ISOLATION AND CHARACTERIZATION OF BIOACTIVE COMPOUNDS OF LACTUCA TARAXACIFOLIA (WILD LETTUCE)

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ABSTRACT

This research work was carried out to identify the bioactive constituents of the leaves, stems and roots of Lactuca (Launaea) taraxacifolia, a medicinally important plant of the Asteraceae family. The plant was selected for this study due to its widespread use in traditional medicine and on the basis that the plant is almost going into extinct in Nigeria. The present study deals with the extraction, isolation and characterization of the bioactive compounds of the chloroform extracts of the leaves, stems and roots of L. taraxacifolia. The extraction was done by subjecting the air dried pulverized samples into the chloroform solvent for a period of some days, followed by filtration and concentration. Separation and purification of the various constituents of the crude extracts were carried out using thin layer chromatography and column chromatography. The TLC and column chromatography were carried out using different mobile phases and the solvent blends used were: normal hexane, chloroform, ethyl acetate and methanol. Qualitative TLC on precoated aluminium silicate strips was used to monitor the column fractions to ascertain the degree of purity of the eluents. The structural elucidation of the isolated compounds was deduced using MS, FTIR, NMR (1H and 13C) and 2D COSY NMR Spectra. This chemical investigation resulted in the isolation of two novel compounds: SB2 (Octadecahydro-4,4-dimethoxy-12b, 14b-dimethyl-10-(napthalen-2-yl) Picen-3-(4H, 6bH, 14bH)-one and SB3 (Octadecahydro-10-(1, 2, 3, 4-tetrahydronaphtalen-3-yl)-4,4-dimethoxy-6b, 12b, 14b-trimethyl Picen-3-(4H, 6bH, 14bH)-one. Compound SB2 was isolated using 90% chloroform and 10% ethyl acetate at an Rf value of 0.821, while compound SB3 was isolated using 50% hexane and 50% chloroform at an Rf value of 0.692. The MS spectrum of compound SB2 gave a molecular ion peak at m/z 527.75, which corresponds to a molecular formular of C36H47O3.The MS spectrum of compound SB3 gave a molecular ion peak at m/z 545.81, which corresponds to a molecular formular of C37H53O3. These terpenoid derivatives characterized by the presence of carbonyl and methoxy groups accounted for the antimicrobial, anti-tumor and anti-oxidant properties of the plant.The antimicrobial activities of the crude extracts were carried out using the disc diffusion technique. Fifteen micro-organisms (five-Gram positive, five Gram-negative and five fungi) were selected for the antimicrobial screening of the solvent extracts of the leaves, stems and roots of L. taraxacifolia. The zone diameters of inhibition of the extracts ranged from 10.1 mm to 17.2 mm. In all cases, the phytochemicals in the chloroform extracts had greater broad spectrum effects when compared to other extracts used in this work, thus inhibiting all the test bacteria used in this work, though with varying diameters of inhibition, while the phytochemicals in methanol extract had the least effect, inhibiting six out of the ten bacteria used in the study. Generally, the extracts had negligible inhibition effects on the selected fungi. Phytochemicals in n-hexane and ethyl acetate were only effective on Candida albicans at zone diameters of inhibition of 17.2 mm and 15.2 mm respectively. A major set-back associated with the intake of herbal medicine is the problem of overdose, which may lead to the destruction of tissues and cells. Hence the minimum inhibitory, bactericidal and fungicidal concentrations of the extracts were carried out. The results showed that the minimum inhibitory concentrations (MIC) of the extracts ranged from 200 mg/ml to greater than 250 mg/ml. Some of the extracts had minimum bactericidal concentration (MBC) of 250 mg/ml, which is the concentration of most conventional drugs.





