Environmental Waste Recycle Institute, Department of Energy Science and Technology, Myongji University, Yongin, Gyeonggi-do, 17058, Republic of Korea.
Environmental Waste Recycle Institute, Department of Energy Science and Technology, Myongji University, Yongin, Gyeonggi-do, 17058, Republic of Korea.
J Environ Manage. 2021 Nov 15;298:113433. doi: 10.1016/j.jenvman.2021.113433. Epub 2021 Aug 2.
Currently, it is essential to consider the rapidly increasing emission of CO into the atmosphere, causing major environmental issues such as climate change and global warming. In this work, we have developed the binary catalyst system (ZnCoO/inorganic salt) for chemical fixation of CO with epoxides into cyclic carbonates without solvent, and all reactions were performed on a large scale using a 100 ml batch reactor. Two mesoporous catalysts of ZnCoO with different architecture, such as flakes (ZnCo-F) and spheres (ZnCo-S) were synthesized and utilized as a heterogeneous catalyst for cycloaddition reaction. The bifunctional property of catalysts is mainly attributed to strong acidic and basic properties confirmed by TPD (NH & CO) analysis. The ZnCo-F catalyst exhibited excellent conversion of propylene oxide (99.9%) with good corresponding selectivity of propylene carbonate (≥99%) in the presence of inorganic salt (KI) at 120 °C, 2 MPa, 3 h. In addition, ZnCo-F catalyst demonstrated good catalytic applicability towards the various substrates scope of the epoxide. Furthermore, the catalytic properties were examined by evaluating the reaction parameter such as catalyst loading, pressure, temperature and time. The proposed catalyst exhibited good reusability for cycloaddition reaction without significant change in its catalytic activity and proposed a possible reaction mechanism for chemical fixation of CO with epoxide into cyclic carbonate over ZnCo-F/KI.
目前,必须考虑到 CO 排放到大气中导致的主要环境问题,如气候变化和全球变暖。在这项工作中,我们开发了用于 CO 与环氧化物在无溶剂条件下化学固定成环状碳酸酯的二元催化剂体系(ZnCoO/无机盐),所有反应均在 100ml 分批式反应器中大规模进行。我们合成了两种具有不同结构的介孔 ZnCoO 催化剂,如薄片(ZnCo-F)和球体(ZnCo-S),并将其用作用于加成反应的多相催化剂。催化剂的双功能特性主要归因于 TPD(NH 和 CO)分析所证实的强酸性和碱性。在 120°C、2MPa、3h 的条件下,在无机盐(KI)存在下,ZnCo-F 催化剂对环氧丙烷表现出优异的转化率(99.9%)和相应的碳酸丙烯酯选择性(≥99%)。此外,ZnCo-F 催化剂对各种环氧化物底物的催化适用性也很好。此外,还通过评估催化剂负载量、压力、温度和时间等反应参数来考察了催化性能。该催化剂在加成反应中表现出良好的可重复使用性,其催化活性没有明显变化,并提出了 ZnCo-F/KI 上 CO 与环氧化物化学固定成环状碳酸酯的可能反应机理。