Eco-friendly synthesis of surface grafted Carbon nanotubes from sugarcane cubes for development of prolonged release drug delivery platform

Document Type : Reasearch Paper

Authors

• Rahul Narkhede ¹
• Mahesh More ²
• Swapnil Patil ¹
• Pravin Patil ³
• Ashwini Patil ⁴
• Prashant Deshmukh ⁵

¹ Post Graduate Department of Pharmaceutics, H. R. Patel Institute of Pharmaceutical Education and Research, Shirpur, Dhule -425405 (M. S.), India.

² Department of Pharmaceutics, Sanjivani College of Pharmaceutical Education and Research, Kopargaon, Dist – Ahemadnagar - 423 603 (M.S.) India.

³ Department of Pharmaceutical Chemistry, H. R. Patel Institute of Pharmaceutical Education and Research, Shirpur, Dhule -425405 (M. S.), India.

⁴ Department of Microbiology and Biotechnology, R.C.Patel Arts, Science, and Commerce College, Shirpur, Dhule -425405 (M. S.) India.

⁵ Department of Pharmaceutics, Dr. Rajendra Gode College of Pharmacy, Malkapur, Dist – Buldhana – 443 101 (M.S.), India.

10.22034/ijnd.2021.681077

Abstract

Surface grafting of nanocarriers could modulate their properties and characteristics. As carbon nanotubes synthesis is a very tricky process and requires high-end methods, hence the present investigation was aimed to develop an eco-friendly method for synthesis carbon nanotubes (CNTs) and subsequent surface grafting for enhanced drug delivery application. The present study elaborates two-step chemical modifications; wherein the first step is catalytic cleavage of natural precursor in the presence of ferrocene and the second step involve chemical grafting of Acyclovir (ACV) as a model drug to understand the drug release behaviour. The catalytic cleavage of sugarcane cubes (natural precursor) was carried out in a closed copper tube, which prevents oxidation and results in a conversion of tubular nanostructures to amorphous carbon. The covalent attachment of ACV on purified CNTs (fCNTs) was done using carbodiimide chemistry. The preliminary Uv-Vis absorbance spectra defined at 260 nm was arised due to π-π* stacking of aromatic C-C bonds. The Fourier Transforms Infrared Spectroscopy (FTIR) indicated the hydroxyl stretch at 3300 cm^-1 while amide I bond formation was observed at 1672 cm^-1. The XRD spectra confirmed successful synthesis of CNTs. The calculated average crystallite size (Scherer equation) of synthesized CNTs was found to be 42.84 and 44.45 nm; it was also in accordance with the morphological observation as confirmed simultaneously using SEM analysis. The covalently attached ACV was released up to 80% during 8h of in vitro drug release study. The surface grafting potential of CNTs was found to be promising compared to other nanomaterials.

Keywords

• Acyclovir
• Amorphous Carbon
• Carbodiimide Chemistry
• Natural Precursor
• Purification

20.1001.1.20088868.2021.12.3.3.2

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References

[1]           Iijima S., (1991), Helical microtubules of graphitic carbon. Nature. 354: 356-364.

[2]           Hirlekar R., Yamagar M., Garse H., Vij M., Kadam V., (2009), Carbon nanotubes and its applications: A review. Asian J. Pharmac. Clinical Res. 2: 17-27.

[3]           Fathy N. A., Basta A. H., Lotfy V. F., (2020), Novel trends for synthesis of carbon nanostructures from agricultural wastes. Carbon Nanomater. Agri-Food Environm. Appl. (Micro and Nano Technol.). 59-74.

[4]           Szabó A., Perri C., Csató A., Giordano G., Vuono D., Nagy J. B., (2010), Synthesis methods of carbon nanotubes and related materials. Materials. 3: 3092-3140.

[5]           Fathy N. A. (2017), Carbon nanotubes synthesis using carbonization of pretreated rice straw through chemical vapor deposition of camphor. RSC. Adv. 7: 28535-28541.

