DETERMINATION OF OPTIMAL CONDITIONS FOR BIODIESEL PRODUCTION FROM JANSA SEED OIL USING LITHIUM DOPED CATALYSTS

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ABSTRACT

This study presents an empirical analysis of biodiesel production from Jansa seed oil using tranesterification process. Following the quest to achieve improved economic viability and clean production process for biodiesel, lithium ion from lithium carbonate was applied to improve the catalytic properties of calcium oxide and magnesium oxide for biodiesel production. Oil produced from jansa seed was characterized to determine its suitability for biodiesel production. Based on the characterization, an appreciable oil weight or yield of 38.09% was produced. Also, 0.493mgKOH/kg free fatty acid (FFA) content, 205.923 gKOH/kg saponification value and 99.95% ester value which specified its great tendency to be converted into methyl ester (biodiesel) were obtained. Li-CaO and Li-MgO catalysts were prepared in diverse concentrations for use in biodiesel production. Li-CaO-1.50 and Li-MgO-1.50 gave the optimal yield of 76 and 83% volume of biodiesel. These were applied to study the effects of other process parameters (reaction time, reaction temperature, agitation speed, and methanol to oil molal ratio) and optimized using a matrix design.  Li-CaO-1.50 gave the optimal yield at other process conditions. A two level, five experimental design matrix was used for transesterification studies for 32 experimental runs using Li-CaO as catalyst. Set of conditions that gave the optimal yield were; catalyst concentration of 1.5 % weight, reaction time of 3 hours, temperature of 600C, methanol and oil molal ratio of 12:1 and agitation speed of 500 rpm respectively. All possible interactions, predicted and actual values, final equation in terms of coded factors and interaction plots were identified. Biodiesel blends from optimal yield of the metallic oxides of the catalysts were formulated and characterized to further determine the physicochemical properties (calorific value, anisidine point, API gravity, diesel index, flash and fire points, cloud and pour points) which were within the ASTM D6751 standard recommendations for use in compression ignition engines. Scanning electron microscopy (SEM) was used to study the active sites of the surface structure of the catalyst in relation to various modifications. The sample indicated increased points of higher porosity as lithium concentration increased (1.5, 2.0 and 2.5%) and less porosity at 0.5 and 1.0% concentration. Gas chromatography (GC) and Fourier transform infrared spectrometry (FTIR) of the jansa seed oil and biodiesel produced were carried out. A total of 7 compounds were identified in the oil of which 4 were FFAs and other 3 were biodiesel esters. For the biodiesel, a total of 12 compounds were identified, of which 9 were methyl esters and 3 non esters, thus, producing 88.35% methyl ester concentration at optimal yield sample. Evidently, the same functional groups identified in the jansa seed oil were present in the optimal biodiesel yield sample which includes; the hydrocarbon group (as a basic characteristics of bio-oil),a halide group and an ester group (as the basic characteristics of biodiesel). Overall, the optimal products developed were found to meet standard properties for biodiesel through free fatty acid methyl ester (FAME) profile test and functional group validation. At such, Li-CaO, Li-MgO, other similar materials should be adopted as catalyst for the production of biodiesel to bridge the energy gaps. 







TABLE OF CONTENTS

Cover Page                                                                                  i
Title Page                      ii
Declaration         ii
Dedication         iv
Certification         v
Acknowledgements         vi
Table of Contents        vii
List of Tables                                 xi
List of Figures                                xii
Abstract                    xv

CHAPTER 1: INTRODUCTION
1.1 Background of the Study                       1
1.2 Statement of  Problem                               2 
1.3 Aim and Objectives of Study                                            3
1.4 Scope of Study                                                        3
1.5 Justification of Study                             4