TABLE OF CONTENTS

Title Page                                                                                                                                i

Declaration                                                                                                                              ii

Certification                                                                                                                            iii

Dedication                                                                                                                              iv

Acknowledgement                                                                                                                  v

Table of Contents                                                                                                                   vi 

List of Tables                                                                                                                          xii

List of Figures                                                                                                                         xiii

List of Plates                                                                                                                           xiv

Abstract                                                                                                                                  xv

 

CHAPTER 1: INTRODUCTION                                                                                     

1.1                    Background of the Study                                                                                        1

1.2                    Significance of  the Study                                                                                       3

1.3                    Justification of the Study                                                                                        4

1.4                    Statement of  the Problem                                                                                       5

1.5                    Aims and Objectives of the Study                                                                          5

1.6                    Scope of  the Study                                                                                                 6

 

CHAPTER 2: LITERATURE REVIEW                                                                         

2.1       Historical and Common Applications of Wild Lettuce                                               7                                                               

2.1.1        Common names of wild lettuce                                                                                  8                                                                                 

2.1.2        Taxonomy of Lactuca taraxacifolia                                                                           8                                                                     

2.1.3        Biological diversity and divergency of the genius                                                     11       

2.2        Taxonomy of the Genus Lactuca Species                                                                   11                                                             

2.2.1              Lactuca                                                                                                                    12                                                                                                    

2.2.2              Phaenixopus                                                                                                             12                                                                                                    

2.2.3              Mulgedium                                                                                                               13                                                                                                    

2.2.4              Lactucopsis                                                                                                              13                                                                                                                

2.2.5              Tuberosae, Micranthae and Sororiae                                                                      13                                                    

2.2.6              African group                                                                                                           14                                                                                                    

2.2.7              North American group                                                                                             14                                                                                        

2.2.8              Geographical distribution and ecology of genus Lactuca species                           16                   

2.2.9              Karyological status, biochemical and molecular markers                                        17                            

2.3                    Gene Pool of Lactuca Sativa and Crossability                                                        17                                                    

2.3.1              Regeneration of accessions of wild Lactuca species                                               19                                        

2.3.2              Chemical composition of wild lettuce                                                                     19                                                                

2.3.3              Pharmacology of wild lettuce                                                                                  20                                                                            

2.3.4              Demulcent and prebiotic effects of wild lettuce                                                     20                                                    

2.3.5              Digestion, inflammation and angiogenesis of wild lettuce                                      20

 

2.3.6              Hypoglycemic activities of wild lettuce                                                                  21       

2.3.7        Immunity                                                                                                                    21                               

2.3.8              Varieties of preclinical studies of wild lettuce                                                        22

                                                        

2.3.9        Hepatobiliary effects of wild lettuce                                                                          22                                                                               

2.4          Inhibitory Effects  of Wild Lettuce                                                                            22                                                                                   

2.4.1        Clinical applications, western studies                                                                         23

2.4.2        Clinical applications, Chinese studies                                                                         24

2.4.3    Dosage and sustainability of wild lettuce                                                                   25                                                       

2.4.4    Safety and drug interaction of wild lettuce                                                                26

2.4.5        Medical indications of wild lettuce                                                                            26                                                                                           

2.4.6        Liver Gall Bladder Statsis                                                                                          27                                                                                           

2.4.7              Edema                                                                                                                      27                                                                                                                

2.4.8              Colitis                                                                                                                       27                                                                                                                

2.4.9              Side effects and toxicity of wild lettuce                                                                 27                                                                                        

2.5                    Bioactive Compounds Found in Asteraceae                                                           28                                                    

2.5.1          Nutritional factors                                                                                                     29                                                                                                       

2.5.2              Structures of sesquiterpenes                                                                                    30                                                                            

2.5.3              Role  of the µ - methylene and – Y – lactone groups                                             33                            

2.5.4              Supression  of NF – KB                                                                                          34                                                                                        

2.5.5              Role of sesquiterpene lactones in people                                                                 36                                                    

2.5.6              Tumor inhibition by sesquiterpene lactones                                                 37                                                    

2.5.7              Alternative mechanism of anti-inflammatory activities                                           39                                        

2.5.8              The function of parthenolide in anti cancer therapy                                                40                            

2.5.9              Sesquiterpenoids in herbal  medicine                                                                       41                                                                

2.6                    Antioxidant Function of Sesquiterpene Lactone                                                     42                                                    

2.6.1              Bitter properties of sesquiterpene lactone                                                                43                                                                

2.6.2              Importance  of sesquiterpenes in plants                                                                   45                                                                

2.6.3              Anti-herbivory activities  of sesquiterpene lactones                                                46                                                    

2.6.4              Antimicrobial roles  of sesquiterpene lactones                                                         47

