HER). In this work, a novel bismuth molybdate nanocatalyst with sufficient oxygen vacancies and high Biconcentration (41.9 at%), BiMoO‐OVs, is synthesized and demonstrated as an excellent NRR electrocatalyst. Benefiting from synergistic effect of the adequate Bi active centers with inert HER activity provided by the high concentration of Bi, and the reinforced N2 adsorption and activation ability of oxygen vacancies, the as‐synthesized BiMoO‐OVs presents a high Faradaic efficiency of 16.38% with a NH3 yield rate of 3.65 µg h−1 cm−2 at −0.4 V (vs RHE) in neutral electrolyte, which outperforms those of most Bi‐based NRR nanocatalysts. Noticeably, it also presents excellent electrochemical durability for at least 24 h. The present work provides a simple and effective strategy for designing low‐cost and high‐performance Bi‐based catalysts.
Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is still seriously impeded by the inferior NH 3 yield and low Faradaic efficiency, especially at low overpotentials. Herein, we report the synthesis of nanosized RuO 2 and Bi 2 O 3 particles grown on functionalized exfoliated graphene (FEG) through in situ electrodeposition, denoted as RuO 2 À Bi 2 O 3 /FEG. The prepared self-supporting RuO 2 À Bi 2 O 3 /FEG hybrid with a Bi mass loading of 0.70 wt% and Ru mass loading of 0.04 wt% shows excellent NRR performance at low overpotentials in acidic, neutral and alkaline electrolytes. It achieves a large NH 3 yield of 4.58 � 0.16 μg NH3 h À 1 cm À 2 with a high Faradaic efficiency of 14.6 % at À 0.2 V versus reversible hydrogen electrode in 0.1 M Na 2 SO 4 electrolyte. This performance benefits from the synergistic effect between Bi 2 O 3 and RuO 2 which respectively have a fairly strong interaction of Bi 6p orbitals with the N 2p band and abundant supply of *H, as well as the binder-free characteristic and the convenient electron transfer via graphene nanosheets. This work highlights a new electrocatalyst design strategy that combines transition and maingroup metal elements, which may provide some inspirations for designing low-cost and high-performance NRR electrocatalysts in the future.
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