EXPERIMENTAL AND QUANTUM STUDIES ON THE CORROSION INHIBITION OF ZINC AND MILD STEEL IN HYDROCHLORIC ACID MEDIUM USING SCHIFF BASES.

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ABSTRACT

The corrosion inhibition of mild steel and zinc plates in 0.5M HCl in the presence and absence of 4-{[(Z)-(4-chlorophenyl)methylidene}amino)-N-(5-methy-l-furan-3-yl) benzenesulfonamide herein referred to as (MMBS) and 4-{[(Z)-(4-dimethyl amino) phenyl] methylidene} amino)-N-(5-methyl furan-3-yl) benzenesulfonamide herein refers to as (CMBS) was investigated at temperature ranges of 303 K to 343 K. Their inhibition performances were tested by weight loss and quantum chemical techniques and were characterised using Fourier Transform Infrared spectrophotometer (FT-IR). The FT-IR spectroscopy showed that the synthesised Schiff bases contained some functional groups which may have aided in the inhibition of the metal species under consideration. The results obtained from the weight loss method showed that inhibition efficiencies of the inhibitors increased as the concentrations of the Schiff-base molecules increased and with the highest inhibition efficiency observed at the optimum concentration of 1.0 g/L employed but decreased with rise in temperature. The inhibitor (MMBS) showed inhibition efficiency of 89.59 % while the inhibitor (CMBS) showed inhibition efficiency of 92.36 % for mild steel while for zinc plate, inhibition efficiencies were 38.19 % and 39.98 % for (MMBS) and (CMBS) respectively. Inhibition efficiencies were also found to decrease with increase in temperature. The inhibition efficiencies followed the order; (MMBS) < (CMBS). The Kinetic data obtained showed that the corrosion process followed first order kinetics. The following adsorption isotherms models including Langmuir and Freundlich employed in the interpretation of the inhibition data showed that Langmuir model provided the best fit to the experimental data (R2>0.96). Thermodynamic studies of the inhibition process showed that the ΔGads values for (MMBS) and (CMBS) were both negative indicating the spontaneity of the reaction and the values were less than -20 kJmol-1, indicating that the mechanism of adsorption is physisorption. The enthalpy values were positive for (MMBS) (121.650 – 148.904 Jmol-1K-1) on mild steel but negative for (MMBS) (-2.1213 to - 0.4059 Jmol-1K-1) on zinc showing that the reaction was endothermic for inhibition of mild steel but exothermic for inhibition of zinc. The quantum chemical parameters such as HOMO, LUMO, EHomo; Elijmoand Energy gap (ΔE), aided in the elucidation of the probable points of interaction of these inhibitors with mild steel and zinc. The results obtained from the chemical studies showed that there exists a relationship between the inhibitors’ efficiency and the energy gap (ΔE), energy of the highest unoccupied molecular orbital (EHomo), energy of the lowest occupied molecular orbital (ELumo), dipole moment (µ), softness (σ), as well as the hardness (η) of the inhibitor. The quantum chemical parameter, as indicators to their comparative inhibition potentials, agreed with experimental data.




TABLE OF CONTENTS.

Title Page                                                                                                                    i

Declaration                                                                                                                  ii

Certification                                                                                                                iii

Dedication                                                                                                                  iv

Acknowledgements                                                                                                    v

Table of Contents                                                                                                       vi

List of Tables                                                                                                              x

List of Figures                                                                                                             xii

Abstract                                                                                                                      xvi

 

CHAPTER 1: INTRODUCTION                                                                          1

1.1       Background of the Study                                                                               2

1.2       Statement of the Problem                                                                               4

1.3       Justification for the Research                                                                         6

1.4       Aim of the Research                                                                                       8

1.5       Specific Objective of the Study                                                                     8

1.6       Scope of the Research                                                                                    8

1.7       Limitation and De-limitation of the study                                                      9

 

CHAPTER 2:  LITERATURE REVIEW                                                             10

2.1       Definition of Corrosion                                                                                  10

2.2       Corrosion Parameters                                                                                      11

2.3       Classification of Corrosion                                                                             16

2.4       Types of Corrosion                                                                                         16

2.5       Corrosion Inhibitors                                                                                        20

2.6       Types and Mechanisms of Inhibitors                                                              23

2.6.1        Passivating inhibitors.                                                                                     23

