Sains Malaysiana 52(11)(2023): 3189-3209

http://doi.org/10.17576/jsm-2023-5211-13

Adsorption of Diclofenac from Aqueous Solution by Amine-Functionalized Poly(Acrylonitrile-Co-Acrylic Acid) Microparticles Adsorbent

(Penjerapan Diklofenak daripada Larutan Berair oleh Penjerap Mikrozarah Berfungsi Amine (Acrylonitrile-Ko-Acrylic Acid))

ZAKIRA AMALIN MOHAMAD¹, SITI NURUL AIN MD JAMIL^1,2,*, NUR NIDA SYAMIMI SUBRI¹, FARHANA SYAKIRAH ISMAIL¹ & RUSLI DAIK^3,4

¹Department of Chemistry, Faculty of Science, Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia

²Centre for Foundation Studies in Science of Universiti Putra Malaysia, 43400 UPM Serdang, Selangor, Malaysia

³Department of Chemical Sciences, Faculty of Science and Technology, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor, Malaysia

⁴Institute of Microengineering and Nanoelectronics, Universiti Kebangsaan Malaysia, 43600 UKM Bangi, Selangor, Malaysia

Diserahkan: 28 Julai 2023/Diterima: 25 Oktober 2023

Abstract

In this study, the synthesis of poly(acrylonitrile) (PAN) and poly(acrylonitrile-co-acrylic acid) (poly(ACN-co-AAc)) was carried out via redox polymerization, using sodium bisulphate (SBS) and potassium persulphate (KPS) as initiators. Subsequently, the resulting poly(ACN-co-AAc) was functionalized with ethanolamine (ETA) and ethylenediamine (EDA) to utilize as adsorbents for the removal of diclofenac from an aqueous solution. Both unfunctionalized and functionalized poly(ACN-co-AAc) were characterized using Fourier-Transform Infrared (FTIR) spectroscopy, Scanning Electron Microscope (SEM), Thermogravimetric Analysis (TGA), and Brunauer-Emmett-Teller (BET) analysis. The effects of pH, initial concentration of diclofenac solution, contact time, and adsorbent dosage were investigated during the adsorption process. The isotherm data were best fitted by the Langmuir model, indicating a mono-layered adsorption mechanism. The maximum adsorption capacities obtained from the Langmuir equation were higher for ETA-functionalized poly(ACN-co-AAc) at 120.5 mg/g, as compared to EDA-functionalized poly(ACN-co-AAc) at 80.6 mg/g. The experimental kinetic results showed that the pseudo-second-order model was a good fit for describing the adsorption rate of diclofenac for both ETA-functionalized poly(ACN-co-AAc) and EDA-functionalized poly(ACN-co-AAc), with R² values of 0.9930 and 0.9906, respectively. This suggests that the chemisorption process is more favourable for the adsorption of diclofenac when using both types of adsorbents.

Keywords: Diclofenac; ethanolamine-functionalized poly(ACN-co-AAc); ethylenediamine- functionalized poly(ACN-co-AAc); isotherm; kinetic; poly(acrylonitrile-co-acrylic acid)

Abstrak

Dalam kajian ini, sintesis poli(akrilonitril) (PAN) dan poli(akrilonitril-ko-asid akrilik) (poli(ACN-ko-AAc)) telah dijalankan melalui pempolimeran redoks dengan menggunakan natrium bisulfat (SBS) dan kalium persulfat (KPS) sebagai pemula. Kemudian, poli(ACN-ko-AAc) yang terhasil telah difungsikan dengan etanolamina (ETA) dan etilendiamina (EDA) untuk digunakan sebagai penjerap bagi penyingkiran diklofenak daripada larutan akueus. Sifat poli (ACN-ko-AAc) yang tidak difungsikan dan yang telah difungsikan telah dikaji menggunakan spektroskopi inframerah transformasi Fourier (FTIR), Mikroskop Elektron Imbasan (SEM), Analisis Termogravimetrik (TGA) dan analisis Brunauer-Emmett-Teller (BET). Semasa proses penjerapan, kami telah mengkaji kesan pH, kepekatan awal larutan diklofenak, masa sentuhan dan dos penjerap. Data isoterma paling sesuai dengan model Langmuir yang menunjukkan mekanisme penjerapan berlapis tunggal. Kapasiti penjerapan maksimum yang diperoleh daripada persamaan Langmuir lebih tinggi untuk poli(ACN-ko-AAc) yang telah difungsikan dengan ETA, iaitu 120.5 mg/g, berbanding dengan poli(ACN-ko-AAc) yang telah difungsikan dengan EDA, iaitu 80.6 mg/g. Selain itu, hasil kinetik uji kaji kami menunjukkan bahawa model pseudo-tertib-kedua berkesan untuk menggambarkan kadar penjerapan diklofenak menggunakan kedua-dua jenis penjerap, iaitu poli(ACN-ko-AAc) yang telah difungsikan dengan ETA dan EDA, dengan nilai R² masing-masing sebanyak 0.9930 dan 0.9906. Ini menunjukkan bahawa proses kimia penjerapan lebih baik untuk penjerapan diklofenak apabila menggunakan kedua-dua jenis penjerap ini.

Kata kunci: Diklofenak; EDA-difungsikan poli(ACN-ko-AAc); ETA-difungsikan poli(ACN-ko-AAc); isoterma; kinetik; poli(ACN-ko-AAc)

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*Pengarang untuk surat-menyurat; email: ctnurulain@upm.edu.my