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A toolbox of living coordination polymerization methods based on CPAM group 4 metal initiators has been applied for the stereomodulation of poly(4‐methyl‐1‐pentene) (PMP) tacticity to provide new fundamental forms in which thermal phase transitions, Tg and Tm, can be adjusted over a wide range. Also reported for the first time are the synthesis and properties of authenticated 1,2‐regioregular atactic...
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