Kinetic Study on the Self-Assembly of Au(I)-Thiolate Lamellar Sheets: Preassembled Precursor vs Molecular Precursor

Molecular self-assembly has played an important role in nanofabrication. Due to the weak driving forces of noncovalent bonds, developing molecular nanoassemblies that have both robust preparation conditions and stable structure is a challenge. In our previous work, we have developed a reversible self-assembly system of Au(I)-thiolate coordination polymer (ATCP) to form colloidal lamellar sheets and demonstrated the high tailorability and stability of their structures, as well as their promising applications in gold nanocluster/nanoparticle fabrication and UV light shielding. Here, we first reported our progress in exploring a robust and green assembly protocol toward ATCP colloidal lamellar sheets in water by allowing the molecular precursors of HAuCl₄ and the thiol ligand to form ATCP preassembled intermediates. In this way, colloidal ATCP lamellar sheets can be prepared in a wide range of synthetic concentrations ([Au]₀ ≥ 2 × 10^-4 M) and at broad assembly temperatures (80-100 °C) with similar high yields (>80%). The assembly kinetics at different conditions are also studied in detail to help understand the robust assembly process. The robust and green synthetic protocols will pave a way for their real applications.