2.6.5              The use of sesquiterpene lactones to protect ozone layer                                        48       

2.6.6              Allelophathy                                                                                                             49                                                                            

2.6.7              Implications for crop production                                                                             50                                                                            

2.7                    Active Chemical Constituents                                                                                 51                                                                            

2.7.1              Cycloartenol                                                                                                             51                                                                                                    

2.7.2              Beta – sitosterol                                                                                                       53                                                                                                    

2.7.3              Vitamin A                                                                                                                54                                                                                                                

2.7.4              Ascorbic acid (vitamin C)                                                                                        56                                                                                        

2.7.5              Tannins                                                                                                                     58                                                                                        

2.7.6        Alkaloids                                                                                                                     59       

2.7.7        Cardiac glycosides                                                                                                      62                   

2.8       The   Biochemistry of Cardiac Glycosides                                                                 63       

2.8.1    Medical analysis of the activities of cardiac glycosides                                             66       

2.8.2    Anticancer characteristics and the mechanisms of cardiac glycosides                       66                   

2.9       Apigenin (Flavonoids)                                                                                                69                                                                                           

CHAPTER 3: MATERIALS AND METHODS                         

3.1          Preparation of Plant Materials for Column Chromatography                                  71

3.1.1       Packing of the large column                                                                        71

3.1.2       Packing of micro column                                                                                         72

3.1.3      Thin layer chromatography                                                                                       72

3.2        Phytochemical Screening of the Extracts                                                                 72

3.2.1      Determination of saponins                                                                                         72

3.2.2      Determination of phenols                                                                                         73

3.2.3      Determination of alkaloids                                                                                       73

3.2.4       Determination of tannins                                                                                         74

3.2.5       Determination of cardiac glycosides                                                                       75

3.2.6       Determination of flavonoids                                                                                   75

3.2.7       Determination of Steroids                                                                                       76

3.2.8       Determination of terpenoids                                                                                    76

3.3          Proximate Composition                                                                                           77

3.3.1       Determination of ash content                                                                                  77

3.3.2       Determination of crude fat                                                                                      77

3.3.3       Determination of crude fibre                                                                                   77

3.3.4       Determination of crude protein by Kjedahl method                                               78

3.3.5       Determination of moisture                                                                                       79

3.3.6       Determination of available carbohydrate                                                                 79

3.3.7       Determination of energy value                                                                                80

3.4          Preparation and Collection of Plant Materials for Antimicrobial                           

               Susceptibility Test.                                                                                                   80

3.4.1       Extraction of plant materials                                                                                    80

3.4.2       Preparation of test organisms                                                                                   80

3.4.3       Antimicrobial susceptibility test of the L. taraxacifolia extracts                             81

3.4.4       Test for minimum inhibitory concentration (MIC) of the

L. taraxacifolia extracts                                                                                           82

3.4.5       Test for minimum bactericidal (MBC) and fungicidal

concentration (MFC) of the extracts                                                                       82

 

CHAPTER 4: RESULTS AND DISCUSSION                                                         

4.1       Chromatographic Separation of L. taraxacifolia Extracts                                          83

4.2          Isolation of compound SB2                                                                                     87

4.2.1       13CNMR Spectrum of compound SB2                                                                    88

4.2.2       1HNMR Spectrum of compound SB2                                                                     90

4.2.3       COSY – 2D Spectrum of compound SB2                                                              93

4.2.4       Infra-red spectrum of compound SB2                                                                     95

4.2.5       Characterization of compound SB2                                                                        98

4.2.6       Mass spectral analysis of compound SB2                                                                99

4.3          Isolation of Compound SB3                                                                                    102

4.3.1       13CNMR spectrum of compound SB3                                                                     103

4.3.2       1HNMR spectrum of compound SB3                                                                      105

4.3.3       COSY – 2D spectrum of compound SB3                                                               108

4.3.4       Infra-red spectrum of compound SB3                                                                     110

4.3.5       Characterization of compound SB3                                                                        113

4.3.6       Mass spectral analysis of compound SB3                                                                114

4.4.         Phytochemical Composition of L. taraxacifolia                                                      117

4.5          Proximate Analysis of L. taraxacifolia Leaves.                                                       122

4.6          Antimicrobial Screening of the Extracts of L. taraxacifolia                                    125

4.7          Minimum Inhibitory/Bactericidal/Fungicidal Concentration of     

Extracts of L. taraxacifolia                                                                                      132

