Catalytic Regulation of Cluster-Mediated Growth Enables Scalable Synthesis of Shape-Controlled Single-Crystalline Silver Nanocrystals

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Abstract Precisely controlling shape and crystallinity is central to defining structure-dependent properties in colloidal nanocrystals (NCs), which is particularly important yet challenging for silver (Ag) NCs. Here, we report catalytic regulation that facilitates cluster-mediated growth pathways to enable the scalable synthesis of single-crystalline Ag-NCs with programmable shapes. A copper (Cu)-assisted, one-pot heating-up process produces highly uniform Ag-NCs with tunable diameters (5–11 nm) and morphologies ranging from truncated-octahedral (“mecon”) to spherical geometries, while maintaining gram-scale batch output, air tolerance, and compatibility with continuous flow synthesis. Spectroscopic and mass spectrometric analyses reveal a stepwise growth pathway involving discrete Ag cluster intermediates, whose formation and interconversion are accelerated by trace Cu species acting as catalysts. Density functional theory calculations further show that Cu modulates surface and stacking-fault energetics, promoting single-crystalline growth with well-defined facets. By introducing a quantitative shape descriptor, we establish predictive relationships linking NC morphology to plasmonic response, supported by discrete dipole approximation simulations. These results define a general synthetic principle in which catalytic species and dynamic ligand environments cooperatively govern cluster-phase evolution, enabling precise and scalable control of NC structure and function.

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