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Simply introducing four viologen units to a tetraphenylmethane framework causes the corresponding viologen radical cation to strongly dimerize intermolecularly, with the apparent equilibrium constant being increased by at least 7600 times, which drives the tetrahedral molecule to self-assemble into a three-dimensional (3D) supramolecular architecture in water.

Graphical abstract: A three-dimensional cross-linking supramolecular polymer stabilized by the cooperative dimerization of the viologen radical cation

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