At present, the gradual and in-depth development of multidisciplinary paradigm has put forward new requirements to traditional chemical synthesis. Recently, with the rapid development of artificial intelligence technology represented by machine learning, the "AI+Chem" model has gradually made automatic synthesis intelligent. By mining massive chemical experiment data, AI can not only help researchers make reasonable analysis and prediction, but also liberate researchers from tedious and complex daily experiments, which can greatly accelerate the related research and development process. This review combs the recent development of chemical research field from automatic synthesis to intelligence. We started with the description of the development of laboratory automation platform. Then, we systematically summarized recent progress on the construction paradigm of laboratory automation platform, emphasized the combination of automatic synthesis technology and artificial intelligence to achieve intelligent closed-loop strategy of chemical synthesis. Finally, we discussed the future development prospects of this field.

Organometallic supramolecular assemblies containing N-heterocyclic carbene (NHC) ligands linked via metal–carbon bonding have attracted attention in recent years because of their functional applications in biochemistry, catalysis, and materials science. However, most methods currently used to construct poly-NHC metallosupramolecular assemblies are solution-based methods that suffer from cumbersome procedures and the need for harsh conditions, which greatly limits the research in this area. Herein, a general, efficient, and simplified mechanochemical synthesis protocol was developed and used to construct more than 70 diverse poly-NHC silver(I) assemblies (e.g., metallacycles, metallocages, and interlocked assemblies), thus overcoming the shortcomings of the solution-based methods. Highly selective narcissistic or social self-sorting was observed during this solid-state mechanochemical complexation process. In addition, this new method, which has the advantages of low energy consumption, high yields, a short reaction time, and minimal solvent waste, facilitates the synthesis of poly-NHC silver(I) assemblies and allows the subsequent large-scale synthesis and functional exploration of such architectures.

Developing discrete radical organometallic nanocages is essential for fabricating functional materials. In this study, we construct a series of poly-NHC-based (NHC = N-heterocyclic carbene) organometallic nanocages 3a–3c with different sizes by employing redox-active bis(triarylamine) derivatives with different π-conjugated spacers as building blocks. The varied sizes of nanocages 3a–3c modulate the distance of the redox-active centers and reversibly convert them to radical nanocages 3a²⁺–3c²⁺ through chemical and electrochemical oxidation. Radical nanocages 3a²⁺–3c²⁺ display clear bond and angle alteration and retention of their three-dimensional topologies. This work not only merely proves that these nanocages are excellent stimulus-responsive materials but also opens a door to the rational design of novel radical organometallic nanocages.

Bottom-up construction of highly complex architecture from simple components remains one of the long-standing challenges in chemistry. Herein two supramolecular isomers based on large trigonal prismatic Pd₃L¹₆ building block are reported. Significantly, they can be controllably obtained by adjusting the solute concentration during crystal growth. Specifically, the square shape crystals, α-[Pd₃L¹₆](PF₆)₁₂ in the cubic system with $I\overline{4}3m$ space group, can be isolated from a high-concentration solution of Pd₃L¹₆. Interestingly, a mesoporous cage assembled from eight Pd₃L¹₆ units with a diameter of 24 Å is observed in the crystal structure. For the low-concentration solution of Pd₃L¹₆, the rectangular shape crystals β-[Pd₃L¹₆](PF₆)₁₂ are obtained, which crystallize in the hexagonal system with P6₃/m space group, and display two-dimension packing pattern and one-dimension mesoporous channels (diameter ca. 22 Å) along the c axis. Moreover, the two supramolecular isomers were used as nanoporous reactors to induce the specific formation of polyiodides with different compositions and shapes as evidenced from single crystal X-ray diffraction studies. These findings provide a reference in targeting functional crystalline mesoporous supramolecular materials from a single complex building unit.