The energy sector in the developing world is expected to account for 27% of global emissions of greenhouse gases from fossil fuel combustion in 2035 – in 1990 it accounted for 7%. The increase is concentrated in rapidly growing countries in Asia that depend on coal for power generation. Maximizing electricity generation using renewable technologies in these countries provides an obvious approach to slowing global emissions growth. A barrier to increased use of renewable generation is cost: financial incentives could help to increase its use in developing countries. The principal objective of this research is to examine the practicability and potential scale of an offset scheme aimed at providing this incentive. Offset schemes have a poor reputation due to problems experienced with the Clean Development Mechanism (CDM). I identify the CDM’s failure to ensure the additionality of projects as a key issue and propose an approach to the assessment of additionality specific to grid connected generation projects. I present case studies of wind and small hydro projects in China and India in which I calculate the marginal abatement cost of emissions cuts and use the new approach to additionality to draw conclusions regarding the eligibility of projects to receive offsets in some hypothetical future scheme. My analysis shows that the proposed approach offers advantages over methodologies permitted by the CDM. I analyze the supply and demand for credits from existing schemes during 2013-2020 and show that oversupply will continue to impact their price, removing any incentive for investment in renewable generation. Using an original approach based on IEA forecasts for the energy sector, I estimate the maximum availability of offsets from a post-2020 scheme based on renewable generation, and assess the potential global demand. / text

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Membrane separation technology has recently emerged as a potential alternative technique for removing higher hydrocarbons (C₃₊) from natural gas. For economic reasons, membranes for this application should be organic vapor selective materials such as poly(dimethylsiloxane) (PDMS) or poly(1-trimethylsilyl-1-propyne) (PTMSP). These polymers, often called solubility selective polymers, sieve penetrant molecules based largely on relative penetrant solubility in the polymer. The sorption and transport properties in such polymers have been reported previously. However, most studies present only pure gas sorption and transport properties. Mixture properties, which are important for estimating membrane separation performance, are less often reported. In addition, mixed gas sorption and diffusion data in such polymers, to the best of our knowledge, have never been investigated before. This research work provides a fundamental database of mixture sorption, diffusion, and permeation data in solubility selective polymers. Two solubility selective polymers were studied: poly(dimethylsiloxane) (PDMS) and poly(1-trimethylsilyl-1-propyne) (PTMSP). The vapor/gas mixture was n-C4H10/CH4. CH4 partial pressures ranged from 1.1 to 16 atm, and [subscript n-]C₄H₁₀ partial pressures ranged from 0.02 to 1.7 atm. Temperatures studied ranged from -20 to 50 oC. The pure and mixed gas [subscript n-]C₄H₁₀ and CH₄ permeability and solubility coefficients in PDMS and PTMSP were determined experimentally using devices constructed specifically for these measurements. The pure and mixed gas diffusion coefficients were calculated from permeability and solubility data. In rubbery PDMS, the presence of [subscript n-]C₄H₁₀ increases CH₄ permeability, solubility, and diffusivity. On the other hand, the presence of CH₄ does not measurably influence [subscript n-]C₄H₁₀ sorption and transport properties. The [subscript n-]C₄H₁₀/CH₄ mixed gas permeability selectivities are lower than those estimated from pure gas measurements. This difference is due to both lower solubility and diffusivity selectivities in mixtures relative to those in pure gas. Plasticization of PDMS by [subscript n-]C₄H₁₀ does little to n-C4H10/CH₄ mixed gas diffusivity selectivity. Increases in mixed gas permeability selectivity with increasing [subscript n-]C₄H₁₀ activity and decreasing temperature were mainly due to increases in solubility selectivity. Unlike PDMS, the presence of [subscript n-]C₄H₁₀ decreases CH₄ permeability, solubility, and diffusivity in PTMSP. The competitive sorption and the blocking effects significantly reduce CH₄ solubility and diffusion coefficients in the polymer, respectively. However, similar to PDMS, the presence of CH₄ has no measurable influence on [subscript n-]C₄H₁₀ sorption and transport properties. [subscript n-]C₄H₁₀ /CH₄ mixed gas permeability selectivities in PTMSP are higher than those determined from the pure gas measurements. This deviation is a result of higher solubility and diffusivity selectivities in mixtures relative to the pure gas values. Mixed gas permeability, solubility, and diffusivity selectivities in PTMSP increased with increasing [subscript n-]C₄H₁₀ activity and decreasing temperature. The partial molar volumes of [subscript n-]C₄H₁₀ and CH₄ in the polymers were determined from sorption and dilation data. The dilation isotherms of PDMS and PTMSP in mixtures agree with estimates based on pure gas sorption and dilation measurements. The partial molar volumes of n-C4H10 and CH4 in PDMS are similar to those in liquids. In contrast, the partial molar volumes of [subscript n-]C₄H₁₀ and CH₄ in glassy PTMSP are substantially lower than those in liquids. Several models were used to fit the experimental data. For instance, the FFV model, the activated diffusion model, and the Maxwell-Stefan model were employed to describe the mixture permeability data in PDMS. Based on the Maxwell-Stefan analysis, the influence of coupling effects on permeation properties in PDMS were negligible. The dual mode sorption and permeation models were used to describe the mixed gas data in PTMSP. The dual mode permeability model must be modified to account for [subscript n-]C₄H₁₀ -induced reductions in CH₄ diffusion coefficients (i.e., the blocking effect). The FFV model provides poor correlations in PTMSP. There seems to be other factors, besides FFV per se, contributing to the temperature and concentration dependence of diffusion coefficients in PTMSP.

The noble gas abundances and isotopic ratios of the terrestrial planets differ from each other and from the average of chondritic meteorites. These different abundance patterns result from primordial heterogeneities or different degassing histories. Magmatic transport is the only degassing mechanism that can be demonstrated to occur on Venus, Earth, and Mars, and is presently the dominant form of volatile transport to a planet's free surface. An alternative technique was developed to determine the partitioning and solubility of noble gases in mineral/melt systems. Natural end member minerals and synthetic melts known to be in equilibrium were held in separate crucibles in a one bar flowing noble gas atmosphere. Experiments were run 7-18 days at 1300 or 1332°C, in 99.95% Ar or a Ne-Ar-Kr-Xe mix. Gas concentrations were measured by mass spectrometry. The solubility of noble gases in minerals was surprisingly high, and individual samples of a particular mineral composition are distinct in their behavior. The data is consistent with lattice vacancy defect siting. Noble gas solubility in the minerals increases with increasing atomic number; this may be related to polarizability. Noble gas solubilities in melts decrease with increasing atomic number. Solubility is directly proportional to melt molar volume; values overlap the lower end of the range defined for natural basalts. The lower solubilities are related to the higher MgO and CaO concentrations and lower degree of polymerization and Fe³⁺ concentration in synthetic vs. natural melts. Partition coefficient patterns show a clear trend of increasing compatibility with increasing noble gas atomic number, but many individual values are > 1. Calculations show that the terrestrial planet atmospheres cannot have formed from partial melting of a common chondritic source. When results are examined with isotopic constraints and MOR and hot-spot activities, there is no compelling evidence that the Earth is substantially outgassed of its primordial or even its radiogenic volatiles. If volcanic degassing was mostly responsible for the atmospheres, then initial volatile abundances were Mars < Earth < Venus. Alternatively, roughly equal abundances could have been modified by catastrophic processes.

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published_or_final_version / abstract / toc / Physics / Master / Master of Philosophy

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