<br>同位素效应使金属有机框架晶体增大,Journal of the American Chemical Society

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同位素效应使金属有机框架晶体增大
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-02-28 , DOI: 10.1021/jacs.3c12866
Lixi Chen ₁ , Junhao Lu ₁ , Xiaoqi Li ₁ , Ni Luan ₁ , Yiting Song ₁ , Shenghai Yang ₁ , Mengjia Yuan ₁ , Haoming Qin ₁ , Huifang Zhu ₂ , Xue Dong ₃ , Kai Li ₁ , Duo Zhang ₁ , Long Chen ₁ , Xing Dai ₁ , Yanlong Wang ₁ , Yaxing Wang ₁ , Chao Xu ₃ , Zhifang Chai ₁ , Shuao Wang ₁

Affiliation

合成大型金属有机骨架（MOF）单晶引起了人们的广泛研究兴趣，尽管它受到产生大量小核的快速成核动力学的阻碍。鉴于各种类型的 MOF 固有的不同化学来源，开发增强其晶体尺寸的通用方法提出了艰巨的挑战。在这里，我们提出了一种简单的同位素替代策略，通过抑制成核来促进 MOF 的尺寸增长，从而导致晶体体积大幅增加 1.7 至 165 倍。令人印象深刻的是，通过常规方法在优化条件下制备的晶体可以通过同位素效应进一步放大，产生一锅法合成方法中最大的MOF单晶（2.9 cm×0.48 cm×0.23 cm）。详细的原位表征表明，同位素效应可以延迟结晶动力学，建立更高的成核能垒，从而产生更少的核，最终变得更大。与较小的晶体相比，同位素效应放大晶体的X射线剂量率检测限提高了33%。这项工作丰富了对同位素调控结晶过程效应的理解，并为探索大型MOF单晶的潜在应用提供了启发。

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Isotope Effect-Enabled Crystal Enlargement in Metal–Organic Frameworks

Synthesizing large metal–organic framework (MOF) single crystals has garnered significant research interest, although it is hindered by the fast nucleation kinetics that gives rise to numerous small nuclei. Given the different chemical origins inherent in various types of MOFs, the development of a general approach to enhancing their crystal sizes presents a formidable challenge. Here, we propose a simple isotopic substitution strategy to promote size growth in MOFs by inhibiting nucleation, resulting in a substantial increase in the crystal volume ranging from 1.7- to 165-fold. Impressively, the crystals prepared under optimized conditions by normal approaches can be further enlarged by the isotope effect, yielding the largest MOF single crystal (2.9 cm × 0.48 cm × 0.23 cm) among the one-pot synthesis method. Detailed in situ characterizations reveal that the isotope effect can retard crystallization kinetics, establish a higher nucleation energy barrier, and consequently generate fewer nuclei that eventually grow larger. Compared with the smaller crystals, the isotope effect-enlarged crystal shows 33% improvement in the X-ray dose rate detection limit. This work enriches the understanding of the isotope effect on regulating the crystallization process and provides inspiration for exploring potential applications of large MOF single crystals.

更新日期：2024-02-28

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