Recovery of succinic acid for bio-based C4 bifunctional building block production
Başlık çevirisi mevcut değil.
- Tez No: 401562
- Danışmanlar: PROF. DR. L. A. M. VAN DER WIELEN, DR. A. J. J. STRAATHOF
- Tez Türü: Doktora
- Konular: Biyokimya, Biochemistry
- Anahtar Kelimeler: Belirtilmemiş.
- Yıl: 2011
- Dil: İngilizce
- Üniversite: Technische Universiteit Delft (Delft University of Technology)
- Enstitü: Yurtdışı Enstitü
- Ana Bilim Dalı: Belirtilmemiş.
- Bilim Dalı: Belirtilmemiş.
- Sayfa Sayısı: 136
Özet
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Özet (Çeviri)
The modern society greatly depends on petroleum derived chemicals and fuel to sustain its existence. Increasing world population and higher living standard accelerate the depletion of energy resources. Currently available resources are expected to last for another century. The rapid consumption of petroleum for fuel and for chemical industry also results in a larger carbon footprint on the ecosystem and a negative effect on climate and environment. To reduce these problems, alternative resources should be identified for fuel and chemical production. The energy need can be resolved with the use of clean energy resources like, solar, wind, tidal power or hydrogen fuel cells. If the raw material requirements of chemical industry shift from petroleum to alternative resources, the pressure on the energy markets would also be relieved to a certain extent. The production of organic chemicals requires carbon based raw materials. The best option for such a raw material is sugar which can be easily metabolized by microorganisms to other valuable chemicals. In this view, in recent decades, the researchers focused on industrial biotechnology to develop microorganisms by metabolic engineering techniques. These microorganisms can be modified to produce valuable chemicals, as their major fermentation products, by metabolizing different kinds of feedstock. There are number of candidate biochemicals to be used as raw material to meet the demand of chemical market. Among them are C4 carboxylic acids, which can be commercially very attractive. They can be chemically or biologically converted to various molecules and their carboxylic groups are suitable for polymer formation to generate materials with different physicochemical properties. This research project focuses on two candidate biochemicals, succinic acid and 4-hydroxybutyrate (4-HB), which have large potential in replacing petroleum derived counterparts. Succinic acid and 4-HB can be used as an intermediate for manufacture of plant growth stimulants, food ingredients, feed additives, green solvents, detergents and surfactants, health agents, corrosion inhibitors and as precursors for the production of gammabutyrolactone, 1,4-butanediol, tetrahydrofuran, 4-aminobutyrate, 4,4 Esters, polysuccinate esters and other carboxylic acids like maleic, fumaric, itaconic and aspartic acids.1,2 Succinic acid is chemically produced by chemical hydrogenation of malic acid and current capacities and sales prices are not in the range of bulk chemicals. The future succinic acid market is estimated to be in the range of 300,000 tons per year. The capacities of chemical/biochemical conversion products of succinic acid are estimated to exceed 1 million tons per year.2 To meet those capacities, the production of succinic acid should be optimized to increase efficiency and reduce costs. Traditionally, succinic acid fermentation has been performed at neutral pH, and high titers and yields have been achieved. However,maintaining neutral pH leads to the necessity to remove succinate counter ions from the fermentation medium, resulting in tedious and costly purification processes, which increase the costs of succinic acid. To overcome this, researchers have started utilizing metabolic engineering techniques to reduce the fermentation pH3 so that succinic acid will be present in its nondissociated form in the fermentation effluent, which is preferred for downstream operations. Anticipating such efforts, this research project focuses on the recovery of succinic acid from low pH fermentation medium and proposes utilization of adsorptive separation using hydrophobic zeolite adsorbents. Fermentative succinic acid is being advocated as a future source of renewable 1,4- butanediol. However, 4-HB, being more reduced than succinic acid, may be a better option, provided it can be obtained efficiently by fermentation. However, up to date there aren't any significant research attempts on fermentative production of 4-HB as final major product. Therefore, as a first step to metabolic engineering, the thermodynamic feasibility of production of 4-HB and its lactone via biochemical routes has been analyzed. In the first part of the study, the thermodynamic feasibility of four potential metabolic pathways from glucose to 4-HB was analyzed. The calculations revealed that when the pathways are NAD+ dependent the intermediate succinate semialdehyde (SSA) accumulates leading to low 4-HB yields at equilibrium. For NADP+ dependent pathways the calculated yield of 4- HB improves, up to almost 100%. In the second part, continuous removal of 4-HB from the solution is considered to shift SSA conversion into 4-HB so that SSA accumulation is minimized. One option is the enzymatic production of GBL from 4-HB. Candida antarctica Lipase B showed good lactonization rates at pH 4, but unfortunately this conversion cannot be performed in-vivo during 4-HB production because