CHAPTER 2: LITERATURE REVIEW
2.1 Catalysts and Compositional Properties       5
2.2 Basic Solid Catalysts             5
2.2.1 MgO as Base Heterogeneous Catalyst       6
2.2.2 CaO as a Base Heterogeneous Catalyst            7
2.2.3 SrO as a Base Heterogeneous Catalyst                       8
2.2.4 Biodiesel Production with Mixed Metal Oxide and Derivatives  8
2.2.5    Biodiesel Production with Transition Metal Oxide and Derivatives               9
2.2.6 Waste Material-Base Heterogeneous Catalysts   11
2.3 Acidic Solid Catalysts         12
2.3.1 Acid-Base Solid Catalysts         13
2.4 Adoption of the Catalysts for the Study                             15
 2.5      Summary of Literature          17  
CHAPTER 3: MATERIALS AND METHODS
3.1 Materials         19
3.1.1 Glass Wares and other Consumables  19
3.1.2 Analytical Grade Reagents         19
3.1.3 Electronic Equipment                      19
3.2 Methods   19
3.2.1 Sample Collection and Preparation   19
3.2.2 Oil Extraction (Soxhlet Method)     20
3.2.3 Oil Characterization         21
3.2.4 Catalyst Preparation         26
3.2.5 Effects of Process Parameters on the Biodiesel Production    26
3.3 Design of Experiment for Biodiesel Production      28
3.3.1 Fractional Factorial Design of Experiment for Biodiesel Production               28
3.4    Biodiesel Blends Preparation and Characterization  31
3.5    Gas Chromatography – Mass Spectrometry (GC-MS) Analysis of the Raw Oil and the Biodiesel         33
3.6       Fourier Transform Infra-Red Spectrometry (FTIR) of Raw Oil and Biodiesel         33
3.7 Scanning Electron Microscopy (SEM) of the Catalysts                     34

CHAPTER 4: RESULTS AND DISCUSSION
4.1       Characterization Test Result of the Jansa seed Bio-Oil   35
4.2 Gas Chromatography Mass Spectrometry (GC-MS) Analysis 
Test Results of the Jansa Seed Oil                                      36
4.3    Scanning Electronic Microscopy (SEM) of the Lithium-Ions-Doped Metallic Oxides Catalysts for Biodiesel Production    39
4.4       Effects of the Process Parameters on the Biodiesel Production Yield using the Lithium-Doped CaO and MgO Catalysts Variants          42
4.4.1    Effect of Catalyst Concentration Variation on the Biodiesel Yield         43
4.4.2    Effect of Reaction Time Variation on the Biodiesel Yield    44
4.4.3    Effect of Reaction Temperature Variation on the Biodiesel Yield         44
4.4.4    Effect of Agitation Speed Variation on the Biodiesel Yield     45
4.4.5    Effect of Methanol and Sample Molal Ratio Variation on the Biodiesel Yield                45
4.5       Results for Optimization Yield Studies of the Biodiesel Production using the Fractional Factorial Matrix Design   46
4.5.1    Predicted and Actual Values for Biodiesel Production from the Jansa Seed Oil.             46
4.5.2    Analysis of Variance (ANOVA) for Quadratic Model  48
4.5.3    Fit Statistics Results for the Biodiesel Production from the Jansa Seed Oil                     50
4.5.4    Results for the Coefficient in Terms of Coded Factors for the Biodiesel Production                                                50
4.5.5 Matrix Design Final Equation Developed in Terms of Coded Factors for the Effects of the Process Parameters on Biodiesel Produced from the Jansa Seed Oil                      51
4.6       Interactions of Significant Variables and Process Factors on the Biodiesel Yield                                                           53
4.6.1  Results of the Predicted and the Actual Interactions of Variables         53
4.6.2    3-Dimensional (3D) Plots Interactions Results of the Process Variables with the Biodiesel Yield.   53
4.7 Characterization of the Developed Biodiesel from the Jansa Seed Oil          59
4.7.1 Physicochemical Characterization Test Result of the Optimal Biodiesel Yield and the Blends from the Jansa Seed Oil.       59
4.7.2    Gas Chromatography of the Optimal Biodiesel Yield from the Jansa Seed Oil                65
4.7.3    Fourier Transfer Infrared Test Results of the Optimal Biodiesel Yield                            68

CHAPTER 5: CONCLUSION AND RECOMMENDATIONS
5.1       Conclusion                     69
5.1.1    Contributions to Knowledge of this Study    71
5.2       Recommendations         71
            References                                                                  72 
           Appendices                                                                     81





LIST OF TABLES
                                                                                                                     
3.1       Studied range of each factor in actual and coded form for heterogeneous catalysts         29

3.2       Experimental design matrix for transesterification studies catalyzed by lithium-ions-doped calcium and magnesium oxides                              30            
        
4.1       Physicochemical properties of the jansa bio-oil   35

4.2       FFAs profile identified in Cussonia bateri seed oil by GC  38

4.3       Fourier transform infrared spectrometry (FTIR) analysis of raw jansa seed oil                39

4.4       Predicted and actual values for biodiesel production from the jansa seed oil         47     
       
4.5       ANOVA results for quadratic model for the jansa seed oil biodiesel production (Response 1: Biodiesel yield)   49

4.6       Fit Statistics result for the biodiesel production    50

4.7       Results for the coefficients in terms of the coded factors for the biodiesel production                                            51

