用于将一氧化碳转化为碳酸盐的锆调制氮掺杂复合材料。
Zr modulated N doping composites for CO conversion into carbonates.
作者信息
Huang Jielin, Wang Jie, Duan Haonan, Dong Li, Chen Songsong, Zhang Junping, Zhang Xiangping
机构信息
School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049, China.
Beijing Key Laboratory of Ionic Liquids Clean Process, CAS Key Laboratory of Green Process and Engineering, State Key Laboratory of Mesoscience and Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China.
出版信息
iScience. 2024 Apr 9;27(5):109714. doi: 10.1016/j.isci.2024.109714. eCollection 2024 May 17.
Acidic and basic sites of catalysts are essential for CO capture and activation. In this work, Zr, N-ZnO/ZnAl-LDH-IL composites in ionic liquid and methanol systems were fabricated, and applied to catalyze the synthesis of ethylene carbonate (EC) from ethylene glycol (EG) and CO with about 4.76 mmol g h. The composites showed more strong basic sites due to the effective induction of reactive groups on the catalyst surface by Zr doping, resulting in an increase of pyridinic-N groups from 5.48% to 22.25%. More C atoms adjacent to pyridinic-N as strong basic sites was conducive to the activation of CO and EG. In addition, the possible catalytic pathway and mechanism of the composites for synthesizing EC as well as the doping of La, Fe, Ce, and Cu were also investigated, which provides an effective strategy for regulating the acid-base centers on the catalyst surface through ionic liquids and methanol solvents.
催化剂的酸性和碱性位点对于二氧化碳的捕获和活化至关重要。在本工作中，制备了离子液体和甲醇体系中的Zr、N-ZnO/ZnAl-LDH-IL复合材料，并将其应用于催化乙二醇（EG）和CO合成碳酸乙烯酯（EC），催化活性约为4.76 mmol g⁻¹ h⁻¹。由于Zr掺杂对催化剂表面反应基团的有效诱导，复合材料表现出更多的强碱性位点，导致吡啶氮基团从5.48%增加到22.25%。更多与吡啶氮相邻的C原子作为强碱性位点有利于CO和EG的活化。此外，还研究了该复合材料合成EC的可能催化途径和机理以及La、Fe、Ce和Cu的掺杂情况，这为通过离子液体和甲醇溶剂调节催化剂表面酸碱中心提供了一种有效策略。
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