Deyu Liu

Epitaxial Growth of Heterogeneous Metal Nanocrystals: From Gold Nano-octahedra to Palladium and Silver Nanocubes

With octahedral Au nanocrystals as seeds, highly monodisperse Au@Pd and Au@Ag core-shell nanocubes were synthesized by a two-step seed-mediated method in aqueous solution. Accordingly, we have preliminarily proposed a general rule that the atomic radius, bond dissociation energy, and electronegativity of the core and shell metals play key roles in determining the conformal epitaxial layered growth mode.

Facet-Selective Epitaxial Growth of Heterogeneous Nanostructures of Semiconductor and Metal: ZnO Nanorods on Ag Nanocrystals

We demonstrate a new approach for synthesizing Ag-ZnO heterogeneous nanostructures in which single-crystalline ZnO nanorods were selectively grown on {111} rather than {100} facets of single-crystalline Ag truncated nanocubes. We have identified the fine structure of the Ag-ZnO heterostructures and proposed a mechanism indicating that structure match plays a critically important role in this type of facet-selective growth. These heterogeneous nanostructures are of special interest and have potential applications in electrical contacts, functional devices, biological sensors, and catalysis.

Supersaturation-Dependent Surface Structure Evolution: From Ionic, Molecular to Metallic Micro/Nanocrystals

Deduced from thermodynamics and the Thomson-Gibbs equation that the surface energy of crystal face is in proportion to the supersaturation of crystal growth units during the crystal growth, we propose that the exposed crystal faces can be simply tuned by controlling the supersaturation, and higher supersaturation will result in the formation of crystallites with higher surface-energy faces. We have successfully applied it for the growth of ionic (NaCl), molecular (TBPe), and metallic (Au, Pd) micro/nanocrystals with high-surface-energy faces. The above proposed strategy can be rationally designed to synthesize micro/nanocrystals with specific crystal faces and functionality toward specific applications.

Silver-Based Intermetallic Heterostructures in Sb2Te3 Thick Films with Enhanced Thermoelectric Power Factors

In this work, Ag(x)Te(y)-Sb(2)Te(3) heterostructured films are prepared by ligand exchange using hydrazine soluble metal chalcogenide. Because of the created interfacial barrier, cold carriers are more strongly scattered than hot ones and thereby an over 50% enhanced thermoelectric power factor (~2 μW/(cm·K(2))) is obtained at 150 °C. This shows the possibility of engineering multiphases to further improve thermoelectric performance beyond phonon scattering through a low-temperature solution processed route.

Inkjet Printing Assisted Synthesis of Multicomponent Mesoporous Metal Oxides for Ultrafast Catalyst Exploration

We describe an inkjet printing assisted cooperative-assembly method for high-throughput generation of catalyst libraries (multicomponent mesoporous metal oxides) at a rate of 1,000,000-formulations/hour with up to eight-component compositions. The compositions and mesostructures of the libraries can be well-controlled and continuously varied. Fast identification of an inexpensive and efficient quaternary catalyst for photocatalytic hydrogen evolution is achieved via a multidimensional group testing strategy to reduce the number of performance validation experiments (25,000-fold reduction over an exhaustive one-by-one search).

A Mesoporous Anisotropic n‐Type Bi2Te3 Monolith with Low Thermal Conductivity as an Efficient Thermoelectric Material

A mesoporous Bi_2Te_3 monolith with ≈20% porosity is fabricated by hot-pressing mesoporous powders. The mesostructures are able to transport carriers and scatter phonons efficiently. The reduction (≈60%) of the thermal conductivity is sufficient to compensate for the loss of electrical conductivity perpendicular to the direction of applied pressure, leading to an enhanced zT of 0.7, highest among all reported self-doped, n-type Bi_2Te_3 at similar temperatures.

Panchromatic Photoproduction of H2 with Surface Plasmons

The optical resonances of plasmonic nanostructures depend critically on the geometrical details of the absorber. We show that this unique property of plasmons can potentially be used to create panchromatic absorbers covering most of the useful solar spectrum, by measuring the light-to-hydrogen conversion capabilities of a series multielectrode photocatalytic devices, based on functionalized gold nanorods of appropriately chosen aspect ratios. Judiciously combining nanorods of various aspect ratios almost doubles the H2 production of the device over what is optimally possible with a device using gold nanorods of a single aspect ratio (all other key parameters being equal). The estimated quantum efficiency (absorbed photons-to-hydrogen) averaged over the entire solar spectrum of the best performing plasmonic multielectrode array was approximately 0.1%, and the measured H2 production rate for all of the devices was found to be approximately proportional to the hot electron generation. The device was monitored continuously for over 200 hr of operation without measurable diminution in the rate.

Hot carrier filtering in solution processed heterostructures: a paradigm for improving thermoelectric efficiency.

An approach based on a solution-based synthesis that produces a thermally stable Ag/oxide/S₂ Te₃ -Te metal-semiconductor heterostructure is described. With this approach, a figure of merit of zT = 1.0 at 460 K is achieved, a record for a heterostructured material made using wet chemistry. Combining experiments and theory shows that the large increase in the materials Seebeck coefficient results from hot carrier filtering.

Uniform gold spherical particles for single-particle surface-enhanced Raman spectroscopy

Surface-enhanced Raman spectroscopy (SERS) benefits from the enhanced electromagnetic field of the localized surface plasmon resonance effect of metallic (especially coinage metals) nanoparticles or nanostructures. The detection sensitivity and reproducibility of SERS measurement appear to be the two critical issues in SERS. To solve the problem associated with traditional nanoparticle aggregates and SERS substrates, we propose in this work single particle SERS. We prepared uniform gold microspheres with controllable size and surface roughness using an etching-assisted seed-mediated method. Single particle dark-field spectroscopy and SERS measurements show that particles with a larger roughness give a stronger SERS signal, but still retain a good reproducibility. This study points to the promising future of the practical application of the single particle SERS technique for trace analysis.

Microwave synthesis of microstructured and nanostructured metal chalcogenides from elemental precursors in phosphonium ionic liquids.

We describe a general approach for the synthesis of micro-/nanostructured metal chalcogenides from elemental precursors. The excellent solubility of sulfur, selenium, and tellurium in phosphonium ionic liquids promotes fast reactions between chalcogens and various metal powders upon microwave heating, giving crystalline products. This approach is green, universal, and scalable.