Recycling Agriculture: Rising value of Agricultural WasteDepartment 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:Catalytic reduction of bromate by Co-embedded N-doped carbon as a magnetic Non-Noble metal hydrogenation catalyst
中文:共嵌入 N 摻雜碳作為磁性非貴金屬加氫催化劑催化還原溴酸鹽
期刊名稱 Separation and Purification Technology
發表年份,卷數,起迄頁數 2021, 227, 119320
作者 Li, Bing-Cheng; Yang, Hongta; Kwon, Eilhann; Tuan, Duong Dinh; Khiem, Ta Cong; Lisak, Grzegorz; Thanh, Bui Xuan; Ghanbari, Farshid*; Lin, Kun-Yi Andrew(林坤儀)*
DOI 10.1016/j.seppur.2021.119320
中文摘要 雖然溴酸鹽的催化加氫是消除致癌溴酸鹽的有用技術,但通常需要昂貴的貴金屬催化劑和過量的氫氣,阻礙了該技術的大規模實施。由於硼氫化物是以更可控的方式釋放 H2 的替代來源,並且非貴金屬催化劑(例如 Co)可以催化硼氫化物水解生成 H2,因此使用 Co 和硼氫化物進行溴酸鹽的加氫是有希望的。此外,開發具有磁性的多相催化劑以更容易處理和回收催化劑更加實用。因此,本研究的目的是開發一種使用硼氫化物還原溴酸鹽的磁性多相催化劑。在此,通過碳化將 Co 取代的普魯士藍類似物轉化為 Co 嵌入的 N 摻雜碳(Co@NC)複合材料,製備了一種特殊的 Co 基催化劑。 Co@NC 還表現出比商業 Co3O4 更高的還原溴酸鹽的催化活性,因為 Co@NC 可以加速 NaBH4 的水解以更快地產生 H2 氣體。 Co@NC 還原溴酸鹽的活化能 (Ea) 也遠低於報導的 Ea Co@NC 在鹼性條件下仍然可以完全去除溴酸鹽並將其還原為溴化物,並且 Co@NC 在其他陰離子存在下對溴酸鹽還原也表現出非常高的選擇性。此外,Co@NC 還可以重複使用多次循環,以不斷將溴酸鹽還原為溴化物。這些特徵表明 Co@NC 無疑是一種用於還原水中溴酸鹽的有利且方便的多相催化劑。
英文摘要 While catalytic hydrogenation of bromate represents a useful technique for eliminating carcinogenic bromate, expensive noble-metal catalysts and excessive H2 gas are usually required, impeding large-scale implementation of this technique. As borohydride is an alternative source for releasing H2 in a more controllable way and non-noble metal catalysts (e.g., Co) can catalyze hydrolysis of borohydride to generate H2, it is promising to employ Co and borohydride for hydrogenation of bromate. Moreover, it is even more practical to develop heterogeneous catalysts with magnetism for easier handle and recovery of catalysts. Therefore, the aim of this study is to develop such a magnetic heterogeneous catalyst for bromate reduction by using borohydride. Herein, a special Co-based catalyst is fabricated by transforming Co-substituted prussian blue analogue into Co-embedded N-doped carbon (Co@NC) composite through carbonization. Co@NC also exhibits a higher catalytic activity for reducing bromate than the commercial Co3O4 as Co@NC could accelerate hydrolysis of NaBH4 to generate H2 gas much faster. The activation energy (Ea) of bromate reduction by Co@NC is also much lower than the reported Ea. Co@NC could still completely remove bromate and reduce it to bromide under alkaline conditions, and Co@NC also exhibit a very high selectivity towards bromate reduction in the presence of other anions. Moreover, Co@NC could be also reused for multiple-cycles to continuously reduce bromate to bromide. These features demonstrate that Co@NC is certainly an advantageous and convenient heterogeneous catalyst for reducing bromate in water.
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!