Corrosion inhibition pre-screening of Nitrobenzaldehyde Meldrum’s acid using response surface methodology (RSM) and Pearson correlation analysis
-
Muhammad Azhan Arif Mansor
, Nur Aiman Najwa Kamarul Baharin, Sheikh Ahmad Izaddin Sheikh Mohd Ghazali
, Nurul Auni Zainal Abidin
, Tuan Norhafizah Tuan Zakaria
and Nur Nadia Dzulkifli
Abstract
Corrosion inhibitors are chemical agents that, even at low concentration, markedly mitigate the rate of metal degradation in acidic media. The objective of this study is to screen and evaluate the corrosion inhibition of Nitrobenzaldehyde Meldrum’s Acid (NitroMA) in HCl medium. The NitroMA compound was successfully synthesized through a condensation method and characterized using ATR-FTIR, NMR, and elemental analysis. Weight loss measures revealed that the corrosion inhibition efficiency of NitroMA increases with its concentration in 1 M HCl concentration. The inhibition efficiency of NitroMA was as high as 80.94 % at 5 mM in 1 M HCl. The alignment with Langmuir and Frumkin models indicates that inhibition efficiency arises from a combination of monolayer adsorption and intermolecular attraction across different surface regions, which may lead to more stable and compact monolayers on the metal surface as confirmed by the SEM-EDX analysis. Both Langmuir and Frumkin isotherms fitted the data with high correlation coefficients (R2 > 0.999). The Langmuir model yielded a Gibbs free energy of adsorption around (−21.1 kJ mol−1), suggesting a borderline case between physisorption and chemisorption. In contrast, the Frumkin model gave a lower value (−9.11 kJ mol−1), consistent with physisorption. The variation arises because Langmuir assumes a homogeneous surface with no adsorbate–adsorbate interaction, while Frumkin accounts for lateral interactions. Therefore, the compound primarily undergoes physisorption, but the Langmuir result also indicates possible contribution of weak chemisorption. Following this, NitroMA was screened using Response Surface Methodology (RSM) with two-factors analysis, incorporating temperature, acid concentration, inhibitor concentration, time, and ratio of volume acid and inhibitor as the parameters. The developed RSM model demonstrated a good fit, as reflected by the statistical parameters: R2 = 0.8962, Adjusted R2 = 0.8851, and Predicted R2 = 0.8644, indicating high reliability and predictive accuracy. The results showed that temperature, time, and acid concentration significantly influence the inhibition efficiency. These findings were validated by computational analysis using the Pearson correlation analysis, which demonstrated that temperature, acid concentration, and time are the most strongly linked to parameters with inhibition efficiency.
Acknowledgements
The authors would like to express their gratitude to the Faculty of Applied Sciences, Universiti Teknologi MARA (UiTM), Negeri Sembilan Branch, for providing the research facilities.
-
Research ethics: Not applicable.
-
Informed consent: Not applicable.
-
Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission. M.A.A. Mansor: Writing – Original draft, Formal analysis. N.A.N. Kamarul Baharin: Formal analysis. S.A.I. Sheikh Mohd Ghazali: Review & Editing. N.A. Zainal Abidin: Formal analysis, Methodology, Review & Editing. T.N. Tuan Zakaria: Formal analysis, Review & Editing. N.N. Dzulkifli: Conceptualization, Supervision, Methodology, Writing – Review & Editing.
-
Use of Large Language Models, AI and Machine Learning Tools: Premium Quillbot licensed by Universiti Teknologi MARA was used to improvise the clarity of language throughout the manuscript.
-
Conflict of interest: Not applicable.
-
Research funding: None.
-
Data availability: None.