2.7       Environmental Conditions (Scavengers)                                                        28

2.7.1    Organic corrosion inhibitors                                                                            29

2.7.2.   Green inhibitors                                                                                              32

2.7.3.   Amino acids as corrosion inhibitor                                                                 34

2.8       Schiff Base                                                                                                     35

2.8.1        Synthesis of Schiff base                                                                                 36

2.8.2.   Schiff base as corrosion inhibitor                                                                    36

2.8.3.      Coordination chemistry of Schiff base                                                           37

2.8.4    Mechanisms of Schiff base inhibitors.                                                            37

2.8.5    Review of current literature on the use of Schiff bases as inhibitors for

            corrosion                                                                                                         39

2.9       Literature Review of Quantum Chemical Method Used in the

            Study of Corrosion                                                                                         40

2.10     Methods of Monitoring Corrosion                                                                  42

2.10.1  X-Ray diffraction (XDS) and X-ray photoelectron spectroscopy                 42

2.10.2  Gasometric method                                                                                         43

2.10.3 Gravimetric technique                                                                                     44

2.10.4  Calculation of thermodynamic parameters                                                     45

2.10.5  Activation energy (Ea)                                                                                    46

2.10.6 Gibbs free energy of adsorption (ΔGads)                                                       47

2.10.7 Fourier transform infra-red spectroscopy (FTIR) technique                           47

2.10.8  Electrical resistance probe technique                                                              48

2.10.9  Scanning electron microscopy technique                                                       48

2.10.10 Thermometric technique                                                                                49

2.10.11. Electrochemical measurements (polarisation)                                               49

2.10.12 Electrochemical impedance spectroscopy (EIS)                                            50

2.11     Adsorption Consideration                                                                              50

2.11.1  Langmuir adsorption isotherm                                                                        51

2.11.2  Temkin adsorption isotherm                                                                           52

2.11.3 Flory - Huggins adsorption isotherm                                                               52

2.11.4  Frumkin adsorption isotherm                                                                          53

2.11.5 Freundlich adsorption isotherm                                                                       53

2.12     Computational Chemistry and Corrosion Study                                            54

 

CHAPTER 3: MATERIALS AND METHODS                                                   56

3.1       Materials                                                                                                         56

3.1.1    Samples                                                                                                           56

3.1.2        Reagents / chemicals                                                                                       56

3.1.3        Apparatus / equipment                                                                                    56

3.2       Methods                                                                                                         56

3.2.1    Metal coupons                                                                                                 56

3.2.2    Preparation of Schiff base (MMBS).                                                              57

3.2.3    Preparation of Schiff base (CMBS).                                                               58

3.2.4       Preparation of 0.5 M HC1 from stock solution                                               58

3.2.5    Preparation of acid solution                                                                            60

3.2.6    Preparation of washing solution (22 % NaOH and 22 g/l Zinc dust)             61

3.2.7    Preparation of inhibitor solutions                                                                    61

3.3       Corrosion Studies                                                                                           62

3.3.1.    Weight loss technique                                                                                     61

3.3.2.      Quantum chemical calculation                                                                        62

3.3.3.      Fourier transform infrared spectroscopy                                                         63

CHAPTER 4: RESULTS AND DISCUSSION                                                    64

4.1       Fourier Transform Infrared (FTIR) Spectroscopy                                          64

4.2:      Weight Loss Results                                                                                       67

4.3       Surface Coverage and Inhibition Efficiency                                                 78

4.4       Concentration and Temperature Dependence on Inhibition Efficiency         93

4.5       Corrosion Rate Results.                                                                                  94

4.6       Corrosion and Corrosion Inhibition Mechanism                                             99

4.7       Kinetic Studies of Mild Steel and Zinc Corrosion in HCl Solution in

            the Presence of Inhibitor                                                                                 100

 4.8      Activation Energy and Frequency Factors                                                     123

 4.9      Enthalpy and Entropy of Activation                                                              129

4.10     Adsorption Isotherm                                                                                       135

4.10.1: The Langmuir model                                                                                       136

4.10.2 The Freundlich isotherm model.                                                                      142

4.11    Quantum Chemical Study                                                                               148

4.11.1    Global molecular reactivity                                                                             152

4.11.2 HOMO energy (Ehomo)                                                                                     152

4.11.3  LUMO energy (Elumo)                                                                                153

4.11.4.  Energy gap (ΔE)                                                                                             153

4.11.5    Dipole moment (µ)                                                                                          153

4.11.6    Softness (δ).                                                                                                    154

