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Controlling the conformational transition of polypeptides under slightly acidic environment is challenging. Herein, we report a class of pH‐responsive helix‐to‐coil conformationally transitionable polypeptides (pCTPs) by simply conjugating tertiary amine groups (TAs) to polylysine. Their conformation is highly dependent on the charge state of TAs, showing a helical structure when most TAs are deprotonated...
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