 

CHAPTER 5: CONCLUSION AND RECOMMENDATIONS             

5.1                    Conclusion                                                                                                               134

5.2                    Contributions to Knowledge                                                                                   135

5.3                    Recommendations                                                                                                   136

References                                                                                                               137

 

 



 

 

 

LIST OF TABLES


2.0                               The taxonomy of Lactuca Species, genetic resources

andtheir categorization to sections, subsections and groups              15       

2.1                               Survey of wild Lactuca and related genera

germplasm maintained in genebank collections                                  18

2.2                               Antiproliferrative activities of cardiac glycosides                              68

4.1                               Large column and thin layer chromatography of                               

L. taraxacifolia extracts                                                                       84

4.1.1                            Micro column and thin layer chromatography

of L. taraxacifolia extracts                                                                  86

4.2                               1HNMR and 13CNMR chemical shift of compound SB2                  92

4.3                               Infra-red spectrum of compound SB2                                                            97

4.4                               1HNMR and 13CNMR chemical shift of compound SB3                  107

4.5                               Infra-red spectrum of compound SB3                                                            112

4.6                               Qualitative screening of photochemicals in L. taraxacifolia               120

4.7                               Quantitative screening of phytochemicals in L. taraxacifolia 121

4.8                               Proximate composition and energy content of the

Leaves of L. taraxacifolia                                                                   124

4.9                               Antimicrobial activities of the extracts of Lactuca taraxacifolia        127     

4.9.1                            MIC, MBC & MFC of the extracts of Lactuca taraxacifolia             133






 

LIST OF FIGURES

2.1             Sesquiterpene lactones                                                                                          32

2.2             Structural characteristics of cardiac glycosides                                                    65

4.1                          13CNMR spectrum of compound SB2                                                                  89

4.1.1                    1HNMR spectrum of compound SB2                                                                   91

4.1.2                    COSY – 2D spectrum of compound SB2                                                                        94

4.1.3                    Infra-red spectrum of compound SB2                                                                  96

4.1.4                    Mass spectral analysis of compound SB2                                                             100

4.1.5                    Fragmentation scheme of compound SB2                                                            101

4.2                          13CNMR spectrum of compound SB3                                                                  104

4.2.1                    1HNMR spectrum of compound SB3                                                                   106

4.2.2                    COSY – 2D spectrum of compound SB3                                                                        109     

4.2.3                    Infra-red spectrum of compound SB3                                                                  111

4.2.4                    Mass spectral analysis of compound SB3                                                             115

4.2.5                    Fragmentation scheme of compound SB3                                                            116

4.3             Proximate composition of the leaves of L. taraxacifolia                                      123

4.4             Zones of inhibition of chloroform extract on different bacterial species             128

4.5             Zones of inhibition of hexane extract on different bacterial species

and on Candida albicans                                                                                      129

4.6             Zone of inhibition of methanol extract on different bacterial species                  130

4.7             Zones of inhibition of ethyl acetate extract on different bacterial

Species and on Candida albicans                                                                         131





LIST OF PLATES

2.0             Lactuca taraxacifolia              10

 

 


 

CHAPTER 1

INTRODUCTION


1.1:      BACKGROUND OF THE STUDY

Data obtained from recent researches showed that a range of 65% to  90% of people in most developing countries rely on  traditional medical practices in addition to herbal medicines in the treatment of ailments and to manage  their basic health-care requirements (WHO, 2002 – 2005). The application of traditional herbal medication is also essential in certain developed nations. Between 68% and 85% of the populace consume traditional medicines under the titles: “Complementary”, “alternative”, or “nonconventional” medications has been reported in developed nations like Canada, France, and Germany (WHO, 2005; Barnes et al., 2007 Traditional Medicine, 2008).

In the United States of America the application of complementary and combined medical methods in health care delivery is gaining grounds. A certain research shows that 43% of Americans used alternative therapies in 1997; 41% for treatment of acute ailments and 59% for disease control. In 2007, the most popularly applied complementary and traditional medical therapy include: non vitamins, non minerals and natural products constituting 17.7% (Barnes et al., 2007). Inspite of this rapid rise in the application of herbal medicines, limited evidence exists for their potency and toxic nature. More researches need to be carried out to develop the evidence base for herbals, botanicals and dietary supplements (Turner, 1965).

