Sains Malaysiana 52(3)(2023): 953-966

http://doi.org/10.17576/jsm-2023-5203-19

Green Synthesis of Silver Nanoparticle Decorated on Reduced Graphene Oxide Nanocomposite using Clinacanthus nutans and Its Applications

(Sintesis Hijau Nanozarah Perak Dihiasi pada Nanokomposit Grafin Oksida Terturun menggunakan Clinacanthus nutans dan Penggunaannya)

DHARSHINI PERUMAL¹, CHE AZURAHANIM CHE ABDULLAH^1,2,3*, EMMELLIE LAURA ALBERT³ & RUZNIZA MOHD ZAWAWI⁴

¹Biophysics Laboratory, Department of Physics, Faculty of Science, Universiti Putra

Malaysia, 43400 UPM Serdang, Selangor Darul Ehsan, Malaysia

²UPM-MAKNA Cancer Research Laboratory, Institute of Bioscience, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor Darul Ehsan, Malaysia

³Institute of Nanoscience and Nanotechnology, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor Darul Ehsan, Malaysia

⁴Department of Chemistry, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor Darul Ehsan, Malaysia

Received: 20 September 2022/Accepted: 4 January 2023

Abstract

A straightforward approach that uses Clinacanthus nutans leaf extract as a bio-reduction agent has been reported to anchor silver nanoparticles onto graphene oxide (rGO-Ag). The nanocomposite was characterized by using ultraviolet-visible spectroscopy, Fourier transform infrared spectroscopy, field emission scanning electron microscopy with energy-dispersive X-ray spectroscopy, and X-ray diffraction. A qualitative colour transition from yellowish to dark brown confirmed the biosynthesis of rGO-Ag nanocomposite and showed a surface plasmon resonance at 263 nm and 425 nm. Utilizing cyclic voltammetry, the electrochemical characteristics of the rGO-Ag nanocomposite modified screen printed carbon electrodes were examined. The rGO-Ag nanocomposite electrode enhanced anodic current approximately 1.29 times greater compared to silver nanoparticles (AgNPs) and 1.34 times greater compared to graphene oxide (GO). Moreover, rGO-Ag nanocomposites exhibited excellent antibacterial activity against typical Gram-positive (S. aureus) (11.99 ± 0.26 mm) and Gram-negative (E. coli) (11.86 ± 0.29 mm) bacteria. Toxicity was assayed using brine shrimp Artemia salina. The results of hatching and mortality assay demonstrates that AgNPs and rGO-Ag nanocomposite is biocompatible with A. salina at a low dosage (0.001 mg/mL). This work offers a guide for the future synthesis of nanocomposites using green reductants. The as- synthesized nanocomposite shows a promising component for the development of biomedical devices applications.

Keywords: Electrochemical; green synthesis; reduced graphene oxide; silver nanoparticles; toxicity

Abstrak

Pendekatan ringkas menggunakan ekstrak daun Clinacanthus nutans sebagai agen bio-penurunan telah dilaporkan berjaya melekatkan nanozarah perak pada grafin oksida (rGO-Ag). Spektroskopi ultralembayung, spektroskopi inframerah transformasi Fourier, mikroskop elektron pengimbasan pelepasan medan dengan spektroskopi penyebaran tenaga sinar-X dan spektroskopi pembelauan sinar-X digunakan untuk menghuraikan ciri nanokomposit yang terbentuk. Peralihan warna secara kualitatif daripada kekuningan kepada coklat gelap mengesahkan keberhasilan biosintesis nanokomposit rGO-Ag selain kewujudan resonans plasmon permukaan pada 263 nm dan 425 nm. Dengan menggunakan kitaran voltammetri, ciri elektrokimia bagi skrin bercetak elektrod karbon diubah suai dengan rGO-Ag nanokomposit telah diperiksa. Keputusan menunjukkan bagi nanokomposit rGO-Ag peningkatan arus anod adalah kira-kira 1.29 kali lebih besar berbanding dengan nanozarah perak (AgNPs) dan 1.34 kali lebih besar berbanding dengan grafin oksida (GO). Selain itu, nanokomposit rGO-Ag menunjukkan aktiviti antibakteria yang sangat baik terhadap bakteria Gram-positif (S. aureus) (11.99 ± 0.26 mm) dan Gram-negatif (E. coli) (11.86 ± 0.29 mm). Ketoksikan telah diuji menggunakan udang air garam Artemia salina. Keputusan penetasan dan asai kemortalan menunjukkan bahawa AgNPs dan rGO-Ag nanokomposit adalah bioserasi dengan A. salina pada dos yang rendah (0.001 mg/mL). Kajian ini memberikan panduan dalam sintesis nanokomposit menggunakan kaedah penurunan hijau pada masa akan datang. Nanokomposit yang telah disintesis menunjukkan potensi untuk diguna pakai sebagai komponen dalam bidang aplikasi peranti bioperubatan.

