METAL NANOMATERIALS: SYNTHESIS, DESIGN, AND APPLICATIONS

As an important part of the periodic table, metal elements have attracted widespread attention due to their special physical and chemical properties, as well as effective functionalities. Many metals at the nanoscale level exhibit a wide array of applications, ranging from catalysis to photonics, electronics, energy conversion/storage, and medicine. To obtain a more effective functionality in application, it is indispensable to synthesize uniform metal nanoparticles with well-defined size, morphology, composition, and crystal structures. In this dissertation, we will demonstrate high-boiling point solvent method for synthesizing metal nanocrystals, ranging from single metal nanocrystals (e.g., iridium (Ir), ruthenium (Ru), germanium (Ge), bismuth (Bi)) to binary metal nanocrystals (e.g., Sn-Ge), and ternary intermetallic compounds (e.g., Pt_1-xPd_xBi). By varying different halogen ions, we can get different morphologies of metal nanocrystals. We will further study the catalytic effect of Pd metal nanocrystals supported on silicon spheres and realize the hydrodeoxygenation reaction of vanillin under mild conditions.
First, we used bismuth as an example to study the shape-controlled synthesis of metal nanocrystals by adjusting the injection temperature and the added halide ions (e.g., Cl^-, Br^-). Our findings indicated that due to the different electronegativities, halide ions are selectively adsorbed on specific crystal planes during the growth of Bi NCs, leading to different morphologies. Then we proposed a tungsten hexacarbonyl (W(CO)₆)-assisted reduction strategy for obtaining uniform metal nanoparticles (e.g., Ir, Ru, Ge, Bi) of different metal salts. This strategy was extended to the synthesis of uniform binary metal (e.g., Sn-Ge) nanoparticles, which we can get tunable bandgap (0.51 eV to 0.72 eV) based on the controlled reaction of Ge²⁺ precursor solution with uniform tin (Sn) nanocrystals (NCs) as the template. Next, we realized the synthesis of intermetallic Pt_1-xPd_xBi nanoplates with controllable compositions, including Pt_0.5Pb_0.5Bi, Pt_0.25Pd_0.75Bi, and Pt_0.75Pd_0.25Bi via the sequential complexation-reduction-sorting method. Furthermore, we used palladium (Pd) metal nanoparticles (NPs) as a photocatalyst to trigger the hydrodeoxygenation reaction of vanillin. We demonstrated a model to disperse free-standing Pd NP on dielectric silica nanospheres (SiO_x NSs). The spherical shape of SiO_x can cause scattering resonance, thereby enhancing the local electric field on or near the surface to enhance light absorption of Pd NPs, further realizing a more effective catalyze on chemical reactions. We found that the adsorption of H₂ on Pd is too strong to support the reaction effectively, but light absorption can reduce the "poisoning effect" by weakening the adsorption of hydrogen on Pd surface. Overall, we use innovative strategies to effectively synthesize a variety of high-quality metal nanomaterials. Our work shows that the Pd-NP/SiO_x-NS composite nanostructure using dielectric SiO_x as an optical nanoantenna is a promising photocatalyst that can drive photonic chemical conversion with high efficiency.

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