Conversely, natural products have been very essential for effective treatment and amelioration of disease burdens of humans and animals (Perry, 1980). Thus it is very important to evaluate natural products for their potency in the diagnosis of ailments. Most plants manufacture substances that are essential for the sustenance of health in humans and other animals. Such organic compounds include: aromatics like phenols, tannins and secondary metabolites of which not more than 12% have been isolated. In most situations, molecules such as alkaloids protect the plant against predators by micro-organisms, insects and herbivores. Most of the herbs and spices applied by humans to season their food give important medicinal phytochemicals (Lai and Roy, 2004; Tapsell et al., 2006). Analogous to the recommended drugs, a range of herbs are thought to have undesirable activities (Talalay, 2001). Additionally, adulteration, wrong combination or lack of knowledge of plants and mechanisms of drug interactions has caused negative effects that are mostly risky to life (Elvin-Lewis, 2001).The application of herbs to mitigate ailments is almost common with non-industrialized communities (Edgar et al., 2002). Most of the drugs currently accessible to medical practitioners have a connection to herbs as a major component as compared to other natural resources because of the belief that they have no side effects (Veale et al., 1992; Ram et al., 1997). The application of such and dietary supplement obtained from plants has greatly increased in recent years. Microbiologists, Pharmacologists, Botanists and Natural Product Chemists are carrying out research into phytochemicals for solutions that could be developed for the diagnosis of different ailments. According to World Health Organization, as much as 26% of the modern drugs obtained from plant products are used in the United States. Over the past one hundred years, about one hundred and twenty one pharmaceutical products have been found as a result of the information obtained from traditional healers (Anesini and Pereez, 1993). In certain Asian and African nations, 82% of the recommendations are to evaluate the safety and efficacy of each plant before they are prescribed for medical use (Vickers, 2007). Invariably, most consumers are of the thought that herbal medicine and synthetic drugs may act in synergy causing harm to the patient. It may also be severely contaminated and without proven potency may ignorantly be used to substitute drugs that do have similar potency (Ernst, 2007).

The use of Lactuca (Launea) taraxacifolia as a health-care remedy is scarcely documented. Despite the fact that not much studies have been done scientifically on the plant, claims from the public and herbalists recommended that the plant is very beneficial in the management of diabetes and as a mild laxative. The plant is also thought to provide a cure to high blood pressure, heart attack, stroke and other cardiovascular diseases (Leung and Foster, 1996). L. taraxacifolia leaves are consumed by  lactating cows in Northern part of Nigeria to enhance  milk production; it is also used to induce multiple birth rates in sheep and goats (Adinortey et al., 2012).Medicinally, the leaves are rubbed on legs to make children in Nigeria and Ghana walk; their leaves are combined  with ashes to cure yaws (Ayensu, 1978).

Lactuca (Launaea) taraxacifolia (Wild) is an annual West African tropical herb popularly known as Wild Lettuce or Dandelion. The plant is known in French as langue de vache which means “tongue of the cow”. There are some common names of the plant; Ga; agbloke, Ewe (anlo); anoto, Tivi; dadeou, Akan Akuapem, nne noa (boil today), Hausa: namijin dayii (applied loosely), Yoruba: efo yanrin, Sierra Leone: Kissi; bekuhoa-pomboe. The plant has leaves which are in arranged basal rosette form of 3-5, pinnately lobed with ultimate margins dentate. The stem is upright towering to about 1-3 meters high from a woody rhizome which is solitary branched and borne with 25-30 floret flowers with yellow corollas in a convex receptacle at the apex slightly narrowed, which gives rise to a white 7-8 mm long pappus air-borne seeds (Burkill, 1985).


1.2:      SIGNIFICANCE OF THE STUDY

Due to the increasing use of herbal medicine in the treatment of disease, it is pertinent to evaluate the extraction and bioactivity of endangered medicinal plants such as L. taraxacifolia in the treatment of wide range of diseases and in the production of conventional drugs.