Kata kunci: Elektrokimia; grafin oksida terturun; ketoksikan; nanozarah perak; sintesis hijau

REFERENCES

Abboud, Z., Vivekanandhan, S., Misra, M. & Mohanty, A.K. 2016. Leaf extract mediated biogenic process for the decoration of graphene with silver nanoparticles. Materials Letters 178: 115-119.

Adyani, S.H. & Soleimani, E. 2019. Green synthesis of Ag/Fe₃O₄/RGO nanocomposites by punica granatum peel extract: Catalytic activity for reduction of organic pollutants. International Journal of Hydrogen Energy 44: 2711-2730.

Ahamed, M., Akhtar, M.J., Majeed Khan, M.A. & Alhadlaq, H.A. 2021. A novel green preparation of Ag/Rgo Nanocomposites with highly effective anticancer performance. Polymers 13: 3350.

Ahmad, M.A., Aslam, S., Mustafa, F. & Arshad, U. 2021. Synergistic antibacterial activity of surfactant free Ag–GO nanocomposites. Scientific Reports 11: 1-9.

Ahmad, N., Al-Fatesh, A.S., Wahab, R., Alam, M. & Fakeeha, A.H. 2020. Synthesis of silver nanoparticles decorated on reduced graphene oxide nanosheets and their electrochemical sensing towards hazardous 4-nitrophenol. Journal of Materials Science: Materials in Electronics 31(14): 11927-11937.

Al-Marri, A.H., Khan, M., Khan, M., Adil, S.F., Al-Warthan, A., Alkhathlan, H.Z., Tremel, W., Labis, J.P., Siddiqui, M.R.H. & Tahir, M.N. 2015. Pulicaria glutinosa extract: A toolbox to synthesize highly reduced graphene oxide-silver nanocomposites. International Journal of Molecular Sciences 16(1): 1131-1142.

Allafchian, A., Vahabi, M.R., Hossein Jalali, S.A., Mahdavi, S.S., Sepahvand, S. & Farhang, H.R. 2022. Design of green silver nanoparticles mediated by Ferula ovina Boiss. Extract with enhanced antibacterial effect. Chemical Physics Letters 791: 139392.

Arulvasu, C., Jennifer, S.M., Prabhu, D. & Chandhirasekar, D. 2014. Toxicity effect of silver nanoparticles in brine shrimp Artemia. The Scientific World Journal 2014: Article ID. 256919.

Azemi Ahmad Khusairi, Siti Safiah Mokhtar & Aida Hanum Ghulam Rasool. 2020. Clinacanthus nutans: Its potential against diabetic vascular diseases. Brazilian Journal of Pharmaceutical Sciences 56: e18838.

Bal, M., Tumer, M. & Kose, M. 2022. Synthesis of reduced graphene oxide-based hybrid compounds and investigation of their sensing behavior against some nitroaromatic explosives. Materials Chemistry and Physics 289: 126480.

Basiri, S., Mehdinia, A. & Jabbari, A. 2018. Green synthesis of reduced graphene oxide-Ag nanoparticles as a dual-responsive colorimetric platform for detection of dopamine and Cu²⁺. Sensors and Actuators, B: Chemical 262: 499-507.