4.11.7    Hardness (η)                                                                                                    154

4.11.8    Electronegativity (χ)                                                                                       154

4.11.9    Electrophilicity index (ω)                                                               155

4.11.10  Number of transferred electrons (ΔN)                                                          155

CHAPTER 5: CONCLUSION AND RECOMMENDATIONS                         157

5.1       Conclusion                                                                                                      157

 5.2      Recommendations                                                                                          158

References                                                                                                     


 

 

LIST OF TABLES

4.1       Absorption frequencies of the various functional groups                               66

4.2       Surface coverage and Inhibition efficiency of MMBS on mild steel.            89

4.3       Surface coverage and inhibition efficiency of CMBS on mild steel.             90

4.4       Surface coverage and inhibition efficiency of MMBS on zinc.                     91

4.5       Surface coverage and inhibition efficiency of CMBS on zinc                       92

4.6       Corrosion rates of mild steel using MMBS at various concentrations and

            temperatures                                                                                                    95

4.7       Corrosion rates of mild steel using CMBS at various concentrations

             and temperatures.                                                                                           96

 

4.8        Corrosion rates of zinc using MMBS at various concentrations and

            temperature                                                                                                     97

4.9       Corrosion rates of zinc using CMBS at various concentrations and

            temperature                                                                                                     98

4.10     Rate constants and half-life of steel for MMBS at 303 K                             103

4.11     Rate constants and half-life of steel for MMBS at 313 K                             104

4.12     Rate constants and half-life of steel for MMBS at 323 K                             105

4.13     Rate constants and half-life of steel for MMBS at 333 K                             106

4.14     Rate constants and half-life of steel for MMBS at 343 K                             107

4.15     Rate constants and half-life of steel for CMBS at 303 K                              108

4.16     Rate constants and half-life of steel for CMBS at 313 K                              109

4.17     Rate constants and half-life of steel for CMBS at 323 K                              110

4.18     Rate constants and half-life of steel for CMBS at 333 K                              111

4.19     Rate constants and half-life of steel for CMBS at 343 K                              112

4.20     Rate constants and half-life of zinc for MMBS at 303 K                              113

4.21     Rate constants and half-life of zinc for MMBS at 313 K                              114

4.22     Rate constants and half-lives of zinc for MMBS at 323 K                            115

4.23     Rate constants and half-life of zinc for MMBS at 333 K                              116

4.24     Rate constants and half-life of zinc for MMBS at 343 K                              117

4.25     Rate constants and half-life of zinc for CMBS at 303 K                               118

4.26     Rate constants and half-life of zinc for CMBS at 313 K                               119

4.27     Rate constants and half-life of zinc for CMBS at 323 K                               120

4.28     Rate constants and half-life of zinc for CMBS at 333 K                               121

4.29     Rate constants and half-life of zinc for CMBS at 343 K                               122

4.30     Activation energy and frequency factor values for MMBS on mild steel      125

4.31     Activation energy and frequency factor values for CMBS on mild steel      126

4.32     Activation energy and frequency factor values for MMBS on zinc               127

4.33     Activation energy and frequency factor values for CMBS on zinc               128

4.34     Entropies and enthalpies of activation values for MMBS on mild steel        130

4.35     Entropies and enthalpies of activation values for CMBS on mild steel         131

4.36     Entropies and enthalpies of activation values for MMBS on zinc                 132

4.37     Entropies and enthalpies of activation values for CMBS on zinc                  133

4.38     Free energy and adsorption parameters for MMBS on mild steel the plots   138

4.39     Free energy and adsorption parameters for CMBS on mild steel the plots    139

4.40     Free energy and adsorption parameters for MMBS on zinc the plots            140

4.41     Free energy and adsorption parameters for CMBS on zinc the plots             141

4.42     Free energy and adsorption parameters for MMBS on mild steel                  143

4.43     Free energy and adsorption parameters for CMBS on mild steel                   144

4.44     Free energy and adsorption parameters for MMBS on zinc                           145

4.45     Free energy and adsorption parameters for CMBS on zinc                            146

4.46     Derived quantum chemical parameters from semi-empirical (PM3)

             method for the Schiff bases MMBS and CMBS.                                         151

4.47     Comparative study of calculated quantum parameters of inhibitors.             151





LIST OF FIGURES.

