【學術亮點】以模板犧牲法建構的分級空心氧化鈷促進催化煙灰氧化:促進形態和氧空位的作用
【學術亮點】Boosted catalytic soot oxidation by hierarchical hollow cobalt oxide constructed from a Template-Sacrificial Method: Promoting Roles of morphologies and oxygen vacancies
Recycling Agriculture: Valorization of Agricultural Residual MaterialsDepartment 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:Boosted catalytic soot oxidation by hierarchical hollow cobalt oxide constructed from a Template-Sacrificial Method: Promoting Roles of morphologies and oxygen vacancies
中文:以模板犧牲法建構的分級空心氧化鈷促進催化煙灰氧化:促進形態和氧空位的作用
期刊名稱 Chemical Engineering Journal
發表年份,卷數,起迄頁數 2025,510, no. 161458
作者 Tsai, Yu-Chih; Wan, Mei-Chen; Lin, Shen Yan; Thuy, Vo Thi Thanh; Huy, Nguyen Nhat; Tuan, Duong Dinh; Lee, Jechan; Lin, Kun-Yi Andrew(林坤儀)*
DOI 10.1016/j.cej.2025.161458
中文摘要 柴油引擎所產生的碳煙(soot)被視為有害污染物,通常需藉由柴油微粒濾清器(diesel particulate filters, DPFs)進行控制。然而,DPF的再生過程需消耗大量熱能,導致能源使用增加,因此亟需開發能在低溫下有效分解碳煙的催化方法。
由金屬有機骨架(metal-organic frameworks, MOFs)衍生的氧化鈷(Co₃O₄)具有極高的碳煙氧化催化活性。本研究以甘油酸鈷(cobalt glycerate, CG)為前驅體,使沸石咪唑骨架材料ZIF-67在其表面生長,形成ZIF-67修飾的CGZCG)。經熱處理後,ZCG轉化為空氣處理後的ZIF衍生氧化鈷修飾CGAZCCG)。
AZCCG具有更多的氧空位與增強的接觸點,能促進活性氧物種的生成及其從催化劑向碳煙的溢流(spillover),進而提升氧化效率。與ACGAZC及商業氧化鈷(COM)相比,AZCCG展現出更佳的氮氧化物(NOx)儲存能力與耐水性,其點火溫度更低。在含500 ppm NO + 10% H₂O + 10% O₂/N₂的鬆散接觸條件下,其碳煙轉化溫度(T₅₀50%碳煙被氧化)比對照組降低了248°C
本研究提出了一種簡單的策略,可製備具有獨特結構與豐富氧空位的氧化鈷基催化劑,用以提升碳煙氧化效率。經此方法合成的催化劑具分層中空形貌與高比表面積,顯著優於先前報導的氧化鈷催化劑。這些結構特徵不僅能提供更多的活性氧物種,亦能增加與碳煙的接觸機會,進一步提升催化性能。
綜上所述,AZCCG展現出優異的碳煙氧化性能與耐久性,極具應用於柴油微粒濾清器(DPFs)的潛力。
英文摘要 Diesel engine soot, deemed harmful, is controlled by diesel particulate filters (DPFs). However, these filters need heat for regeneration, leading to energy use. An effective way to decompose soot at lower temperatures is sought. Co3O4 from metal organic frameworks (MOFs) has high catalytic activity for soot oxidation. Using cobalt glycerate (CG) as a precursor, zeolitic imidazolate framework (ZIF)-67 grows on CG’s surface, forming ZIF-67-decorated CG (ZCG). Heat treatment turns ZCG into air-treated ZIF-derived Co3O4-decorated CG (AZCCG). AZCCG, with more oxygen vacancies and increased contact points, enhances active oxygen species, promoting spillover from catalysts to soot. It also exhibits superior NOx storage capacity and high H2O tolerance with ignition temperature compared to ACG, AZC, and commercial Co3O4 (COM); as a result, the conversion temperature (T50, 50 % soot was oxidized) was reduced by 248℃ with loose contact mode in 500 ppm NO + 10 %H2O + 10 % O2/N2. This study proposes a simple method to create a cobalt oxide-based catalyst with a unique structure and abundant oxygen vacancies to boost soot oxidation. The catalyst developed through this method demonstrates hierarchical hollow morphology and a high specific surface area, distinguishing it from previously reported cobalt oxide catalysts. These features not only provide a greater abundance of active oxygen species but also offer increased opportunities for contact with soot, thereby improving its catalytic performance. As a result, AZCCG is highly promising for application in diesel particulate filters(DPFs).
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!