References
1. Winston Revie, R. Uhlig’s Corrosion Handbook; Wiley eBooks: Hoboken, New Jersey, 2011.10.1002/9780470872864Search in Google Scholar
2. Schweitzer, P. A. Fundamentals of Metallic Corrosion; CRC Press eBooks: Boca Raton, Florida, 2006.10.1201/9780849382444Search in Google Scholar
3. Ahmad, Z. Principles of Corrosion Engineering and Corrosion Control; Butterworth-Heinemann/IChemE Series: USA, 2006.10.1016/B978-075065924-6/50004-0Search in Google Scholar
4. Sastri, V. S. Corrosion Inhibitors: Principles and Applications; Wiley: New York, 1998.Search in Google Scholar
5. Jones, D. A. Principles and Prevention of Corrosion, 2nd ed.; Prentice Hall: USA, 1995.Search in Google Scholar
6. Fontana, M. G. Corrosion Engineering; McGraw-Hill: United States, 1987.Search in Google Scholar
7. Quraishi, M.; Sardar, R.; Jamal, D. Corrosion Inhibition of Mild Steel in Hydrochloric Acid by Some Aromatic Hydrazides. Mater. Chem. Phys. 2001, 71 (3), 309–313. https://doi.org/10.1016/s0254-0584(01)00295-4.Search in Google Scholar
8. Popova, A.; Sokolova, E.; Raicheva, S.; Christov, M. AC and DC Study of the Temperature Effect on Mild Steel Corrosion in Acid Media in the Presence of Benzimidazole Derivatives. Corros. Sci. 2003, 45 (1), 33–58. https://doi.org/10.1016/S0010-938X(02)00072-0.Search in Google Scholar
9. Ebenso, E. E.; Oguzie, E. E. Corrosion Inhibition of Mild Steel in Acidic Media by Some Organic Dyes. Mater. Lett. 2005, 59 (17), 2163–2165. https://doi.org/10.1016/j.matlet.2005.02.055.Search in Google Scholar
10. Verma, C.; Ebenso, E. E.; Quraishi, M. A. Corrosion Inhibitors for Ferrous and Non-ferrous Metals and Alloys in Ionic Sodium Chloride Solutions: a Review. J. Mol. Liq. 2017, 248, 927–942. https://doi.org/10.1016/j.molliq.2017.10.094.Search in Google Scholar
11. Obot, I. B.; Obi-Egbedi, N. O. Adsorption Properties and Inhibition of Mild Steel Corrosion in Sulphuric Acid Solution by Ketoconazole: Experimental and Theoretical Investigation. Corros. Sci. 2009, 52 (1), 198–204. https://doi.org/10.1016/j.corsci.2009.09.002.Search in Google Scholar
12. Ferreira, E. S.; Giacomelli, C.; Giacomelli, F. C.; Spinelli, A. Evaluation of the Inhibitor Effect of l-ascorbic Acid on the Corrosion of Mild Steel. Mater. Chem. Phys. 2003, 83 (1), 129–134. https://doi.org/10.1016/j.matchemphys.2003.09.020.Search in Google Scholar
13. Miralrio, A.; Espinoza Vázquez, A. Plant Extracts as Green Corrosion Inhibitors for Different Metal Surfaces and Corrosive Media: a Review. Processes 2020, 8 (8), 942. https://doi.org/10.3390/pr8080942.Search in Google Scholar
14. Abdel-Gaber, A. M.; Khamis, E.; Abo-ElDahab, H.; Adeel, Sh. Inhibition of Aluminium Corrosion in Alkaline Solutions Using Natural Compound. Mater. Chem. Phys. 2008, 109 (2–3), 297–305. https://doi.org/10.1016/j.matchemphys.2007.11.038.Search in Google Scholar
15. Shaabani, A.; Samadi, S.; Rahmati, A. One‐Pot, Three‐Component Condensation Reaction in Water: an Efficient and Improved Procedure for the Synthesis of Pyran Annulated Heterocyclic Systems. Synth. Commun. 2007, 37 (3), 491–499. https://doi.org/10.1080/00397910601039242.Search in Google Scholar