[6]           Janas D., (2020), From bio to nano: A review of sustainable methods of synthesis of carbon nanotubes. Sustainability. 12: 4115-41131.

[7]           Vivekanandhan S., Schreiber M., Muthuramkumar S., Misra M., Mohanty A. K., (2017), Carbon nanotubes from renewable feedstocks: A move toward sustainable nanofabrication. J. Appl. Polym. Sci. 134: 44255-44262.

[8]           Suriani A., Dalila A., Mohamed A., Mamat M., Salina M., Rosmi M., Rosly K., Roslan M. N., Rusop M., (2013), Vertically aligned carbon nanotubes synthesized from waste chicken fat. Mater. Lett. 101: 61-64.

[9]           Garmaroudi F., Vahdati R., (2010), Functionalized CNTs for delivery of therapeutics. Int. J. Nano Dimens. 1: 89-102.

[10]         More M., Ganguly P., Pandey A., Dandekar P., Jain R., Patil P., Deshmukh P. K., (2017), Development of surface engineered mesoporous alumina nanoparticles: Drug release aspects and cytotoxicity assessment. IET Nanobiotechnol. 11: 661-668.

[11]         More M. P., Deshmukh P. K., (2020), Development of amine-functionalized superparamagnetic iron oxide nanoparticles anchored graphene nanosheets as a possible theranostic agent in cancer metastasis. Drug. Deliv. Transl. Re. 2020: 1-16.

[12]         More M. P., Chitalkar R. V., Bhadane M. S., Dhole S. D., Patil A. G., Patil P. O.,  Deshmukh P. K., (2019), Development of graphene-drug nanoparticle based supramolecular self assembled pH sensitive hydrogel as potential carrier for targeting MDR tuberculosis. Mater. Technol. 34: 324-335.

[13]         Shirazi Y., Tofighy M. A., Mohammadi T., Pak A., (2011), Effects of different carbon precursors on synthesis of multiwall carbon nanotubes: Purification and functionalization. Appl. Surf. Sci. 257: 7359-7367.

[14]         Naderi A., Abdi Tahne B., (2017), Band bending engineering in pin gate all around Carbon nanotube field effect transistors by multi-segment gate. Int. J. Nano Dimens. 8: 341-350.

[15]         Qureshi D., Nadikoppula A., Mohanty B., Anis A., Cerqueira M., Varshney M., Pal K., (2021), Effect of carboxylated carbon nanotubes on physicochemical and drug release properties of oleogels. Colloid. Surf. A. 610: 125695-125701.

[16]         He H., Pham-Huy L. A., Dramou P., Xiao D., Zuo P., Pham-Huy C., (2013), Carbon nanotubes: Applications in pharmacy and medicine. Biomed. Res. Int. 2013: 12-19.

[17]         Heidarian M., Khazaei A., Saien J., (2021), Grafting drugs to functionalized single-wall carbon nanotubes as a potential method for drug delivery. Phys. Chem. Res. 9: 57-68.

[18]         Kang Z., Wang E., Mao B., Su Z., Chen L., Xu L., (2005), Obtaining carbon nanotubes from grass. Nanotechnol. 16: 1192-1197.

[19]         Rance G. A., Marsh D. H., Nicholas R. J., Khlobystov A. N., (2010), UV–vis absorption spectroscopy of carbon nanotubes: Relationship between the π-electron plasmon and nanotube diameter. Chem. Phys. Lett.  493: 19-23.

[20]         Tavares G. D., Ishikawa G. M., Monteiro T. F., Zanolini C., Kedor-Hackmann É. R. M., Bou-Chacra N. A., Consiglieri V. O., (2012), Derivative spectrophotometric method for determination of acyclovir in polymeric nanoparticles. Quím. Nova. 35: 203-206..

[21]         Stobinski L., Lesiak B., Kövér L., Tóth J., Biniak S., Trykowski G., Judek J., (2010), Multiwall carbon nanotubes purification and oxidation by nitric acid studied by the FTIR and electron spectroscopy methods. J. Alloy. Compd. 501: 77-84.