2.1       Evans type diagram showing corroding system under anodic inhibition       25

2.2       Evans type diagram showing corroding system under cathodic inhibition    26

2.3       Evans type diagram showing corroding system under mixed inhibition                       26

2.4       Type diagram – showing corrosion kinetics for mixed inhibition                   28

2.5       Structure of Schiff Base                                                                                 36

3.1       Scheme 1-preparation of Schiff base CMBS                                                  58

3.2       Scheme 2- preparation of Schiff base CMBS                                                 59

4.1       The FTIR spectrum of MMBS                                                                       65

4.2       The FTIR spectrum of CMBS                                                                                    67

4.3       Plot of weight loss (mild steel) vs time for MMBS at 303K.                         68

4.4       Plot of weight loss (mild steel) vs time for MMBS at 313K.                         68

4.5       Plot of weight loss (mild steel) vs time for MMBS at 323K.                         69

4.6       Plot of weight loss (mild steel) vs time for MMBS at 333K.                         69

4.7       Plot of weight loss (mild steel) vs time for MMBS at 343K.                         70

4.8       Plot of weight loss (mild steel) vs time for CMBS at 303K.                          70

4.9       Plot of weight loss (mild steel) vs time for CMBS at 313K.                          71

4.10     Plot of weight loss (mild steel) vs time for CMBS at 323K.                          71

4.11     Plot of weight loss (mild steel) vs time for CMBS at 333K                           72

4.12     Plot of weight loss (mild steel) vs time for CMBS at 343K.                          72

4.13     Plot of weight loss (zinc plate) vs time for MMBS at 303K.                         73

4.14     Plot of weight loss (zinc plate) vs time for MMBS at 313K.                         73

4.15     Plot of weight loss (zinc plate) vs time for MMBS at 323K.                         74

4.16     Plot of weight loss (zinc plate) vs time for MMBS at 333K.                         74

4.17     Plot of weight loss (zinc plate) vs time for MMBS at 343K.                         75

4.18     Plot of weight loss (zinc plate) vs time for CMBS at 303K.                          75

4.19     Plot of weight loss (zinc plate) vs time for CMBS at 313K.                          76

4.20     Plot of weight loss (zinc plate) vs time for CMBS at 323K.                          76

4.21     Plot of weight loss (zinc plate) vs time for CMBS at 333K.                          77

4.22     Plot of weight loss (zinc plate) vs time for CMBS at 343K.                          77

4.23     Plot of I.E. vs concentration of inhibitors (MMBS) for mild steel at 303 K. 79

4.24     Plot of I.E. vs concentration of inhibitors (MMBS) for mild steel at 313 K. 79

4.25     Plot of I.E. vs concentration of inhibitors (MMBS) for mild steel at 323 K. 80

4.26     Plot of I.E. vs concentration of inhibitors (MMBS) for mild steel at 333 K. 80

4.27     Plot of I.E. vs concentration of inhibitors (MMBS) for mild steel at 343 K. 81

4.28     Plot of I.E. vs concentration of inhibitors (CMBS) for mild steel at 303 K. 81

4.29     Plot of I.E. vs concentration of inhibitors (CMBS) for mild steel at 313 K. 82

4.30     Plot of I.E. vs concentration of inhibitors (CMBS) for mild steel at 323 K  82

4.31     Plot of I.E. vs concentration of inhibitors (CMBS) for mild steel at 333 K. 83

4.32     Plot of I.E. vs concentration of inhibitors (CMBS) for mild steel at 343 K. 83

4.33     Plot of I.E. vs concentration of inhibitors (MMBS) for Zinc at 303 K.         84

4.34     Plot of I.E. vs concentration of inhibitors (MMBS) for Zinc at 313 K.         84

4.35     Plot of I.E. vs concentration of inhibitors (MMBS) for Zinc at 323 K          85

4.36     Plot of I.E. vs concentration of inhibitors (MMBS) for Zinc at 333 K.         85

4.37     Plot of I.E. vs concentration of inhibitors (MMBS) for Zinc at 343 K.         86

4.38     Plot of I.E. vs concentration of inhibitors (CMBS) for Zinc at 303 K           86

4.39     Plot of I.E. vs concentration of inhibitors (CMBS) for Zinc at 313 K           87

4.40     Plot of I.E. vs concentration of inhibitors (CMBS) for Zinc at 323 K.          87

4.41     Plot of I.E. vs concentration of inhibitors (CMBS) for Zinc at 333 K           88

4.42     Plot of I.E. vs concentration of inhibitors (CMBS) for Zinc at 343 K.          898

4.43     A plot of –log (weight loss of steel) vs. time for MMBS at 303 K                103

