Broccoli-like CeO2 with Hierarchical/Porous Structures, and promoted oxygen vacancy as an enhanced catalyst for catalytic diesel soot elimination | IDCSA, NCHU

Broccoli-like CeO2 with Hierarchical/Porous Structures, and promoted oxygen vacancy as an enhanced catalyst for catalytic diesel soot elimination 2021-10-05

Recycling Agriculture: Rising value of Agricultural Waste【Department of Environmental Engineering / Lin, Kun-Yirew / Distinguished Professor】
循環農業：農業廢棄物高價值化【環境工程學系/林坤儀特聘教授】

論文篇名	英文：Broccoli-like CeO2 with Hierarchical/Porous Structures, and promoted oxygen vacancy as an enhanced catalyst for catalytic diesel soot elimination 中文：具有分層/多孔結構的西蘭花狀 CeO2，促進氧空位作為催化柴油煙灰消除的增強催化劑
期刊名稱	SEPARATION AND PURIFICATION TECHNOLOGY
發表年份,卷數,起迄頁數	2022, 281 ,119867
作者	Tsai, Yu-Chih; Kwon, Eilhann; Park, Young-Kwon; Huy, Nguyen Nhat; Lisak, Grzegorz; Hsu, Pei-Syuan; Hu, Chechia; Lin, Kun-Yi Andrew(林坤儀)*
DOI	10.1016/j.seppur.2021.119867
中文摘要	雖然 CeO₂ 是一種有前途的煙灰消除催化劑，但必須開發具有更高接觸面積的 CeO₂，以及有效煙灰氧化的反應性，因為催化煙灰氧化主要由催化劑的結構和表面性質控制。在這項研究中，採用由 Ce 和均苯三酸 (TA) 組成的 Ce-Metal 有機框架 (MOF) 作為前體，因為 CeTA 表現出獨特的西蘭花狀層次結構，該結構轉化為具有由 CeO₂ 納米纖維組成的層次結構的 CeO₂捆綁在一起，形成西蘭花狀的 CeO₂ 納米結構。更重要的是，這種花椰菜狀 CeO₂ (BCL-CeO₂) 中的 CeO₂ 納米纖維具有多孔結構和更多的氧空位，使 BCL-CeO₂ 成為一種有前途的煙塵氧化催化劑。因此，對於菸灰氧化，BCL-CeO₂ 顯示出比商業 CeO₂ 納米顆粒 (com-CeO₂) 高得多的催化活性，並且點火溫度 (T_ig) 顯著降低。更重要的是，雖然 com-CeO₂ 的煙灰氧化會導致 CO 與 CO₂ 一起產生，但 BCL-CeO₂ 可以將煙灰完全轉化為 CO₂。緊密接觸模式還使 BCL-CeO₂ 表現出 295 °C 的非常低的 T_ig，而 NO 和 H₂O 的存在也增強了 BCL-CeO₂ 的煙灰氧化以降低 T_ig。還檢查了 NO 輔助煙塵氧化的機制，並通過 DRIFTS 進行驗證，以確定含氮中間體的存在和轉化。 BCL-CeO₂ 還可以在許多連續循環中回收，並保持其對煙灰氧化的高催化活性。這些結果表明，BCL-CeO₂ 是一種有前途且易於製備的用於菸灰氧化的分層 Ce 基催化劑。
英文摘要	While CeO₂ is a promising catalyst for soot elimination, it is essential to develop CeO₂ with higher contact areas, and reactivity for effective soot oxidation as catalytic soot oxidation is dominantly controlled by structures, and surficial properties of catalysts. In this study, a Ce-Metal organic frameworks (MOFs) consisting of Ce and trimesic acid (TA) is employed as the precursor as CeTA exhibits a unique broccoli-like hierachitecture which is transformed into CeO₂ with a hierarchical structure consisting of nanofibers of CeO₂ bundled together, forming a broccoli-like CeO₂ nanostructure. More importantly, these CeO₂ nanofibers in this broccoli-like CeO₂ (BCL-CeO₂) possesses porous structures, and also more oxygen vacancies, enabling BCL-CeO₂ to become a promising catalyst for soot oxidation. Thus, BCL-CeO₂ shows a much higher catalytic activity than commercial CeO₂ nanoparticle (com-CeO₂) for soot oxidation with a significantly lower ignition temperature (T_ig). More importantly, while soot oxidation by com-CeO₂ leads to production of CO together with CO₂, BCL-CeO₂ can completely convert soot to CO₂. The tight contact mode also enables BCL-CeO₂ to exhibit a very low T_ig of 295 °C, whereas the existence of NO and H₂O also enhances the soot oxidation by BCL-CeO₂ to reduce the T_ig. The mechanism of NO-assisted soot oxidation is also examined, and validated by DRIFTS to identify the presence and transformation of nitrogen-containing intermediates. BCL-CeO₂ is also recyclable over many consecutive cycles and maintained its high catalytic activity for soot oxidation. These results demonstrate that BCL-CeO₂ is a promising and easily-prepared hierarchitectured Ce-based catalyst for soot oxidation.
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!