1.3:      JUSTIFICATION OF THE STUDY

The worldwide use for medicinal plants is fast advancing (Yadav et al., 2010). The use of traditional medicine to aid orthodox medicine in the treatment of ailments in developing nations is increasing (Salahdeen and Yemitan, 2006). Conversely, these traditional medicines do not have enough proof for their potency or safety (WHO, 2000; Patwardhan, 2005; Mosihuzzaman and Choudhary, 2008).

Plant extracts and phytochemicals are very essential in therapeutic medicine (Varalakshmi et al., 2011). Safety evaluations of   these plants for medicines are very important since plants have many phytochemicals which may lead to toxicity either on their own or by interacting with other chemicals (Teixera et al., 2003).

Chaya leaves (Cnidoscolous acontifolius) are toxic as they contain cyanogenic glycosides that can cause electrolyte imbalance particularly hypokalemia (Westendorf, 1993). It was discovered that a high risk of lung cancer occurred in individuals consuming a mixture of betacarotene and vitamin E supplements (Goodman et al., 2004). Plants of the genus Euphorbia synthesize caustic lattices, which poses a health problem to humans and livestocks (Adedapo et al., 2004).

Launaea (Lactuca) taraxacifolia is a plant used  in  traditional herbal medicine for the treatment of skin and eye diseases – conjunctivitis, measles, diabetes mellitus and also rubbed on the legs  of toddlers to enhance  walking (Ayensu, 1978; Adebisi, 2004; Obi et al.,2006), abdominal disorders, heart burn, dyslipidaemia, liver diseases and also as food (Adinortey, 2012). Unfortunately, there is scarcity of evidence to support these uses and to determine the bioactive compounds in this plant. The World Health Organization supports research into the agents for diagnosis, management and control of ailments by the application of traditional medical practices (Atta and Mouneir, 2004).

Here, the plant Launaea taraxacifolia is evaluated for its phytochemical composition, antimicrobial activities, minimum inhibitory concentration (MIC), minimum bactericidal and fungicidal concentrations (MBC & MFC) of the extracts. In addition, advanced chromatographic techniques followed by spectral analysis of the extracts were used to elucidate the structures of the bioactive compounds of the plant. It is expected that the findings from this work may add to the overall value of the medicinal potential of the Launaea taraxacifolia.


1.4:      STATEMENT OF THE PROBLEM

There has been few documented work on L. taraxacifolia. These reports focused on the extraction of active components of L. taraxacifolia using a specific solvent and its antimicrobial activities on few microbes. In view of this, this current research evaluates the effectiveness of four different solvent extracts of the plant on microbes. There is few documented work on the structures of the bioactive compounds in L. taraxacifolia, hence there is need to carry out spectral analysis on the isolated components. A problem or disadvantage of herbal medicine is the consumption of overdose leading to the destruction of tissues and cells.

Hence, this research work further evaluates the Minimum Inhibitory Concentration and Minimum Bactericidal Concentration of the results of antimicrobial screening.


1.5:      AIM AND OBJECTIVES OF THE STUDY

The aim of this present study is to isolate and characterize the bioactive compounds of the plant Launaea (Lactuca) taraxacifolia.

The aim will be achieved using the following objectives:

ü   Effective utilization of chromatographic techniques and other extractive processes to isolate the components of L. taraxacifolia.

ü   Determination of the phytochemicals of L. taraxacifolia using different conventional methods

ü   Determination of the antimicrobial potency of solvent extracts of L. taraxacifolia

ü   Determination of the minimum inhibitory concentration, minimum bacterial concentration and minimum fungicidal concentration of the solvent extracts.


1.6:      SCOPE OF THE STUDY

This research work involved the separation of the components of air-dried plant materials of L. taraxacifolia by means of column chromatography. Four solvents namely: hexane, chloroform, ethyl acetate and methanol were employed in the chromatographic separation. The extracts obtained were then subjected to Thin Layer Chromatography (TLC) using pre-coated aluminium-silicate strips, in order to isolate pure samples for spectral analysis. The biological properties (antimicrobial, phytochemical content, minimum bactericidal concentration and minimum fungicidal concentration) of the extracts from the four solvents were also evaluated. Fifteen micro-organisms which include: five gram positive bacteria, five gram negative bacteria and five fungi were used in the antimicrobial susceptibility tests.

 

 

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