4.44     A plot of –log (weight loss of steel) vs. time for MMBS at 313 K                104

4.45     A plot of –log (weight loss of steel) vs. time for MMBS at 323 K                105

4.46     A plot of –log (weight loss of steel) vs. time for MMBS at 333 K                106

4.47     A plot of –log (weight loss of steel) vs. time for MMBS at 343 K                107

4.48     A plot of –log (weight loss of steel) vs. time for CMBS at 303 K                 108

4.49     A plot of –log (weight loss of steel) vs. time for CMBS at 313 K                 19

4.50     A plot of –log (weight loss of steel) vs. time for CMBS at 323 K                 110

4.51     A plot of –log (weight loss of steel) vs. time for CMBS at 333 K                 111

4.52     A plot of –log (weight loss of steel) vs. time for CMBS at 343 K                 112

4.53     A plot of –log (weight loss of zinc) vs. time for MMBS at 303 K                 113

4.54     A plot of –log (weight loss of zinc) vs. time for MMBS at 313 K                 114

4.55     A plot of –log (weight loss of zinc) vs. time for MMBS at 323 K                 115

4.56     A plot of –log (weight loss of zinc) vs. time for MMBS at 333 K                 116

4.57     A plot of –log (weight loss of zinc) vs. time for MMBS at 343 K                 117

4.58     A plot of –log (weight loss of zinc) vs. time for MMBS at 303 K                 118

4.59     A plot of –log (weight loss of zinc) vs. time for CMBS at 313 K                 119

4.60     A plot of –log (weight loss of zinc) vs. time for CMBS at 323 K                 120

4.61     A plot of –log (weight loss of zinc) vs. time for CMBS at 333 K                 121

4.62     A plot of –log (weight loss of zinc) vs. time for CMBS at 343 K                 122

4.63     An Arrhenius plot of ln CR vs. 1/T for MMBS on mild steel                        125

4.64     An Arrhenius plot of ln CR vs. 1/T for CMBS on mild steel                         126

4.65     An Arrhenius plot of ln CR vs. 1/T for MMBS on zinc                                 127

4.66     An Arrhenius plot of ln CR vs. 1/T for CMBS on zinc                                  128

4.67     Eyring plot of ln (CR/T) vs. 1/T for MMBS on mild steel                             130

4.68     Eyring plot of ln (CR/T) vs. 1/T for CMBS on mild steel                              131

4.69     Eyring plot of ln (CR/T) vs. 1/T for MMBS on zinc                                      132

4.70     Eyring plot of ln (CR/T) vs. 1/T for CMBS on zinc                                       133

4.71     Langmuir plots for MMBS on mild steel at various temperatures.                 138

4.72     Langmuir plots for CMBS on mild steel at various temperatures.                 139

4.73     Langmuir plots for MMBS on zinc at various temperatures                           140

4.74     Langmuir plots for CMBS on zinc at various temperatures                           141

4.75     Freundlich isotherm plots for MMBS on mild steel                                       143

4.76     Freundlich isotherm plots for CMBS on mild steel                                        144

4.77     Freundlich isotherm plots for MMBS on zinc.                                               145

4.78     Freundlich isotherm plots for MMBS on zinc                                                146

4.79     Optimised geometry of MMBS Schiff base (inhibitor)                                  149

4.80     Homo orbitals of MMBS Schiff base (inhibitor)                                            149

4.81     Lumo orbitals of MMBS Schiff base (inhibitor)                                            149

4.82     Optimised geometry of CMBS Schiff base (inhibitor)                                   150

4.83     Homo orbitals of CMBS Schiff base (inhibitor)                                             150

4.84     Lumo orbitals of CMBS Schiff base (inhibitor)                                             150

 

 

 

 

 

CHAPTER 1

INTRODUCTION

The surface of iron and steel, existing in many forms ranging from exposed metal to oxidized metal and to different degrees of states, finds many industrial applications (Ballesteros et al., 2015; Barros et al., 2016; Souza et al., 2016). Some investigations have emphasized the importance for the protection of the metal surfaces in various applications (Amitha, 2012). The spontaneous destruction of metals, starting from their surfaces, due to the corrosive attack of environment brings the undesirable changes at the surfaces and reduces their lifetime, strength and changes the desirable properties of metal surfaces. In some cases, the corrosion products formed are toxic. An accurate description of surface not only helps to identify the prevailing form of corrosion but also the prescription of appropriate anti-corrosion measures.

