以花生殼基碳材負載鎳金屬作為雙功能催化劑於六價鉻還原與抗生素降解之研究

Please use this identifier to cite or link to this item: https://ir.lib.ncu.edu.tw/handle/987654321/97451

Title:	以花生殼基碳材負載鎳金屬作為雙功能催化劑於六價鉻還原與抗生素降解之研究
Authors:	陳宛妤;Chen, Wan-Yu
Contributors:	化學學系
Keywords:	汙染物;六價鉻還原;四環素降解
Date:	2025-07-28
Issue Date:	2025-10-17 11:19:50 (UTC+8)
Publisher:	國立中央大學
Abstract:	本篇論文研究分為兩部分。第一部分研究中，以農業廢棄物花生殼作為碳源，經碳化與化學活化處理後製備具微孔結構之花生殼生質碳材，再使用 NaBH4和NH3BH3作為還原劑，，將不同含量的Ni金屬還原附載其上，形成Ni(X)@N-PS-DA複合材料。經由粉末X射線繞射(XRD)， N2吸附脫附等溫曲線(BET)，穿透電子顯微鏡(TEM)與X光電子能譜(XPS)等分析確認Ni金屬成功附載於碳材，並具微量氮摻雜特性。催化測試以六價鉻還原為三價鉻之反應為對象，探討不同金屬比例 pH值初始Cr濃度反應時間與材料回收次數等條件對催化表現之影響。結果顯示，當Ni金屬含量為15 wt%時，材料展現最佳的六價鉻還原能力。然而，經過多次循環使用後，催化效率逐漸下降，第五次回收時回收率下降至 44.51%，推測可能與微孔結構導致部分Ni金屬流失有關。第二部分中，針對不同Ni含量之Ni(X)@N-PS-DA催化劑，結合多項反應參數（如催化劑添加量 PMS 濃度與 pH 值）進行系統性測試，探討其於過硫酸鹽（PMS）活化促進抗生素四環素（TC）降解反應之效能。結果顯示，Ni(5)@N-PS-DA於最佳反應條件下展現最優異之催化活性，於6分鐘內可降解96.79%的TC，，對應反應速率常數（k）為54.04 min⁻¹ g_cat⁻¹。進一步探討催化劑添加量對降解效率的影響，發現隨著劑量由5 mg提升至15 mg，，反應時間由28分鐘大幅縮短至11 分鐘，顯示材料表面活性位點數量及PMS活化能力對降解速率具有顯著影響。整體而言，Ni(X)@N-PS-DA複合材料兼具還原與氧化雙功能，展現其於水中重金屬及有機物之高效催化潛力，具備環境應用價值與資源再利用意義。;This thesis is divided into two parts. In the first part, peanut shells, an agricultural waste, were used as a carbon source to synthesize microporous biochar through carbonization and chemical activation. Subsequently, different amounts of nickel (Ni) were reduced and loaded onto the carbon matrix using NaBH₄ and NH₃BH₃ as reducing agents, forming Ni(X)@N-PS-DA composite materials. Characterizations including powder X-ray diffraction (XRD), nitrogen adsorption–desorption isotherms (BET), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) confirmed the successful incorporation of Ni nanoparticles into the porous structure with minor nitrogen doping. The catalytic performance was evaluated via the reduction of hexavalent chromium (Cr(VI)) to trivalent chromium (Cr(III)), investigating the effects of Ni loading, solution pH, initial Cr concentration, reaction time, and catalyst recyclability. The results showed that the Ni(15)@N-PS-DA exhibited the highest reduction efficiency. However, after multiple reuse cycles, the catalytic activity gradually declined, with the reduction efficiency decreasing to 44.51% in the fifth cycle, possibly due to the loss of Ni caused by the microporous structure. In the second part, Ni(X)@N-PS-DA catalysts with varying Ni contents were evaluated for the degradation of tetracycline (TC) through peroxymonosulfate (PMS) activation. A systematic investigation was conducted, including the effects of catalyst dosage, PMS concentration, and solution pH. Among the tested samples, Ni(5)@N-PS -DAdemonstrated the best catalytic performance under optimal conditions, achieving 96.79% TC degradation within 6 minutes, with a corresponding rate constant (k) of 54.04 min⁻¹ g_cat⁻¹. Further experiments revealed that increasing the catalyst dosage from 5 mg to 15 mg significantly reduced the reaction time from 28 minutes to 1 minute, indicating that the number of active sites and the efficiency of PMS activation play key roles in degradation performance. Overall, the Ni(X)@N-PS-DA composite exhibited dual redox functionality, highlighting its promising potential for the treatment of both heavy metal ions and organic pollutants in water, with strong implications for environmental applications and resource reutilization.
Appears in Collections:	[Graduate Institute of Chemistry] Electronic Thesis & Dissertation

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