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J Am Chem Soc. 2016 Apr 13;138(14):4927-37. doi: 10.1021/jacs.6b01089. Epub 2016 Mar 29.

Construction of Smart Supramolecular Polymeric Hydrogels Cross-linked by Discrete Organoplatinum(II) Metallacycles via Post-Assembly Polymerization.

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Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University , Shanghai 200062, People's Republic of China.
The State Key Laboratory of Molecular Engineering of Polymers and Department of Macromolecular Science, Fudan University , Shanghai 200433, People's Republic of China.
Department of Chemistry and Biochemistry & Materials Science, Engineering, and Commercialization Program, Texas State University , San Macros, Texas 78666, United States.
Key Laboratory of Colloid, Interface and Chemical Thermodynamics, Institute of Chemistry, The Chinese Academy of Sciences , Beijing 100080, People's Republic of China.


Postassembly modification strategy has been successfully employed in the construction of discrete metallosupramolecular assemblies. However, the most known reports have been limited to the simple structural conversion through the easy covalent reactions, thus hindering the development of organometallic functional materials. In this study, we first combined coordination-driven self-assembly and postassembly reversible addition-fragmentation chain-transfer (RAFT) polymerization to produce a new family of star supramolecular polymers containing well-defined metallacycles as cores, which featured typical lower critical solution temperature (LCST) behavior in water because of the existence of poly(N-isopropylacrylamide) (PNIPAAM) moieties. Moreover, the obtained star polymers could further form supramolecular hydrogels cross-linked by discrete hexagonal metallacycles at room temperature without heating-cooling process. Interestingly, the resultant polymeric hydrogels exhibited stimuli-responsive behavior toward temperature and bromide anion as well as self-healing property. We demonstrated that the dynamic nature of Pt-N bonds in the hexagonal metallacycles played an important role in determining the stimuli-responsive and self-healing property of the final soft matters. Thus, merging coordination-driven self-assembly and postassembly polymerization provided a new avenue to the preparation of functional materials containing well-defined, discrete metal-organic assemblies as main scaffolds.


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