[22]         Patterson A., (1939), The scherrer formula for X-ray particle size determination. Phys. Rev. 56: 978-983.

[23]         Yang M.-H., Jong S.-B., Lu C.-Y., Lin Y.-F., Chiang P.-W., Tyan Y.-C., Chung T.-W., (2012), Assessing the responses of cellular proteins induced by hyaluronic acid-modified surfaces utilizing a mass spectrometry-based profiling system: Over-expression of CD36, CD44, CDK9, and PP2A. Analyst. 137: 4921-4933.

[24]         Shoukat H., Pervaiz F., Noreen S., Nawaz M., Qaiser R., Anwar M., (2020), Fabrication and evaluation studies of novel polyvinylpyrrolidone and 2-acrylamido-2-methylpropane sulphonic acid-based crosslinked matrices for controlled release of acyclovir. Polym. Bull. 77: 1869-1891.

[25]         Karolewicz B., Nartowski K., Pluta J., Górniak A., (2016), Physicochemical characterization and dissolution studies of acyclovir solid dispersions with Pluronic F127 prepared by the kneading method. Acta Pharmaceut. 66: 119-128.

[26]         Mahmood A., Ahmad M., Sarfraz R. M., Minhas M. U., Yaqoob A., (2016), Formulation and in vitro evaluation of acyclovir loaded polymeric microparticles: A solubility enhancement study. Acta Pol. Pharm. 73: 1311-1324.

[27]         Li Z., Luo G., Zhou W., Wei F., Xiang R., Liu Y., (2006), The quantitative characterization of the concentration and dispersion of multi-walled carbon nanotubes in suspension by spectrophotometry. Nanotechnol. 17: 3692-3696.

[28]         Yano T., Ichimura T., Kuwahara S., H’Dhili F., Uetsuki K., Okuno Y., Verma P., Kwata S., (2013), Tip-enhanced nano-raman analytical imaging of locally induced strain distribution in carbon nanotubes. Nat. Commun. 4: 2592-2596.

[29]         Cuesta A., Dhamelincourt P., Laureyns J., Martinez-Alonso A., Tascón J. D., (1994), Raman microprobe studies on carbon materials. Carbon. 32: 1523-1532.

[30]         Heise H., Kuckuk R., Ojha A., Srivastava A., Srivastava V., Asthana B., (2009), Characterisation of carbonaceous materials using Raman spectroscopy: A comparison of carbon nanotube filters, single and multi walled nanotubes, graphitised porous carbon and graphite. J. Raman Spectrosc. 40: 344-353.

[31]         Asokan V., Myrseth V., Kosinski P., (2015), Effect of Pt and Fe catalysts in the transformation of carbon black into carbon nanotubes. J. Phys. Chem. Solids. 81: 106-115.

[32]         Zhao X., Ando Y., Qin L.-C., Kataura H., Maniwa Y., Saito R., (2002), Radial breathing modes of multiwalled carbon nanotubes. Chem. Phys. Lett. 361: 169-174.

[33]         Allaedini G., Tasirin S. M., Aminayi P., Yaakob Z., Meor Talib M. Z., (2016), Carbon nanotubes via different catalysts and the important factors that affect their production: A review on catalyst preferences. Int. J  Nano Dimens. 7: 186-200.

[34]         Farahani B. V., Behbahani G. R., Javadi N., (2016), Functionalized multi walled carbon nanotubes as a carrier for doxorubicin: Drug adsorption study and statistical optimization of drug loading by factorial design methodology. J. Brazil. Chem. Soc. 27: 694-705.

[35]         Ghoshal S., Kushwaha S. K. S., Srivastava M., Tiwari P., (2014), Drug loading and release from functionalized multiwalled carbon nanotubes loaded with 6-mercaptopurine using incipient wetness impregnation method. Am. J. Adv. Drug Deliv. 2: 213-223.