4.8 Methyl esters identified in the optimal biodiesel yield by gas chromatography         67      

4.9 FTTR analysis of the optimal biodiesel yield from the jansa seed oil                     68      








LIST OF FIGURES

2.1       Mechanism of SrO catalyst transesterification adapted           8

2.2       Flow chart for biodiesel production from heterogeneous catalyst (Lee et al., 2015)        10

3.1       Soxhlet apparatus set-up for bio-oil extraction from jansa seed            20

4.1  Gas chromatography column over ramping schedule of the jansa seed oil                       36  

4.2       Gas chromatograph of Cussonia bateri seed oil showing elution peaks of FFAs             37

4.3       Fourier transform infrared spectrometry (FTIR) of oil jansa seed oil                     39

4.4 Scanning electron microscopy of lithium doped metal oxides                                          42

4.5 Variation of biodiesel yield with catalyst variants for the initial biodiesel production     43

4.6 Effect of process conditions variation on biodiesel yield                                                  43

4.7 Effect of reaction time variation on the biodiesel yield                                                     44

4.8  Effect of reaction temperature variation on the biodiesel yield                                         44

4.9 Effect of agitation speed variation on the biodiesel yield                                                  45

4.10 Effect of methanol and sample molal ratio variation on the biodiesel yield                     45

4.11 Predicted versus actual plots for the biodiesel yield                        53

4.12 3D plot of Catalyst concentration and reaction temperature with biodiesel yield             54

4.13 3D plot of Catalyst concentration and reaction time with biodiesel yield                         54

4.14 3D plot of Catalyst concentration and agitation speed with biodiesel yield                      55

4.15 3D plot of Catalyst concentration and molal ratio with biodiesel yield                            55

4.16 3D plot of reaction temperature and reaction time with biodiesel yield                            56

4.17 3D plot of reaction temperature and agitation speed for the biodiesel yield                     57

4.18 3D plot of reaction temperature and molal ratio for the biodiesel yield                            57

4.19 3D plot of reaction time and agitation speed with biodiesel yield                                     58

4.20 3D plot of reaction time and molal ratio with the biodiesel yield                                     58

4.21 3D plot of agitation speed and molal ratio with the biodiesel yield                                  59

4.22 Variations of specific gravity with the fuel blends                                                            59          
                            
4.23 Variations of kinetic viscosity with the fuel blends                                                           60

4.24 Variations of flash point with the fuel blends                                                                    61

4.25 Variations of fire point with the fuel blends                                                                      61

4.26 Variation of cloud point with the fuel blends                                                                    62

4.27 Variations of pour point with the fuel blends                                                                    62

4.28 Variations of free fatty acid with the fuel blends                                                              63

4.29 Variations of API gravity with the fuel blends                                                                  63

4.30 Variations of anisidine value with the fuel blends                                                             64

4.31 Variation of diesel index with the fuel blends                                                                   64

4.32     Variation of calorific value with the fuel blends                                                               65

4.33     Gas chromatography column-oven ramping schedule of methyl ester (biodiesel) analysis                              66

4.34     Chromatogram of the optimal biodiesel yield from the jansa seed oil showing elution peaks of the methyl ester    67

4.35    Fourier transform infrared spectrometry (FTIR) of the optimal biodiesel yield from jansa seed oil                            68




CHAPTER 1
 INTRODUCTION

1.1 BACKGROUND OF THE STUDY

The environmental benefits of biodiesel fuel has made it more attractive in recent times. Its primary advantages deal with it being one of the renewable fuels currently available and it is also non-toxic and biodegradable. It can also be used directly in most diesel engines without requiring extensive engine modifications.
Van Gerpen (2005) defined biodiesel as a renewable, biodegradable, environmentally benign, energy efficient, substitution fuel which can fulfill energy security needs without sacrificing engine’s operational performance. From the above definition, it can be deduced that biodiesel is a resource that satisfies both vehicular and industrial energy need (fuel for engines without causing damage to them) as well as being environmentally compatible (renewable and biodegradable). In coming years, some crucial factors that will drive research and development in biodiesel production technologies as Van Gerpen (2005) stated are; fluctuation in the pricing of fossil based petrol, necessity for climate stabilization, economic policies and domestication of biodiesel production technologies. To further this cause, 38 nations recently from America, Asia and Europe adopted the biodiesel blend program (B5 to B10) aimed at widening its use for transportation and industrial purpose. 

Biodiesel according to Arzamendi et al.(2008) is an alternative to petroleum-based fuels. It has found a very wild application as energy source to drive passenger cars, sport utility vehicles, light trucks, buses, ships, trains, off-road heavy equipment, and mining equipment, as well as for home heating fuel, power generation, and as a mixing agent in two-stroke engines. Thus, in long term prospect, biodiesel usage will radically cover all types of consumer demand in ground transportation, aviation, and maritime fuel markets (Arzamendi et al., 2008).

