Fabrication of a two-dimensional covalent network of honeycomb nanosheets comprising small 1,3,5-triamino benzene and benzene-1,3,5-tricarboxaldehyde aromatic building blocks was conducted on Au(111) in a pH-controlled aqueous solution. In situ scanning tunneling microscopy revealed a large defect-free and homogeneous honeycomb π-conjugated nanosheet at the Au(111)/liquid interface. An electrochemical potential dependence indicated that the nanosheets were the result of thermodynamic self-assembly based not only on the reaction equilibrium but also on the adsorption (partition) equilibrium, which was controlled by the building block surface coverage as a function of electrode potential.
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