Bhangoji, J.C., Sahoo, S., Satpati, A.K. & Shendage, S.S. 2021. Facile and green synthesis of silver nanoparticle-reduced graphene oxide composite and its application as nonenzymatic electrochemical sensor for hydrogen peroxide. Current Chemistry Letters 10: 295-308.

Chinnaraj, S., Palani, V., Yadav, S., Arumugam, M., Sivakumar, M., Maluventhen, V. & Singh, M. 2021. Green synthesis of silver nanoparticle using Goniothalamus wightii on graphene oxide nanocomposite for effective voltammetric determination of metronidazole. Sensing and Bio-Sensing Research 32: 100425.

Dinh, D.A., Hui, K.S., Hui, K.N., Cho, Y.R., Zhou, W., Hong, X. & Chun, H.H. 2014. Green synthesis of high conductivity silver nanoparticle-reduced graphene oxide composite films. Applied Surface Science 298: 62-67.

Dominic, R.M., Punniyakotti, P., Balan, B. & Angaiah, S. 2022. Green synthesis of reduced graphene oxide using plectranthus amboinicus leaf extract and its supercapacitive performance. Bulletin of Materials Science 45: 1-8.

Gómez de Saravia, S.G., Rastelli, S.E., Angulo-Pineda, C., Palza, H. & Viera, M.R. 2020. Anti-adhesion and antibacterial activity of silver nanoparticles and graphene oxide-silver nanoparticle composites. Revista Materia 25(2): 1-9.

Handayani, M., Suwaji, B.I., Asih, G.I.N., Kusumaningsih, T., Kusumastuti, Y., Rochmadi & Anshori, I. 2022. In-situ synthesis of reduced graphene oxide/silver nanoparticles (RGO/AgNPs) nanocomposites for high loading capacity of acetylsalicylic acid. Nanocomposites 8: 74-80.

Herbin, H., Basalius, M., Amalanathan, A.M., Michael Mary, M.S., Maria Lenin, M., Parvathiraja, C., Siddiqui, M.R., Wabaidur, S.M. & Islam, M.A. 2022. Synthesis of silver nanoparticles using Syzygium malaccense fruit extract and evaluation of their catalytic activity and antibacterial properties. Journal of Inorganic and Organometallic Polymers and Materials 32: 1103-1115.

Jarmoshti, J.A., Nikfarjam, A., Hajghassem, H. & Banihashemian, S.M. 2019. Visible light enhancement of ammonia detection using silver nanoparticles decorated on reduced graphene oxide. Materials Science & Engineering B 6: 066306.

Karthik, C., Swathi, N., Pandi Prabha, S. & Caroline, D.G. 2020. Green synthesized RGO-AgNP hybrid nanocomposite - An effective antibacterial adsorbent for photocatalytic removal of DB-14 dye from aqueous solution. Journal of Environmental Chemical Engineering 8(1): 103577.

Khane, Y., Benouis, K., Albukhaty, S., Sulaiman, G.M., Abomughaid, M.M., Al Ali, A., Aouf, D., Fenniche, F., Khane, S., Chaibi, W., Henni, A., Bouras, H.D. & Dizge, N. 2022. Green synthesis of silver nanoparticles using aqueous citrus limon zest extract: Characterization and evaluation of their antioxidant and antimicrobial properties. Nanomaterials 12(12): 2013.

Khorrami, S., Abdollahi, Z., Eshaghi, G., Khosravi, A., Bidram, E. & Zarrabi, A. 2019. An improved method for fabrication of Ag-GO nanocomposite with controlled anti-cancer and anti-bacterial behavior: A comparative study. Scientific Reports 9: 1-10.

Krishnaraj, C., Krishnamoorthi Kaliannagounder, V., Rajan, R., Ramesh, T., Kim, C.S., Park, C.H., Liu, B. & Yun, S.I. 2022. Silver nanoparticles decorated reduced graphene oxide: Eco-friendly synthesis, characterization, biological activities and embryo toxicity studies. Environmental Research 210: 112864.

