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Realizing the reversible transformation of the supramolecular hydrogels is essential for their application as smart materials. The reversible sol‐gel transition of the polypseudorotaxane (PPR) hydrogels is achieved through adding a CO2‐switchable guest molecule into the PPR hydrogel of poly(ethylene glycol) (PEG) and α‐cyclodextrins (α‐CDs). Alternating treatments with CO2 and heating drive such reversible...
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