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HighlightsThe Bi 2 O 3  nanoplates homogeneously decorated free-standing exfoliated graphene (Bi 2 O 3 /FEG) was prepared by a facile electrochemical deposition method.    The Bi 2 O 3 /FEG first used as nitrogen reduction electrocatalyst exhibits excellent electrocatalysis performance and stability for nitrogen reduction reaction in neutral media.    The superior electrocatalytic nitrogen reduction activity is attributed to the strong interaction of the Bi 6 p  band with the N 2 p  orbitals, binder-free nature of the electrodes, and facile electron transfer through the graphene nanosheets.Electronic supplementary material  The online version of this article (10.1007/s40820-020-00444-y) contains supplementary material, which is available to authorized users.

Bismuth-Based Free-Standing Electrodes for Ambient-Condition Ammonia Production in Neutral Media