Acid solutions, (in particular HCl solutions) are widely used in industries for many purposes, such as acid pickling, industrial acid cleaning, acid descaling and oil well acidizing (Ochoa et al., 2013; Danaee et al., 2013; Gerengi et al., 2014; Rocha et al., 2014). Due to the general aggressive nature of acid solutions, the corrosive attack will be severed (Ochoa et al., 2013) and bring undesirable changes at the surface of metals. Chemical inhibitors are often used to control the corrosive attack and acid consumptions of environment (Ghasemi et al., 2013; Santana et al. 2015,). Most of the well-known corrosion inhibitors are the organic compounds containing N, S, O and P atoms (Santos et al., 2017; Barreto et al., 2018). These organic compounds reduce the metal dissolution by the adsorption onto the metal surfaces (Sivakumar et al., 2018). The adsorption and inhibition efficiency of these compounds greatly depend on the electron density around the hetero atoms, the number of adsorption active canters in the molecule and their surface charge density, molecular size, mode of adsorption and formation of metallic complexes (Barreto et al., 2018; Abdallah et al., 2019).

However, the choice of inhibitors is based on two considerations, first economic consideration and seconds the presence of the electronegative atoms such as N, O, P in the relatively long compounds. Thermodynamic model is an important tool used for analyzing the corrosion inhibition mechanism of inhibitors and their adsorption onto the metal surfaces (Fergachi et al., 2018; Santos et al., 2019). Based on the type of adsorption isotherm that the inhibitor molecule follows for the adsorption onto the metal surface, values of thermodynamic parameters such as adsorption equilibrium constant (Kads) and free energy change of adsorption(ΔGads) can be calculated and used for predicting the nature of adsorption and inhibition mechanisms.


1.1              BACKGROUND OF THE STUDY

Corrosion inhibitors are the compounds that are usually added in small amount into an aggressive medium. The presence of these compounds in the medium, will reduce the corrosivity of the medium significantly. Many authors have written papers on this subject, and they are available in chemical literature on the varieties of inhibitors which have been developed according to the metal/environment combinations. The inhibitors are either anodic or cathodic, oxidizing, or non-oxidizing and organic or inorganic depending on the end use requirement. Majority of the effective inhibitors from this category are toxic or possess a hazard in their use. It would be advantageous if environment friendly compounds would be used instead. For this thesis, more environmentally friendly inhibitors will be used in this experiment.

Zinc ions have long been considered as valuable corrosion inhibitors for carbon steel in aerated water because of the protection afforded by a cathodic polarization mechanism. Zinc increases the cathodic polarization and hence inhibits corrosion of steel. Its action is attributed to precipitation of zinc hydroxide on the cathodic areas because of locally high pH. Moreover, at the cathodes, oxygen is reduced with the generation of hydroxyl ions. This zinc can be added as any zinc containing salt, but most people use either zinc sulphate or zinc chloride as the source. Zinc chloride is readily available as a 50% aqueous solution for ease of handling and safety as well as economy (Thomas, 1991).

The adverse effect of corrosion can be seen in daily life. Corrosion causes accidents in industry, on highways, and in homes.  It is wasteful financially, costing industrialized nations 4-5% of their gross domestic products (GDP) annually. A little knowledge of electrochemistry, material science and corrosion could save nations some 25% of this loss (Hansson, 2011).

Corrosion chemistry is the application of science and art to prevent or control corrosion damage in a safe and economical manner. To perform this function properly, the corrosion scientist must rely on experimental research. This is because the major aspects of corrosion chemistry are largely empirical in nature.

