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Thermally rearranged (TR) polymers show unprecedented gas permeability and selectivity, exceeding the Robeson upper bound. Therefore, they have been widely considered as the material of choice for next-generation gas separation membranes. This chapter provides an overview of TR polymer development over the past decade. Details regarding the TR polymer structural design, synthesis routes, free volume topology, and gas permeation properties are given in this chapter. In addition, we address the industrial-scale implementation of TR polymer membranes.

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