16. Kamarul Baharin, N. A. N.; Sheikh Mohd Ghazali, S. A. I.; Sirat, S. S.; Mohd Tajuddin, A.; Pungot, N. H.; Normaya, E.; Mohd Kamarudin, S. R.; Dzulkifli, N. N. In-depth Investigation of Corrosion Inhibition Mechanism: Computational, Electrochemical, and Theoretical Studies of Vanillin Meldrum’s Acid on Mild Steel Surface in 1 M Hcl. J. Mol. Liq. 2024, 416, 126390. https://doi.org/10.1016/j.molliq.2024.126390.Search in Google Scholar
17. Mansor, M. A. A.; Zainal Abidin, N. A.; Yasin, Y.; Sheikh Mohd Ghazali, S. A. I.; Dzulkifli, N. N. Optimisation of the Corrosion Inhibition Performance of Isatin 4-ethyl-3-thiosemicarbazone for Mild Steel in Sulfuric Acid Medium Using Response Surface Methodology. Chem. Pap. 2024, 78 (13), 7409–7422. https://doi.org/10.1007/s11696-024-03603-2.Search in Google Scholar
18. Montgomery, D. C. Design and Analysis of Experiments, 8th ed.; Wiley: Arizona, United States, 2012.Search in Google Scholar
19. Myers, R. H.; Montgomery, D. C.; Anderson-Cook, C. M. Response Surface Methodology: Process and Product Optimization Using Designed Experiments, 4th ed.; Wiley: New Jersey, 2016.Search in Google Scholar
20. Ahmadi, S.; Khormali, A. Optimization of the Corrosion Inhibition Performance of 2-mercaptobenzothiazole for Carbon Steel in Hcl Media Using Response Surface Methodology. Fuel 2023, 357, 129783. https://doi.org/10.1016/j.fuel.2023.129783.Search in Google Scholar
21. Noor, E. A. Temperature Effects on the Corrosion Inhibition of Mild Steel in Acidic Solutions by Aqueous Extract of Fenugreek Leaves. Int. J. Electrochem. Sci. 2007, 2 (12), 996–1017. https://doi.org/10.1016/s1452-3981(23)17129-x.Search in Google Scholar
22. Singh, A.; Ebenso, E. E.; Quraishi, M. A. Corrosion Inhibition of Carbon Steel in HCL Solution by Some Plant Extracts. Int. J. Corros. 2012, 1–20. https://doi.org/10.1155/2012/897430.Search in Google Scholar
23. Singh, D. D. N.; Singh, M. M.; Chaudhary, R. S.; Agarwal, C. V. Inhibition and Polarization Studies of Some Substituted Urea Compounds for Corrosion of Aluminium in Nitric Acid. Electrochim. Acta 1981, 26 (8), 1051–1056. https://doi.org/10.1016/0013-4686(81)85076-1.Search in Google Scholar
24. Khaled, K. F. Application of Electrochemical Frequency Modulation for Monitoring Corrosion and Corrosion Inhibition of Iron by Some Indole Derivatives in Molar Hydrochloric Acid. Mater. Chem. Phys. 2008, 112 (1), 290–300. https://doi.org/10.1016/j.matchemphys.2008.05.056.Search in Google Scholar
25. Dong, Z.; Ding, L.; Meng, Z.; Xu, K.; Mao, Y.; Chen, X.; Ye, H.; Poursaee, A. Machine Learning-based Corrosion Rate Prediction of Steel Embedded in Soil. Sci. Rep. 2024, 14, 18194. https://doi.org/10.1038/s41598-024-68562-w.Search in Google Scholar PubMed PubMed Central
26. Deprez, M.; Robinson, E. C. Machine Learning for Biomedical Applicationsw with Scikit-Learn and Pytorch; Academic Press: London, 2022.Search in Google Scholar
27. Nettleton, D. Selection of Variables and Factor Derivation; Elsevier eBooks: Burlington, Massachusetts, 2014; pp 79–104.10.1016/B978-0-12-416602-8.00006-6Search in Google Scholar
28. Malaret, F. Semi-Quantitative Categorization Method for the Corrosion Behavior of Metals Based on Immersion Test. Metals 2024, 14 (4), 409. https://doi.org/10.3390/met14040409.Search in Google Scholar
29. Shwetha, K. M.; Praveen, B. M.; Devendra, B. K. A Review on Corrosion Inhibitors: Types, Mechanisms, Electrochemical Analysis, Corrosion Rate and Efficiency of Corrosion Inhibitors on Mild Steel in an Acidic Environment. Results Surf. Interfaces 2024, 16, 100258. https://doi.org/10.1016/j.rsurfi.2024.100258.Search in Google Scholar