Corrosion tests are conducted for several reasons including:

1.   Establishing corrosion mechanisms.

2.   Defining corrosion resistance of materials and how to develop new corrosion resistant alloys.

3.   Estimating service life of equipment.

4.   Developing corrosion protection processes.

5.   Defining the critical potential values for materials in various environments.


1.2       STATEMENT OF THE PROBLEM

Mild steel and zinc are the major items of construction of the cisterns in the petrochemical industrial processes involving storage of acids (often referred to as hold up tanks) before use. This is a major operation in all industries utilizing these acids. The mild steel option as a material of choice is because it is cheap and easily obtained when compared to stainless steel (six times as expensive). Also, in the transport of these acids from one point to another in the process plant, mild steel pippings are used because of the cost advantage. These pippings are also connected to fittings (valves, actuators and strainers) made of aluminium alloys and some other metallic alloys in some instances. However, they are prone to the damaging effects of the acid over time as they continuously interact with the acids. The damaging effects become obvious when the load carrying capacity of such facilities like shafts or shell thickness become compromised by reduction in the effective diameter or thickness as a result of metal loss from corrosive attack. The effective diameter or thickness is unable to support the tensile, compressive, or radial load and so failure becomes imminent and sometimes catastrophic.

Over the years, reports of product spillage in industries have pervaded the tabloids.

Many of such incidents are the direct effect of corrosion on facilities in service. In 2001, a United States (U.S) refinery experienced an incident in which one worker was killed, eight injured and significant offsite environmental impact on the surrounding water body which led to loss of marine life (CSB, 2002). Subsequent ultrasonic test report identified progressive corrosion of hydrochloric acid steel storage tank as the major cause of the incidence. In specific terms it said approximately half of the corrosion allowance was used up in the large sections of the entire exposed area of the tank. This meant that the mechanical integrity of the tank was compromised which led to failure of the tank. A finite elemental analysis of the tank further revealed that the load carrying capacity of the tank had been reduced drastically. Additional challenges associated with these failures include:

(a)    Economic loss due to replacement of corroded equipment resulting in heavy expenditure and man-hour loss.

(b)   Facility replacement cost,

(c)    Litigation for compensation by affected communities,

(d)   Negative publicity,

(e)    Inferred costs resulting from investigating/monitoring, overhaul and revamping and

(f)    Untold hardship on the populace because of withdrawal of such facilities from use.

It is thus essential that these metallic structures are protected. Several means are available for preventing or protecting metallic structures in service. These techniques include: materials selection, coatings, cathodic/anodic protection and use of corrosion inhibitors. The use of inhibitors has grown in popularity over the years. There exist two major types of inhibitors. These are organic and inorganic/chemical inhibitors.

The inorganic inhibitors contaminate the environment after use and cause a lot of problems like disposal and destruction of plant and animal life. Restrictions have been placed on the use of some of these chemical inhibitors because of their toxic nature (CSPC, 1977). The organic inhibitors are further sub-divided into synthetic or artificial organic inhibitors and the green organic inhibitors. Some of the artificial organic inhibitors are harmful to human existence. The focus of this study, therefore, is on the utilization and partial substitution of chemical inhibitors with green inhibitors because it is a sustainable means of arresting corrosion problems.

Moreover, it is cheap and easily available. It does not contaminate the environment and disposal is not an issue. For this reason, litigations are not a common issue of concern. Also, the use of green inhibitors could prove to be an employer of labour. Once suitable plant extracts have been identified by appropriate testing in curtailing corrosion in particular environments by researchers in the field, the information could be communicated to growers who would in turn produce in commercial quantities based on agreements with investors.

Due to its economic and ecological implications and low-level awareness, the problems of metallic degradation continue to reoccur worldwide. The world corrosion organization on April 24, 2009, started a campaign of creating awareness for corrosion and the problems associated with it. It was tagged international corrosion awareness day. The purpose was to stimulate education and best practices in corrosion control for socio-economic welfare of society, preservation of resources and protection of the environment.


1.3       JUSTIFICATION FOR THE RESEARCH

Corrosion is the degradation of the metallic properties of a metal. It progressively expends limited mineral resources and the energy utilized in the mining and processing of metals together with that employed in the production of machinery and infrastructures. Corrosion is known to affect practically all facet of contemporary development or advancement. Therefore, the deterrence of corrosion is of foremost commercial and ecological significance. The world corrosion organization has posited that the annual cost of corrosion globally is approximately 2.2 trillion US dollars. This represents more than 3 % of the World’s Gross Domestic Product (GDP) (Koch et al., 2002). In Nigeria, the cost of corrosion has not yet been surveyed; however, the Central Intelligence Agency (CIA) world fact book on Nigeria however puts it at an estimated 3.2 billion USD annually (CIA, 2006). This implies that further increases in corrosion control measures are required in every area of human life and industry.

