【學術亮點】MOF-derived hollow Co@N-doped carbon as an efficient peroxymonosulfate activator for acetaminophen degradation: Dominant sulfate radical-induced degradation pathway
Recycling Agriculture: Valorization of Agricultural Residual Materials【Department of Environmental Engineering / Lin, Kun-Yirew / Distinguished Professor】
循環農業：農業剩餘資材及生質衍生物高值化轉換再利用【環境工程學系/林坤儀特聘教授】
| 論文篇名 | 英文：MOF-derived hollow Co@N-doped carbon as an efficient peroxymonosulfate activator for acetaminophen degradation: Dominant sulfate radical-induced degradation pathway 中文：MOF衍生的空心Co@N摻雜碳作為對乙醯氨基酚降解的有效過氧單硫酸鹽活化劑：主要硫酸鹽自由基誘導的降解途徑 |
| 期刊名稱 | Separation and Purification Technology |
| 發表年份,卷數,起迄頁數 | 2025 ,354, no.129381 |
| 作者 | Tuan, Duong Dinh; Tsai, Yu-chih; Linh, Ha Xuan; Van Thanh, Dang; Khiem, Ta Cong; Lin, Kun-Yi Andrew(林坤儀)* |
| DOI | 10.1016/j.seppur.2024.129381 |
| 中文摘要 | 碳基材料已被證實是具有潛力的過一硫酸氫鹽（peroxymonosulfate, PMS）活化劑，可用於去除廢水中難降解的有機污染物。本研究提出一種新策略，製備出具有中空結構的鈷（Co）嵌入氮摻雜碳（H-Co@SNC）材料。該材料是以星狀雙金屬有機骨架（S-ZnCoMOF）為前驅體，經由兩步修飾法合成而得。 所製備的H-Co@SNC展現出中空結構與獨特的物理化學特性，經由多種表徵技術（如XRD、BET、Raman、TGA、XPS等）驗證，這些特性有助於其在PMS活化中表現出優異的催化活性，用以降解水中的殘留藥物污染物——對乙醯氨基酚（acetaminophen, ACE）。 實驗結果顯示，H-Co@SNC/PMS系統可在10分鐘內完全降解ACE，並達到高達76.5%的總有機碳（TOC）去除率，明顯優於其他對照系統。此外，藉由自由基猝滅實驗與電子順磁共振（EPR）分析，揭示了反應過程中各種活性物種的產生、高價鈷氧物種的形成以及電子轉移機制，其中硫酸根自由基（SO₄●⁻）在ACE降解中起關鍵作用。 研究同時提出了ACE的中間產物與可能的降解途徑，並評估了中間產物的毒性。綜合而言，本研究提供了一種新穎的中空結構金屬摻雜碳材料的合成策略，該材料有望成為高效的PMS活化劑，用於廢水中有機污染物的去除。 |
| 英文摘要 | Carbonaceous materials have been proven as promising peroxymonosulfate (PMS) activators to eliminate recalcitrant organic contaminants in wastewater. Herein, in this study, we proposed to fabricate hollow-structured cobalt (Co)-embedded in nitrogen-doped carbon (H-Co@SNC) derived from a star-like bimetallic ZnCoMOF (S-ZnCoMOF) through two-step modifications. This as-prepared H-Co@SNC exhibited a hollow configuration with peculiar physicochemical properties verified by different characterizations (XRD, BET, Raman, TGA, XPS, etc) that would be contributed to its excellent catalytic activity in PMS activation to degrade a residual pharmaceutical contaminant, acetaminophen (ACE) in water. Based on the experimental results, H-Co@SNC/PMS system can completely degrade ACE in 10 min with a high total organic carbon (TOC) removal content of 76.5 % compared with other tested systems. On the other hand, quenching experiments and electron paramagnetic resonance (EPR) analysis were employed to explore the generation of various reactive species, high-valent cobalt-oxo, and electron transfer involved in ACE degradation, in which SO4●− played a pivotal role. The intermediate products and plausible degradation pathways of ACE were proposed whereas the toxicity of the intermediates was also assessed. This work provides an insight into the preparation strategy for synthesizing a hollow-structured metal-doped carbon material that would be a promising PMS activator for eliminating organic pollutants in wastewater. |
| 發表成果與本中心研究主題相關性 | 透過本研究可進一步建立開發本研究計算所需之觸媒材料，並釐清可適合應用之環境條件! |