of the neutral intracellular pH. To be able to minimize the use of acid and base and to reduce solid waste generation during carboxylic acid production, a separation method that is selective towards neutral species should be identified. One of the physicochemical characteristics that distinguishes nondissociated organic acids from their ionic species is the charge density and resulting polarity due to charged functional groups. Therefore, the neutral species can be selectively recovered by making use of hydrophobic interactions. Hydrophobic zeolite particles are suitable candidates to achieve this separation. To check the validity of this claim, three 3 types of powder zeolites have been screened for succinic acid adsorption efficiencies. CVB-28014 (high-silica ZSM-5) showed higher equilibrium loadings (up to 0.16 g/g) than CBV-901, and CP811C-300, and was used for follow up studies. In the presence of Na+ counter ions, the succinic acid adsorption decreased in parallel with the succinic acid dissociation, but the adsorbent also showed some affinity towards sodium hydrogensuccinate with selectivities in the range 10-20 towards succinic acid. The presence of acetic acid resulted in lower succinic acid loadings, but the capacities remained sufficient for efficient recovery. The selectivity between succinic acid and acetic acid ranged from 1 to 6. Increasing the temperature to 70ºC reduced the equilibrium loadings, but in ethanol the succinic acid loadings showed a more significant drop.In adsorptive separation processes, regeneration of the adsorbent plays an important role. Depending on the type of product the regeneration strategy might differ from one process to another. To be able to claim that zeolites are suitable candidates for succinic acid purification, the recovery of succinic acid from the zeolites should also be feasible and easy. To test this, the desorption of succinic acid from a high silica ZSM-5 adsorbent was studied, using displacement by an organic solvent, CO2 or temperature swing. According to a number of process criteria and solvent selection criteria, 2-butanone performed better than the other studied displacing agents. However, the subsequent regeneration step involved desorption of butanone, which proved to be difficult and required a temperature above the normal boiling point of water under elevated pressure. Such a temperature swing with hot water can also be applied for direct succinic acid desorption without intermediate displacement by butanone. A countercurrent continuous adsorption process was modeled to compare these options. Direct temperature swing using pressurized water at >100 oC proved to be more attractive to achieve a sustainable process. This study focuses on development of an adsorption process for efficient separation of succinic acid from its salts in a low pH fermentation medium. High silica ZSM-5 zeolite particles (Si/Al2 » 220) were packed in laboratory columns. Solutions of succinic acid and acetic acid in water and Saccharomyces cerevisiae growth fermentation medium were fed to the fixed bed at different pH values. No or negligible adsorption of succinate salts was observed and they were eluted from the column with an early breakthrough. Experiments in the presence of acetic acid (1/4 of succinic acid mass concentration) showed slight drops in succinic acid capacity and almost 60% of acetic acid was eluted from the column in an early breakthrough. The adsorbed succinic acid was completely desorbed at 80 °C, resulting in lower concentrations in the eluent than in the feed. After three loading cycles, experiments with fermentation medium yielded lower capacities. However, the column regained its original capacity by calcining at 600 °C. To facilitate transition from small scale to large scale a good mathematical model is needed to lower the cost of pilot runs during optimization. The modeling of adsorption of dissociating species on fixed bed packed column involves increased computational load due to the equilibrium reactions. A simplified mathematical model has been constructed, which correctly described the breakthrough behavior. However, to be able to apply the model to different process conditions, the nonlinear mass transfer needs to be taken into account. Efficient large scale operation of this process requires special attention on the stability of the adsorbent particles under conditions of low pH and high temperatures. Finally an economical analysis has been performed. The proposed process begins with aerobic fermentation of a hypothetical Saccharomyces cerevisiae strain. After centrifugation the broth is sent to adsorption. A ZSM-5 zeolite is used to preferentially adsorb succinic acid. The flowthrough succinic acid salts are recycled to fermentor as pH control. Desorption is performed using hot water. This water is then flashed off, and the stream is sent to crystallization and drying. The plant capacity is set to 30,000 ton/year according to the projected demand. Cane sugar is the selected feedstock. The calculated market price of succinic acid is 2.26 $/kg with a large reduction margin based on the cost of fermentation unit. The total downstream contribution to the cost price of succinic acid was not larger than 40 ¢/kg. This thesis concludes that, in case an economical fermentation unit is developed, the proposed purification step can minimize chemicals usage and lower the production costs of succinic acid.
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