Zhang Jing, Liu Yu, Liu Mingyang, Wang Zhenzhu, Qi Ting, Zhang Mingming, Shi Hao, Song Jun
College of Materials and Chemistry & Chemical Engineering, Chengdu University of Technology Chengdu 610059 P. R. China
Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL) 1015 Lausanne Switzerland.
Chem Sci. 2024 Jun 12;15(27):10585-10591. doi: 10.1039/d4sc01569j. eCollection 2024 Jul 10.
Selective synthesis of nanocluster (NC) isomers with tailored structures holds significant importance for enhancing their applications. Here, we develop an effective strategy for the selective synthesis of CdS NC isomers through the judicious choice of a pair of carboxylic acid isomer additives. Specifically, CdS NC-312 and NC-323 (denoted by their UV-vis absorption peak position) could be selectively produced by introducing a conventional mixture of Cd and S precursors, with the addition of 2-methylbutyric acid (2-MA) and 3-methylbutyric acid (3-MA), respectively. The synthesized NC isomers demonstrated a precise isomeric relationship, sharing both the isomeric inorganic core and organic surface. Alternatively, the as-synthesized NCs were interconvertible by re-adding the acid isomers. The density functional theory calculations further support that 2-MA and 3-MA have specific selectivity for producing CdS NC isomers by interfacial tuning. Finally, the generality of this methodology was also evidenced with applications in other CdS NC synthetic systems. This study unveils the intriguing correlation between additive structures and the configuration of NCs, providing a foundation for the selective synthesis of NC isomers.
选择性合成具有定制结构的纳米团簇(NC)异构体对于增强其应用具有重要意义。在此,我们通过明智地选择一对羧酸异构体添加剂,开发了一种选择性合成CdS NC异构体的有效策略。具体而言,通过引入常规的Cd和S前驱体混合物,分别添加2-甲基丁酸(2-MA)和3-甲基丁酸(3-MA),可以选择性地制备CdS NC-312和NC-323(由其紫外-可见吸收峰位置表示)。合成的NC异构体表现出精确的异构关系,共享异构的无机核心和有机表面。此外,通过重新添加酸异构体,合成的NC可以相互转化。密度泛函理论计算进一步支持,2-MA和3-MA通过界面调控对生成CdS NC异构体具有特定的选择性。最后,该方法在其他CdS NC合成系统中的应用也证明了其通用性。这项研究揭示了添加剂结构与NC构型之间的有趣关联,为NC异构体的选择性合成提供了基础。