30. Rudolf, P.; Buback, J.; Aulbach, J.; Nuernberger, P.; Brixner, T. Ultrafast Multisequential Photochemistry of 5-Diazo Meldrum’s Acid. J. Am. Chem. Soc. 2010, 132 (43), 15213–15222. https://doi.org/10.1021/ja1025529.Search in Google Scholar PubMed
31. Idelfitri, N. I. F.; Dzulkifli, N. N.; Ash’ari, N. A. N.; Sapari, S.; Abdul Razak, F. I.; Pungot, N. H. Synthesis, Characterisation and Corrosion Inhibitory Study of Meldrum’s Acid Thiosemicarbazone: Weight Loss, SEM-EDX and DFT. Inorg. Chem. Commun. 2023, 150, 110485. https://doi.org/10.1016/j.inoche.2023.110485.Search in Google Scholar
32. Pesyan, N. N.; Gharib, A.; Behroozi, M.; Shokr, A. New full-substituted Cyclopropanes Derived from the one-pot Reaction of Meldrum’s Acid with Aldehydes and BrCN in the Presence of Et3N. Arab. J. Chem. 2013, 10, S1558–S1566. https://doi.org/10.1016/j.arabjc.2013.05.024.Search in Google Scholar
33. Al-Amiery, A. A.; Isahak, W. N. R. W.; Al-Azzawi, W. K. Corrosion Inhibitors: Natural and Synthetic Organic Inhibitors. Lubricants 2023, 11 (4), 174. https://doi.org/10.3390/lubricants11040174.Search in Google Scholar
34. Veza, I.; Spraggon, M.; Fattah, I. M. R.; Idris, M. Response Surface Methodology (RSM) for Optimizing Engine Performance and Emissions Fueled with Biofuel: Review of RSM for Sustainability Energy Transition. Results Eng. 2023, 18, 101213. https://doi.org/10.1016/j.rineng.2023.101213.Search in Google Scholar
35. Zheng, X.; Zhang, S.; Gong, M.; Li, W. Experimental and Theoretical Study on the Corrosion Inhibition of Mild Steel by 1-Octyl-3-methylimidazolium L-Prolinate in Sulfuric Acid Solution. Ind. Eng. Chem. Res. 2014, 53 (42), 16349–16358. https://doi.org/10.1021/ie502578q.Search in Google Scholar
36. Wang, B.; Du, M.; Zhang, J.; Li, C.; Liu, J.; Liu, H.; Li, R.; Li, Z. Corrosion Inhibition of Mild Steel by the Hydrolysate of an Imidazoline-based Inhibitor in CO2-saturated Solution. RSC Adv. 2019, 9 (63), 36546–36557. https://doi.org/10.1039/c9ra05322k.Search in Google Scholar PubMed PubMed Central
37. Bijapur, K.; Molahalli, V.; Shetty, A.; Toghan, A.; De Padova, P.; Hegde, G. Recent Trends and Progress in Corrosion Inhibitors and Electrochemical Evaluation. Appl. Sci. 2023, 13 (18), 10107. https://doi.org/10.3390/app131810107.Search in Google Scholar
38. Ibrahimi, B. E.; Nardeli, J. V.; Guo, L. An Overview of Corrosion. ACS Symp. Ser. 2021, 1403, 1–19. https://doi.org/10.1021/bk-2021-1403.ch001.Search in Google Scholar
39. Gómez-Sánchez, G.; Olivares-Xometl, O.; Arellanes-Lozada, P.; Likhanova, N. V.; Lijanova, I. V.; Arriola-Morales, J.; Díaz-Jiménez, V.; López-Rodríguez, J. Temperature Effect on the Corrosion Inhibition of Carbon Steel by Polymeric Ionic Liquids in Acid Medium. Int. J. Mol. Sci. 2023, 24 (7), 6291. https://doi.org/10.3390/ijms24076291.Search in Google Scholar PubMed PubMed Central
40. Zinad, D. S.; Hanoon, M.; Salim, R. D.; Ibrahim, S. I.; Al-Amiery, A. A.; Takriff, M. S.; Kadhum, A. A. H. A New Synthesized coumarin-derived Schiff Base as a Corrosion Inhibitor of Mild Steel Surface in HCl Medium: Gravimetric and DFT Studies. Int. J. Corros. Scale Inhib. 2020, 9 (1), 228–243. https://doi.org/10.17675/2305-6894-2020-9-1-14.Search in Google Scholar
© 2025 IUPAC & De Gruyter