Lim, V., Chong, H.W., Nozlena Abdul Samad, Siti Aisyah Abd Ghafar, Ida Shazrina Ismail, Rafeezul Mohamed, Yong, Y.K., Gan, C.Y. & Tan, J.J. 2022. Vibrational spectroscopy-based chemometrics analysis of Clinacanthus nutans extracts after postharvest processing and extract effects on cardiac C-Kit cells. Evidence-Based Complementary and Alternative Medicine 2022: 1967593.

Mahendran, N., Anand, B., Rajarajan, M., Muthuvel, A. & Mohana, V. 2021. Green synthesis, characterization and antimicrobial activities of silver nanoparticles using Cissus quadarangularis leaf extract. Materials Today: Proceedings 49: 2620-2623.

Mahmoud, A.E.D., Hosny, M., El-Maghrabi, N. & Fawzy, M. 2022. Facile synthesis of reduced graphene oxide by Tecoma stans extracts for efficient removal of Ni (II) from water: Batch experiments and response surface methodology. Sustainable Environment Research 32: 1-16.

Marcano, D.C., Kosynkin, D.V., Berlin, J.M., Sinitskii, A., Sun, Z., Slesarev, A., Alemany, L.B., Lu, W. & Tour, J.M. 2010. Improved synthesis of graphene oxide. ACS Nano 4(8): 4806-4814.

Mindivan, F. & Göktaş, M. 2020. Rosehip-extract-assisted green synthesis and characterization of reduced graphene oxide. ChemistrySelect 5(29): 8980-8985.

Minh, P.N., Hoang, V.T., Dinh, N.X., Hoang, O.V., Cuong, N.V., Hop, D.T.B., Tuan, T.Q., Khi, N.T., Huy, T.Q. & Le, A.T. 2020. Reduced graphene oxide-wrapped silver nanoparticles for applications in ultrasensitive colorimetric detection of Cr(vi) ions and the carbaryl pesticide. New Journal of Chemistry 44(18): 7611-7620.

Noor Hashim, Noor Haslinda, Amatul Hamizah Ali, Alfi Khatib & Jalifah Latip. 2019. Discrimination of Clinacanthus nutans extracts and correlation with antiplasmodial activity using ATR-FTIR fingerprinting. Vibrational Spectroscopy 104: 102966.

Nunes, B.S., Carvalho, F.D., Guilhermino, L.M. & Van Stappen, G. 2006. Use of the genus artemia in ecotoxicity testing. Environmental Pollution 144: 453-462.

Olorunkosebi, A.A., Eleruja, M.A., Adedeji, A.V., Olofinjana, B., Fasakin, O., Omotoso, E., Oyedotun, K.O., Ajayi, E.O.B. & Manyala, N. 2021. Optimization of graphene oxide through various hummers’ methods and comparative reduction using green approach. Diamond and Related Materials 117: 108456.

Ooi Swee Hong, Nur Mazidah Noor Mohamed, Ravi Kumar Kalaichelvam, Vuanghao Lim, & Ida Shazrina Ismail. 2021. Effects of Clinacanthus nutans extracts on cytokine secretion in PMA-induced U937 macrophage cells. Research Journal of Pharmacognosy 8: 27-35.

Parthipan, P., Cheng, L., Rajasekar, A., Govarthanan, M. & Subramania, A. 2021. Biologically reduced graphene oxide as a green and easily available photocatalyst for degradation of organic dyes. Environmental Research 196: 110983.

Pumera, M. 2010. Graphene-based nanomaterials and their electrochemistry. Chemical Society Reviews 39: 4146-4157.

Qu, F., Lu, H., Yang, M. & Deng, C. 2011. Electrochemical immunosensor based on electron transfer mediated by graphene oxide initiated silver enhancement. Biosensors and Bioelectronics 26: 4810-4814.

Rai, S., Bhujel, R., Biswas, J. & Swain, B.P. 2021. Biocompatible synthesis of RGO from ginger extract as a green reducing agent and its supercapacitor application. Bulletin of Materials Science 44: 1-11.

