▎ 摘　　要

In this research, we report an innovative, chemical strategy for the in situ synthesis and direct two-dimensional (2D) arraying of various nanoparticles (NPs) on graphenes using both programmed-peptides as directing agents and graphenes as pre-formed 2D templates. The peptides were designed for manipulating the enthalpic (coupled interactions) constraint of the global system. Along with the functionalization of graphene for the stable dispersion, peptides directed the growth and array of NPs in a controllable manner. In particular, the sequences of peptides were encoded by the combination of glutamic acid (E), glycine (G), and phenylalanine (F) amino acids as follows: (E-G-F)(3)-G, with E for the interaction with NPs and F and G for the interaction with graphenes. For the entropic (restricted geometry) constraint, graphene was used as a 2D scaffold to tune the size, density, and position of NPs, while maintaining the intrinsic properties for electrochemical applications. The excellent quality of the resultant hybrids was demonstrated by their high electrocatalytic activity in the electrooxidation of methanol. This synergistic combination of peptides and graphenes allowed for a uniform 2D array and spontaneous organization of various NPs (i.e., Pt, Au, Pd, and Ru), which would greatly expand the utility and versatility of this approach for the synthesis and array of the advanced nanomaterials.