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Mesocellular foam incorporated with copper and iron as catalyst for azo dyes degradation / Nur Azimah Jamalluddin

Mesocellular foam incorporated with copper and iron as catalyst for azo dyes degradation_Nur Azimah Jamalluddin_K4_2016_MYMY
Penggunaan mangkin sokongan berasaskan besi (Fe) di samping hidrogen peroksida (H₂O₂) bagi proses penguraian bahan pewarna organik telah menarik perhatian disebabkan oleh kemampuan mangkin tersebut untuk mencapai kadar penguraian yang tinggi. Walau bagaimanapon, mangkin yang sedia mempunyai beberapa had yang menghalang untuk mencapai kadar penguraian yang terbaik. Untuk mengatasi kelemahan mangkin yang sedia ada, penggunaan busa meso bersel yang mengandungi logam Fe (FeMCF) sebagai mangkin telah disintesis bagi merawat bahan pewarna azo yang mempunyai strcutur yang berbeza iaitu asid merah B dan reaktif hitam 5. Perubahan dalam dos 1,3,5- trimetilbenzena (TMB) (TMB /P123 = 0.125, 0.5 dan 0.75) dan kepekatan asid hidroklorik (HCl) (2.5, 0.5 dan 1.5 M) telah membawa kepada perbezaan pembentukan sifat akhir bahan sokongan yang ketara untuk secara langsung mempengaruhi kandungan spesis Fe di dalam bahan sokongan. Mangkin busa meso bersel yang mengandungi Fe yang disintesis pada nisbah TMB/P123 0.75 dan kepekatan asid hidroklorik 1.5 M telah berjaya menggabungkan kebanyakan Fe di dalam struktur liang yang mempunyai saiz tingkap (6 nm) and saiz sel (13 nm) yang cukup besar untuk menampung Fe. Mangkin FeMCF yang disintesis dengan menggabungkan Fe semasa langkah pertama sebelum dimasukkan silika, kandungan Fe dengan peratus berat sebanyak 10 (10 wt. %), dos ammonium florida sebanyak 0.023 g dan pengolahan suhu setinggi 450 ⁰C menunjukkan luas permukaan yang tinggi (814 m²/g), isipadu liang yang luas (1.808 cm³/g ), saiz tingkap (6 nm) dan sel (13 nm) yang besar, taburan Fe yang paling baik di samping kehadiran Fe yang berasingan di dalam struktur MCF dan saluran liang yang berkebolehan untuk mengatasi masalah yang berkaitan dengan pembentukan gumpalan Fe dan liang tersumbat. Secara tidak langsung, ini telah menyumbang kepada pembentukan radikal aktif bebas yang banyak dan dapat membantu dalam mendapatkan kadar peyahwarnaan (100 %) dan penguraian yang tertinggi (95 %) di samping dapat mengekalkan aktiviti dengan mempunyai kadar larut lesap yang rendah (< 0.1 mg/L). Penambahan logam kuprum terhadap mangkin FeMCF (Cu-FeMCF) menunjukkan kadar kecekapan yang tinggi (100 %) di dalam keadaan pH kurang berasid (pH 4). Mangkin Cu-FeMCF memerlukan tenaga pengaktifan yang lebih rendah (23.25 kJ/mol) berbanding mangkin FeMCF (62.57 kJ/mol). Ini adalah disebabkan oleh kesan sinergi antara Cu⁺, Fe²⁺ dan Fe³⁺ di atas permukaan mangkin Cu-FeMCF dimana mereka dapat mengambil bahagian di dalam proses berbalik Fe³⁺ kepada Fe²⁺ yang dapat menggalakkan pembentukan radikal aktif bebas yang cukup dan berterusan dan menyumbang kearah sistem serupa-Fenton yang lebih aktif dan kemampuan kebolehgunaan semula sebanyak tujuh kali (penyahwarnaan > 95 %) didalam sistem serupa-Fenton. __________________________________________________________________________________ The use of supported catalysts based on iron (Fe) in conjunction with hydrogen peroxide (H₂O₂) for catalytic degradation of organic dyes is attracting much attention due to their capability in achieving high rate of degradation. However, conventional Fenton-based heterogeneous catalysts still suffer from some limitations that could prevent them to achieve excellent performance in reusability study. To address the drawbacks of current types of heterogeneous Fenton-based catalyst, Fe incorporated mesocellular foam (FeMCF) catalyst have been developed to treat azo dyes with different structures namely acid red B (ARB) and reactive black 5 (RB5). Variations in the swelling agent (TMB) dosage (TMB/P123 = 0.125, 0.5 and 0.75) and hydrochloric acid (HCl) concentration (2.5, 0.5 and 1.5 M) led to significant differences in the final properties of the support materials to directly influence the distribution of Fe. Fe-MCFC catalyst developed at TMB/P123 ratio of 0.75 and 1.5 M HCl was capable of incorporating most of the Fe within the pore structure as the window (6 nm) and cell (13 nm) size were large enough to accommodate Fe particles. FeMCF catalyst developed by incorporating Fe during the first step before the subsequent addition of silica precursor, Fe concentration of 10 wt. %, ammonium fluoride dosage of 0.023 g and calcination temperature of 450 °C gave the largest surface area (814 m²/g), pore volume (1.808), window/cell size (6/13 nm), highest Fe distribution with the presence of isolated Fe in the MCF framework and along with the pore channels that could overcome the formation of large Fe aggregates and pore blockages. All these features directly contributed to the generation of large amount of •OH radicals to consequently demonstrate 100 % decolorization and 95 % degradation efficiency of ARB while maintaining its activity with minor leaching of Fe (Fe leaching < 0.1 mg/L). The addition of Cu before Fe (Cu-FeMCF) gave the highest decolorization (100 %) and degradation efficiencies (99 %). Cu-FeMCF required a relatively lower energy (23.25 kJ/mol) than FeMCF (62.57 kJ/mol) to degrade RB5. The excellent performance of Cu-FeMCF could be due to a synergistic effect between Cu⁺, Fe²⁺ and Fe³⁺ on the surface of Cu-FeMCF as they could effectively participate in the reversible Fe³⁺ to Fe²⁺ processes, which are essential to continuously lead to the generation of sufficient •OH radicals to maintain the high catalytic activity and reusability performances for up to 7 cycles (decolorization > 95 %) in Fenton-like systems.
Contributor(s):
Nur Azimah Jamalluddin - Author
Primary Item Type:
Thesis
Identifiers:
Accession Number : 875008425
Language:
English
Subject Keywords:
heterogeneous; concentration; calcination
First presented to the public:
10/1/2016
Original Publication Date:
12/3/2019
Previously Published By:
Universiti Sains Malaysia
Place Of Publication:
School of Chemical Engineering
Citation:
Extents:
Number of Pages - 318
License Grantor / Date Granted:
  / ( View License )
Date Deposited
2019-12-03 16:52:01.555
Date Last Updated
2020-11-16 15:07:34.98
Submitter:
Mohamed Yunus Yusof

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Mesocellular foam incorporated with copper and iron as catalyst for azo dyes degradation / Nur Azimah Jamalluddin1 2019-12-03 16:52:01.555