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- All Subjects: chemical engineering
- All Subjects: Positron Annihilation Lifetime Spectroscopy
- Creators: Bliss, Lyle Brewster
- Member of: Barrett, The Honors College Thesis/Creative Project Collection
Description
Layered double hydroxides (LDHs), also known as hydrotalcite-like materials, are extensively used as precursors for the preparation of (photo-)catalysts, electrodes, magnetic materials, sorbents, etc. The synthesis typically involves the transformation to the corresponding mixed metal oxide via calcination, resulting in atomically dispersed mixed metal oxides (MMOs). This process alters the porosity of the materials, with crucial implications for the performance in many applications. Yet, the mechanisms of pore formation and collapse are poorly understood. Combining an integrated in situ and ex situ characterization approach, here we follow the evolution of porosity changes during the thermal decomposition of LDHs integrating different divalent (Mg, Ni) and trivalent (Al, Ga) metals. Variations in porous properties determined by high-resolution argon sorption are linked to the morphological and compositional changes in the samples by in situ transmission electron microscopy coupled with energy dispersive X-ray spectroscopy, which is facilitated by the synthesis of well crystallized LDHs of large crystal size. The observations are correlated with the phase changes identified by X-ray diffraction, the mass losses evidenced by thermogravimetric analysis, the structural changes determined by infrared and nuclear magnetic resonance spectroscopy, and the pore connectivity analyzed by positron annihilation spectroscopy. The findings show that the multimetallic nature of the LDH governs the size and distribution (geometry, location, and connectivity) of the mesopores developed, which is controlled by the crystallization of the MMO phase, providing key insights for the improved design of porous mixed metal oxides.
ContributorsMurty, Rohan Aditya (Author) / Deng, Shuguang (Thesis director) / Nielsen, David R. (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2017-05
Description
As global population and demand for electrical power increase, humanity is faced with the growing challenge of harnessing and distributing enough energy to sustain the developing world. Currently, fossil fuels (coal
atural gas) are our main sources of electricity. However, their cost is increasing, they are nonrenewable, and they are very harmful to the environment. Thus, capacity expansion in the renewable energy sector must be realized to offset higher energy demand and reduce dependence on fossil fuels. Solar energy represents a practical solution, as installed global solar capacity has been increasing exponentially over the past 2 decades. However, even with government incentives, solar energy price ($/kWh) continues to be highly dependent on political climate and raw material (silicon and silver) cost. To realistically and cost effectively meet the projected expansions within the solar industry, silver must be replaced with less costly and more abundant metals (such as copper) in the front-grid metallization process of photovoltaic cells. Copper, while offering both higher achievable efficiencies and a raw material cost nearly 100 times cheaper than silver, has inherent disadvantages. Specifically, copper diffuses rapidly into the silicon substrate, requires more complex and error-prone processing steps, and tends to have less adhesive strength, reducing panel robustness. In this study, nickel deposition via sputtering was analyzed, as well as overall potential of nickel as a seed layer for copper plating, which also provides a barrier layer to copper diffusion in silicon. Thermally-formed nickel silicide also reduces contact resistivity, increasing cell efficiency. It was found that at 400 \u00B0C, ideal nickel silicide formation occurred. By computer modeling, contact resistivity was found to have a significant impact on cell efficiency (up to 1.8%). Finally, sputtering proved useful to analyze nickel silicide formation, but costs and time requirements prevent it from being a practical industrial-scale metallization method.
atural gas) are our main sources of electricity. However, their cost is increasing, they are nonrenewable, and they are very harmful to the environment. Thus, capacity expansion in the renewable energy sector must be realized to offset higher energy demand and reduce dependence on fossil fuels. Solar energy represents a practical solution, as installed global solar capacity has been increasing exponentially over the past 2 decades. However, even with government incentives, solar energy price ($/kWh) continues to be highly dependent on political climate and raw material (silicon and silver) cost. To realistically and cost effectively meet the projected expansions within the solar industry, silver must be replaced with less costly and more abundant metals (such as copper) in the front-grid metallization process of photovoltaic cells. Copper, while offering both higher achievable efficiencies and a raw material cost nearly 100 times cheaper than silver, has inherent disadvantages. Specifically, copper diffuses rapidly into the silicon substrate, requires more complex and error-prone processing steps, and tends to have less adhesive strength, reducing panel robustness. In this study, nickel deposition via sputtering was analyzed, as well as overall potential of nickel as a seed layer for copper plating, which also provides a barrier layer to copper diffusion in silicon. Thermally-formed nickel silicide also reduces contact resistivity, increasing cell efficiency. It was found that at 400 \u00B0C, ideal nickel silicide formation occurred. By computer modeling, contact resistivity was found to have a significant impact on cell efficiency (up to 1.8%). Finally, sputtering proved useful to analyze nickel silicide formation, but costs and time requirements prevent it from being a practical industrial-scale metallization method.
ContributorsBliss, Lyle Brewster (Author) / Bowden, Stuart (Thesis director) / Karas, Joseph (Committee member) / Chemical Engineering Program (Contributor) / Barrett, The Honors College (Contributor)
Created2017-05