PhD ceremony Mr. J. Li: Self-assembly in complex chemical systems

PhD ceremony: Mr. J. Li

Dissertation: Self-assembly in complex chemical systems

Promotor(s): prof. S. Otto

Faculty: Mathematics and Natural Sciences

In this thesis, we used the tool of dynamic combinatorial chemistry (DCC) to fabricate complex synthetic systems and investigated self-assembly of molecules in these chemical systems. In Chapter 1, we introduced the fundamental principles behind the subject of DCC and reviewed the current state of art in DCC. We concluded that there is still plenty of room for further development. In Chapter 2, upon the addition of a template into a library prepared from a disulfide building block, a family of catenanes was produced by interlocking macrocycles of building blocks with ring like templates. A method for quantitative assessment of equilibrium constants for catenane was developed which is potentially applicable to any catenanes containing dynamic covalent bonds. In Chapter 3, simultaneous use of two templates in one single library yielded complex systems where a Russian-doll like termolecular complex was obtained through a process of simultaneous casting and molding. Since there are only limited examples of self-replication dynamic combinatorial libraries (DCLs), in Chapter 4 and Chapter 5 we showed two different systems which revealed that the self-assembly in DCLs may drive the occurrence of self-replication. As a result of self-assembly, self-synthesizing materials should be explored using DCC. Based on this point, In Chapter 6 and Chapter 7, two hydrogels were developed in DCLs. The contribution of each of these chapters was put into perspective and prospects for self-assembly in complex chemical systems were discussed in Chapter