1.2   STATEMENT OF PROBLEM
One of the earliest forms of fuel for engine combustion is straight vegetable oil of which majority are edible. However, the use of vegetable oil as a direct form of fuel has its challenges following some of the unfavourable physical properties. Lee et al.(2015) identified the undesirable physical properties of straight vegetable oils that  made them non excellent choices for biodiesel production. They include; high viscosity which leads to poor fuel atomization, inefficient mixing of oil with air leading to high smoke emission, coking and trumpet formation (carbon deposit) on the injectors which results to clogged orifices, low volatility as a result of high flash point, lubrication oil dilution, thickening or gelling of lubricating oil, high carbon deposits, oil ring sticking, scuffing of the engine liner, injection nozzle failure and high cloud and pour points. To this end, it is important to formulate a product, through modification of straight vegetable oil, with superior physical properties for energy production. Though significant progress have been made in the utilization of biodegradable materials for the production of biodiesel, there still exist some challenges in feed stock sourcing and selection, production pathway, choice of catalyst and other production conditions, product storage and distribution. 

Homogeneous alkaline catalysts (sodium hydroxide and potassium hydroxide) have been widely applied as catalysts for the production of biodiesel from various feed stock. Even as high yields are obtained most times, the process is mostly time consuming and could be expensive. The process of biodiesel production through reaction between vegetable oil feed stock and an alcohol in the presence of catalyst is called transesterification. When alkaline catalyst is used, it involves a set of sequential processes which requires neutralization to ensure the free fatty acid (FFA) content is considerably low. 

Also, following the use of alkaline catalyst, the process effluent, being alkaline, if passed into farm lands and fresh water bodies could be a major source of environmental concern. In strict adherence to local environmental safety standard, effluent treatment such that it should be neutralized will in no lesser form add to the production cost. These, notwithstanding, the processes are still time consuming even when other competitive processes are adapted to reduce time and cost. Using lithium- doped in magnesium or calcium oxides consequently will ensure that the catalysts are used up before disposal. The doping will increase the transesterification process and make it alkaline, as the waste water is neutralized before disposal to the municipal waste route. Hence, this causes no harm to the environment.

1.3   AIM AND OBJECTIVES OF STUDY

The aim of this study is to determine the optimum conditions for biodiesel production from jansa (Cussonia bateri) seed oil using lithium-doped (Li-doped) catalysts. The specific objectives are to  :

i. produce biodiesel by transesterification process from the jansa seed oil using methanol in the presence of the alkaline metal-based catalysts, and make the characterization.

ii. establish the optimal biodiesel yield (by volume) from the metallic oxides of the catalysts.

iii. formulate the biodiesel blends from the optimal yields of the two metallic oxides of the catalysts in the following forms; B100, B90, B80, B70, B60, B50, B40, B30, B20, B10 and D100 ; and characterize the blends.

iv. perform scanning electron microscopy (SEM) of the doped / modified catalysts.

v. carryout gas chromatography (GC) and Fourier transfer infrared spectrometry (FTIR) analyses of the Jansa seed oil and the optimal biodiesel yield from the two metallic oxides of the catalysts to determine the available free fatty acids methyl ester (FAME) profiles and the functional groups respectively. 

1.4   SCOPE OF STUDY

The study is limited to :

i.   Jansa seed (Cussonia bateri or Ugbaokwe in Igbo) oil production and its characterization.

ii. Transesterification process of the bio-oil with methanol in the presence of alkaline based catalysts (Li-CaO and Li-MgO) and their characterization.

iii. Perform gas chromatography (GC) and Fourier transfer infrared spectrometry (FTIR) analyses of the Jansa seed oil and the optimal biodiesel yield from the two metallic oxides of the catalysts

iv. Evaluation of the results and making comparison of the results with standard conventional diesel to establish the produced biodiesel suitability in diesel engine operations.

1.5   JUSTIFICATION OF THE STUDY

This research is an attempt to add value towards reducing the cost, as well as managing time of biodiesel production. This intention was achieved through the use of lithium-doped heterogeneous (CaO and MgO) catalysts. Though lithium being alkaline was applied, its adoption basically modified the physical properties of the heterogeneous catalysts, thus increasing their catalytic properties. The development in no little way provided significant foundational knowledge that created curiosity into further research opportunities on technological innovation. The development directed towards providing cleaner and safer transportation and industrial energy for power plant and automotive operations, was the hallmark for this research effort.     

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