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We theoretically and experimentally show that, with water being adsorbed, the graphene oxide (GO) is converted to a spontaneously dynamic covalent material under ambient conditions, where the dominated epoxy and hydroxyl groups are mediated by water molecules to spontaneously break/reform their C–O bonds to achieve dynamic oxygen migration. This dynamic material presents structural adaptivity for response to biomolecule adsorption. Both density functional theory calculations and ab initio molecular dynamics simulations demonstrate that this spontaneously dynamic characteristics is attributed to the adsorption of water molecules, which sharply reduces the barriers of these oxygen migration reactions on GO to the level less than or comparable to the hydrogen bonding energy in liquid water. [ABSTRACT FROM AUTHOR]

[Display omitted] • The graphitic carbon nitride (g-C 3 N 4) shows unique geometrical characterizes to anchoring metal trimer clusters. • They have excellent catalytic performances for yielding NH 3 products with limiting potential of 0.02–0.50 V involving kinetic barrier of 0.03–0.46 eV. • The establish the relationship between surficial activities and electronic properties. As a cleaner and more energy-efficient alternative, the electrochemical reduction of N 2 to NH 3 under mild conditions has emerged as a promising avenue for environmental protection. However, developing catalysts with both high activity and selectivity has been a challenging task. The advent of atomically dispersed catalysts is revolutionizing the field of catalysis. Drawing inspiration from the successful fabrication of Ru trimer on graphitic carbon nitride (g-C 3 N 4) nanosheets, herein, we adopted a series of trimeric metal clusters anchored on g-C 3 N 4 monolayer (TM 3 @g-C 3 N 4 , TM = 3 d , 4 d and 5 d transition metal atom), as well as utilized the criteria range to describe the stability, activity, energy cost and selectivity of supported trimers for N 2 reduction reaction based on ab initio calculations combined with multi-level screening strategies. Finally, 5 candidate TM 3 @g-C 3 N 4 (TM = Rh, Ru, V, Mo, and Re) exhibits decent catalytic activity with limiting potential ranging of –0.50 – –0.02 V. These spatially confined triatomic metal centers demonstrated proficiency in activating N 2 molecules while exhibiting tunable surficial reactivity through modulation of the metal elements and interfacial electron coupling between trimers and underlying substrates. More importantly, a structure–activity relationship was established, which provides crucial insights for precise design of highly efficient atomically-precise catalysts at an atomic level for hydrogen fuel storage. [ABSTRACT FROM AUTHOR]