From the power sector where energy is generated and the wastewater treatment plants that purify our water to the pipelines and storage cisterns that transport our much-needed petroleum products, corrosion control products are being used extensively. The addition of an inhibitor to a system is one major technique of controlling corrosion. A study conducted by the National Association of Corrosion Engineers (NACE) in 2002, showed that the total expenditure on corrosion inhibitors in the United States increased by 83.3% from about $600 million in 1982 to almost $1.1 billion in 1998 (NACE, 2002). This shows a fast-growing interest in the use of inhibitors as a corrosion protection technique. A passive protective film is formed on the metal when the inhibitor interacts with the metal. Inhibitors that work this way are normally the types added to vehicle cooling units and corrosion retarding extracts in protective coatings for metals. Conversely, most of the inhibitors employed presently are harmful with attendant undesirable effect on plant and animal life. Now in the industrialized countries like the U.S, there is mounting demands by lawmakers for the eradication of heavy metal mixtures and noxious inorganic and organic corrosion inhibitors, thus making research efforts geared towards the enhancement and development of efficient and eco-friendly inhibitors crucial. A look at literature shows that there has been some progress made in the emergence of new and efficient inhibitors currently (Shveta, and Ashish, 2020). Metal-based and anionic inhibitors like potassium, magnesium, lead, chromates, and those comprising of a mixture of lethal anions (molybdates, benzoates, nitrites, phosphates, and fluorides) are to a great extent adequate or suitable but not eco-friendly. Accordingly, a greater part of inhibitors presently utilized in the metal surface engineering and finishing, chemical, coatings and automobile industry need substitution by eco-friendly materials. Unfortunately, too, there are insufficient facts on eco-friendly corrosion inhibitors. Therefore, it is the desire of this work to come up with corrosion inhibitor compositions appropriate for use on hydrochloric acid solution on mild steel and zinc metals.

 

1.4       AIM OF THE RESEARCH

The aim of the present research pertains to the generation of measurable and testable experimental data towards the control of corrosion of mild steel and zinc in HCl through the development of environmentally friendly synthesized Schiff bases as organic corrosion inhibitors.


1.5       SPECIFIC OBJECTIVES OF THE STUDY

The objectives of the research are:

i. To evaluate the effects of two Schiff bases on the corrosion of mild steel and zinc in   0.5 M HCl through weight loss measurement.

ii. To determine metal-inhibitor interaction mechanism using some adsorption isotherms namely, Langmuir, Freundlich, and Temkin.

iii. To determine the mode of inhibition of the inhibitors using the kinetic parameters.

iv. To investigate the surface morphology of the metals in the presence and absence of the inhibitors and

v. To carry out quantum chemical studies of the corrosion test.


1.6       SCOPE OF THE STUDY

The scope of this study includes the following:

        i.            Laboratory designed experimentation for weight loss study of mild steel and zinc specimens in hydrochloric acid medium in the presence of varying concentrations of green inhibitors (two Schiff bases) at different temperatures.

      ii.            Surface characterization of the inhibitors using Fourier Transform Infra-red spectroscopy (FTIR).

    iii.            Quantum chemical studies were also performed.

 

1.7       LIMITATION AND DELIMITATION OF THE STUDY

The experiment carried out shows that the effectiveness of corrosion inhibitors depends upon factors such as the electron density of the donor atom in the inhibitor molecules, molecular geometry and the size of the inhibitor molecule and the solubility/dispersibility of the inhibitor. The following factors can pose limitation to this as stated below

·         Use non-corrosive metals, such as stainless steel or aluminium.

·         State of the metal surface stays which must be cleaned and dry.

·         Use drying agents.

·         Use a coating or barrier product such as grease, oil, paint or carbon fibre coating.

·         Lay a layer of backfill, for example limestone, with underground piping.

 

For this reason, this study is not preoccupied with bioaccumulation study, storage stability, durability of the Schiff base inhibitors and other non-electrochemical methods. Of course, other non-electrochemical methods like chemical analysis and X-ray fluorescence for determining corrosion products in process liquor; acoustic emission with application in the aviation industry; ultrasonic techniques for thickness measurements to detect metal losses caused by corrosion and hydrogen probes for obtaining corrosion rate data have proved very useful in corrosion monitoring. However, computer software studies together with weight or Weight loss measurements are adequate to carry out the analytical work in this research and results are valid with enough merit.

 


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