雙亞硝基鐵化合物催化二氧化碳硼氫化反 應與小分子之應用;CO2 Hydroboration and Small Molecule Activation Catalyzed by Dinitrosyl Iron Complexes

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题名:	雙亞硝基鐵化合物催化二氧化碳硼氫化反應與小分子之應用;CO2 Hydroboration and Small Molecule Activation Catalyzed by Dinitrosyl Iron Complexes
作者:	張哲瑋;Chang, Che-Wei
贡献者:	化學學系
关键词:	二氧化碳還原;雙亞硝基鐵化合物;無溶劑反應;機械化學;Carbon dioxide reduction;Dinitrosyl iron complexes;Solvent-free;Mechanochemistry
日期:	2025-06-26
上传时间:	2025-10-17 11:13:05 (UTC+8)
出版者:	國立中央大學
摘要:	隨著人類活動與工業發展，二氧化碳的過度排放使得全球面臨日益嚴峻的氣候變遷與碳排放等問題。為了有效解決這問題，科學家正積極開發將二氧化碳作為C1碳源，生產高附加價值化學品與燃料的有效方法。在本研究中，合成出含有吡唑硼氫化合物的雙亞硝基鐵化合物[Fe(NO)2(3,5MePz)2BH2]- (2, 3,5MePz = 3,5-dimethylpyrazole)，作為催化劑能夠有效催化二氧化碳還原反應。2能夠與二氧化碳反應形成甲酸階段產物[Fe(NO)2(3,5MePz)2BHOCHO]- (4)。隨後與pinacolborane (HBPin)進一步反應，生成甲醇階段產物BPinOCH3，並能夠經由水解反應轉化成甲醇。本研究亦對反應機制進行深入研究，藉由質譜(Mass)與核磁共振(NMR)光譜捕捉到兩個關鍵中間體(IntA與IntB)，並進一步探討反應機制。此催化劑除了能在有機溶劑中進行反應，在無溶劑的條件下也能夠進行催化。利用機械化學(mechanochemistry)的方式，能夠提高其催化效率且保有高選擇性。此外，我們也嘗試活化其他小分子如甲醛，展現出良好的應用潛力。機械化學不僅為二氧化碳還原反應提供一種新的催化方式，也突顯了在綠色化學與永續技術中的應用價值。 ;Industry development has led to the accumulation of CO2 in the atmosphere, associated with climate change and global carbon balance. To address this issue, the scientific community has been actively exploring efficient strategies to utilize CO2 as a C1 feedstock for the production of value-added chemicals and fuels. In this study, we report the synthesis of dinitrosyl iron complex (DNICs), [Fe(NO)2(3,5MePz)2BH2]⁻ (2, 3,5MePz = 3,5-dimethylpyrazole), as a catalyst for CO2 reduction. Upon exposure to CO2, 2 transformed to formate species, which was subsequently reduced by pinacolborane (HBPin) to afford methoxylborane (BPinOCH3). Key intermediates involved in the catalytic cycle were characterized by mass spectrometry and NMR spectroscopy. Notably, the BPinOCH3 was obtained with high selectivity and even under solvent-free conditions using a mechanochemical (ball-milling) approach. In addition, the catalyst demonstrated the ability to activate other small molecules such as formaldehyde, leading to the formation of methanol derivatives and underscoring its potential versatility. This work highlights mechanochemistry as a promising and sustainable approach for CO2 reduction and small molecule activation, offering a new direction in the field of green chemistry.
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