No abstract

We present a new flame-based aerosol reactor configuration that combines thermal decomposition and hydrogen reduction to produce metal nanoparticles. This approach uses a fuel-rich hydrogen flame as a source of low-cost energy to initiate particle synthesis, but separates the flame chemistry from the particle formation chemistry. Hot combustion products pass through a nozzle to produce a high-temperature reducing jet. A liquid precursor solution is rapidly atomized, evaporated, and decomposed by the expanding jet, initiating particle formation. In particular, here we have produced carbon-coated copper nanoparticles from an aqueous copper formate precursor solution and characterized them by aerosol mobility distribution measurements, electron microscopy, and x-ray diffraction. Copper serves here as a prototype for nonoxide materials that are generally difficult to produce in flamebased reactors. This work demonstrates that such materials can be produced in substantial quantities with particle diameters below 50 nm in this new process.

We report the continuous one-step synthesis of bimetallic copper-nickel nanostructured coatings by deposition and sintering of metal nanoparticles produced as an aerosol using a flame driven high temperature reducing jet (HTRJ) process. The HTRJ process allows gas-phase (aerosol) formation of metal nanoparticles from low-cost metal salt precursors. These can be collected as discrete powders for subsequent use in formulating conductive inks or for other applications. However, direct deposition of nanoparticles to form coatings allows measurements of electrical conductivity of films of deposited nanoparticles as a function of composition and sintering temperature, without actually formulating and printing inks. This is the approach taken here for the purpose of screening nanoparticle compositions quickly. We characterized the microstructure and composition of both nanopowders and films and found that their composition consistently matched the ratio of metals in the precursor solution. The electrical conductivity was highest (∼10(4) S/m) for films with 60:40 and 40:60 copper-to-nickel mass ratios. These films maintained their conductivity during extended storage (1 month) under ambient conditions. The oxidation resistance and high conductivity observed here suggest that 60:40 and 40:60 Cu:Ni nanoparticles have promise as lower cost replacements for silver nanoparticles in conductive ink formulations.

We report production of bimetallic nanostructured coppersilver coatings by in situ deposition and sintering of metal nanoparticles produced as an aerosol. The metal nanoparticles themselves have potential applications in printed electronics, catalysis, antibacterial coatings, and heat transfer fluids. In many applications, nanoparticles are dispersed in an ink, which is then printed or coated onto a substrate and converted into a nanostructured thin film. Direct deposition from the aerosol allows us to produce nanostructured thin films without first dispersing the particles in a solvent. The high temperature reducing jet process allows formation of these metal nanoparticles from low-cost metal salt precursors in the gas phase. In this method, a fuel-rich hydrogen flame provides a low-cost source of energy to drive nanoparticle formation in a reducing environment. The aqueous precursor solution is delivered into the hot combustion product gases within a converging-diverging nozzle. The high-speed gas flow atomizes the precursor and provides exceptionally rapid mixing of the precursor with the hot gases. Here, particles are formed, then immediately quenched and deposited on a glass substrate. The effect of the silver content of the mixed copper-silver films on their electrical conductivity was studied systematically, revealing an abrupt transition from low conductivity to high conductivity between 30 wt.% and 40 wt.% silver.

A new high-pressure catalytic partial oxidation reactor was developed for high-pressure production of synthesis gas from natural gas and pure oxygen, and the integration of the new reactor with the gas to liquids process was investigated. The experimental work was performed at Praxair's laboratory, process design and economic estimates were performed by Foster Wheeler, and theoretical simulations were preformed by University of Delaware. The reactor system was based on a millisecond contact time mixer capable of delivering a fueloxygen mixture to the catalyst without onset of homogeneous reactions. Significant differences were observed between high-and low-pressure operation. With proper mixer and catalyst bed design the system was able to operate stably at pressures up to 18 bar with performance comparable to low-pressure operation. Process economic analysis predicted a small economic advantage for a catalytic partial oxidation reactor compared to conventional technology.