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從腐泥土型紅土鎳礦制備共摻雜MgFe2O4物相轉化規律及催化性能

Phase transformation and catalytic performance of metal-doped MgFe2O4 prepared from saprolite laterite

  • 摘要: 采用酸浸-水熱-煅燒法從腐泥土型紅土鎳礦中制備磁性多金屬共摻雜型MgFe2O4異相類芬頓(Fenton)催化劑.利用X射線衍射(XRD)、傅立葉紅外光譜(FTIR)、掃描電子顯微鏡(SEM)和比表面積及孔徑分布測定(BET-BJH)等手段, 考察了煅燒溫度對所制備產物結構、形貌和比表面積及孔徑分布的影響, 并研究了所制備產物作為異相Fenton催化劑降解羅丹明B (RhB)溶液的催化活性.結果表明, 水熱合成產物為層狀雙(多)金屬氫氧化物和尖晶石型MgFe2O4復合物.通過300℃的煅燒, 層狀雙(多)金屬氫氧化物就能分解并生成MgFe2O4; 隨著煅燒溫度的提高, 產物結晶度增加、粒徑尺寸變大, 形貌逐漸生長為近球型顆粒且分散度漸漸提高, 同時介孔數量減少、比表面積減小.經過500℃煅燒的試樣H-C500顯示出優異的催化降解活性.在體系反應溫度為45℃、pH值為6.44、催化劑用量為0.625 g·L-1且H2O2體積分數為1.0%的條件下, 經過300 min, 10 mg·L-1的羅丹明B溶液降解率可達到97.8%, 同時總有機碳(TOC)去除率達到77.8%.重復使用3次后, 催化劑仍能保持較高活性, 降解率和TOC去除率減少量分別少于3.0%和5.0%.

     

    Abstract: Heterogeneous Fenton-like method has attracted considerable attention because of its potential effectiveness in mineralization of organic contaminants in a wide range of reaction medium pH. Spinel ferrites MFe2O4 (M=Fe, Zn, Cu, Ni, Mn, Co) as heterogeneous Fenton-like catalysts have been studied extensively due to their good catalytic activity, prominent physical and chemical stability, and excellent magnetic properties, which allow their easy separation from the reaction medium by magnetic field for further circular utilization. Considering the group of ferrites, limited research focused on the utilization of MgFe2O4 as heterogeneous Fenton catalytic agent, whereas most of the catalysts are synthesized by pure chemical reagents. In this study, magnetic multi-metal co-doped MgFe2O4 heterogeneous Fenton-like catalyst was synthesized from saprolite laterite by acid leaching-hydrothermal calcination method. The effect of calcination temperature on the phase, morphology, specific surface area, and pore size distribution of samples were characterized by X-ray diffraction, scanning electron microscopy, Fourier-transform infrared, Brunauer-Emmett-Teller/Barrett-Joyner-Halenda analysis. The catalytic activity of the as-prepared products as heterogeneous Fenton catalysts for the degradation of Rhodamine B (RhB) solution was also investigated. The results show that the layered double (multi) hydroxides coupled with a portion of magnesium ferrite are synthesized by hydrothermal method, and the cubic crystal MgFe2O4 is obtained by decomposition of the layered double (multi) hydroxides after calcination above 300℃. With the increase in calcining temperature, the crystallinity of the products increases, and the particle size becomes larger. The morphology gradually grows to near spheroidal particles, and the dispersion degree gradually increases. Meanwhile, the pore size becomes larger, and the specific surface area is reduced. Calcination of sample H-C500 exhibits the best catalytic activity for the degradation of RhB after 500℃, achieving 97.8% degradation efficiency of 10 mg·L-1 RhB after 300 min at the reaction conditions of 45℃, pH 6.44, 0.625 g·L-1 catalyst dosage, and 1.0% (volume fraction) H2O2. The total organic carbon (TOC) removal could reach 77.8%. The reused catalyst can still maintain high activity, and after three consecutive degradation cycles, the reduction of degradation efficiency and TOC removal efficiency are less than 3.0% and 5.0%, respectively.

     

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