Luo Dan, Liu Chen-Hui, Chen Yi-Bo, Wang San-Tai, Fang Wei-Hui, Zhang Jian
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, P. R. China.
Adv Sci (Weinh). 2024 Jan;11(2):e2305833. doi: 10.1002/advs.202305833. Epub 2023 Nov 16.
The motivation for making heterometallic compounds stemmed from their emergent synergistic properties and enhanced capabilities for applications. However, the atomically precisely controlled synthesis of heterometallic compounds remains a daunting challenge of the complications that arise when applying several metals and linkers. Herein, a stepwise and controlled method is reported for the accurate addition of second and third metals to homometallic aluminum macrocycles based on the synergistic coordination and hard-soft acid-base theory. These heterometallic compounds showed a good Lewis acid catalytic effect, and the addition of hetero-metals significantly improved the catalytic effect and rate, among that the conversion rate of compound AlOC-133 reached 99.9% within half an hour. This method combines both the independent controllability of stepwise assembly with the universality of one-step methods. Based on the large family of clusters, the establishment of this method paves the way for the controllable and customized molecular-level synthesis of heterometallic materials and creates materials customized for preferential application.
制备异金属化合物的动机源于其新出现的协同性质以及增强的应用能力。然而，异金属化合物的原子精确控制合成仍然是一个艰巨的挑战，因为在应用多种金属和连接体时会出现复杂情况。在此，基于协同配位和软硬酸碱理论，报道了一种逐步且可控的方法，用于将第二和第三种金属精确添加到同金属铝大环化合物中。这些异金属化合物显示出良好的路易斯酸催化效果，并且添加杂金属显著提高了催化效果和速率，其中化合物AlOC - 133在半小时内转化率达到99.9%。该方法结合了逐步组装的独立可控性和一步法的通用性。基于大量的簇合物家族，此方法的建立为异金属材料的可控和定制分子水平合成铺平了道路，并创造出为优先应用而定制的材料。