Rajeswari, R., Gurumallesh Prabu, H. & Amutha, M. 2017. One pot hydrothermal synthesis characterizations of silver nanoparticles on reduced graphene oxide for its enhanced antibacterial and antioxidant properties. IOSR Journal of Applied Chemistry 10: 64-69.

Rekulapally, R., Murthy Chavali, L.N., Idris, M.M. & Singh, S. 2019. Toxicity of TiO₂ , SiO₂, ZnO, CuO, Au and Ag engineered nanoparticles on hatching and early Nauplii of Artemia sp. PeerJ 6: e6138.

Rodríguez-González, C., Velázquez-Villalba, P., Salas, P. & Castaño, V.M. 2016. Green synthesis of nanosilver-decorated graphene oxide sheets. IET Nanobiotechnology 10: 301-307.

Rudrappa, M., Rudayni, H.A., Assiri, R.A., Bepari, A., Basavarajappa, D.S., Nagaraja, S.K., Chakraborty, B., Swamy, P.S., Agadi, S.N., Niazi, S.K. & Nayaka, S. 2022. Plumeria alba-Mediated green synthesis of silver nanoparticles exhibits antimicrobial effect and anti-oncogenic activity against glioblastoma U118 MG cancer cell line. Nanomaterials (Basel) 12(3): 493.

Ruiz, O.N., Shiral Fernando, K.A., Wang, B., Brown, N.A., Luo, P.G., McNamara, N.D., Vangsness, M., Sun, Y.P. & Bunker, C.E. 2011. Graphene oxide: A nonspecific enhancer of cellular growth. ACS Nano 5: 8100-8107.

Siti Nur Aishah Mat Yusuf, Che Nurul Azieyan Che Mood, Nor Hazwani Ahmad, Doblin Sandai, Chee Keong Lee & Vuanghao Lim. 2020. Optimization of biogenic synthesis of silver nanoparticles from flavonoid-rich Clinacanthus nutans leaf and stem aqueous extracts: Biogenic synthesis of C. nutans AgNPs. Royal Society Open Science 7: 200065.

Soleymani, A.R., Rafigh, S.M. & Hekmati, M. 2020. Green synthesis of RGO/Ag: As evidence for the production of uniform mono-dispersed nanospheres using microfluidization. Applied Surface Science 518: 146264.

Tran, H.V., Nguyen, N.D., Tran, C.T.Q., Tran, L.T., Le, T.D., Tran, H.T.T., Piro, B., Huynh, C.D., Nguyen, T.N., Nguyen, N.T.T., Dang, H.T.M., Nguyen, H.L., Tran, L.D. & Phan, N.T. 2020. Silver nanoparticles-decorated reduced graphene oxide: A novel peroxidase-like activity nanomaterial for development of a colorimetric glucose biosensor. Arabian Journal of Chemistry 13(7): 6084-6091.

Vu, Q.K., Nguyen, T.H., Le, A.T., Vu, N.P., Ngo, X.D., Nguyen, T.K., Nguyen, T.T., Pham, C.V., Nguyen, T.L., Dang, T.L.T., Tonezzer, M. & Tran, Q.H. 2022. Enhancing electron transfer and stability of screen-printed carbon electrodes modified with AgNP-reduced graphene oxide nanocomposite. Journal of Electronic Materials 51: 1004-1012.

Yang, J., Xia, X., He, K., Zhang, M., Qin, S., Luo, M. & Wu, L. 2021. Green synthesis of reduced graphene oxide (RGO) using the plant extract of Salvia spinosa and evaluation of photothermal effect on pancreatic cancer cells. Journal of Molecular Structure 1245: 131064.

Yu, F., Ma, J., Qi, Y., Song, H., Tan, G., Huang, F. & Yang, M. 2022. Geographical traceability of Clinacanthus Nutans with near-infrared pectroscopy and chemometrics. American Journal of Analytical Chemistry 13: 63-77.

Zhu, S., Luo, F., Chen, W., Zhu, B. & Wang, G. 2017. Toxicity evaluation of graphene oxide on cysts and three larval stages of Artemia salina. Science of the Total Environment 595: 101-109.

^*Corresponding author; email: azurahanim@upm.edu.my