Preparation of CO 2 ‐Based Peelable Adhesives Featuring Fully Cross‐Linked Networks via Metal‐Chelate Cross‐Link and Dual‐Curing Process

ABSTRACT This work presents a green, high‐performance, residue‐free, UV‐induced peelable pressure‐sensitive adhesive (UV‐P‐PSA) featuring a fully cross‐linked network, developed via an orthogonal heat–light dual‐curing strategy. A CO 2 ‐based poly(propylene carbonate) diol bearing pendant allyl groups (PPCAGE) was synthesized and converted into a polyurethane acrylate (PPCAGE‐DMPA‐PUA) carrying both unsaturated side chains and carboxyl groups, which was formulated with a carboxyl‐containing polyacrylate, a multifunctional acrylate, and aluminum acetylacetonate (AlACA). The formulated adhesive mixture exhibits a storage‐stable pot life of at least 7 days without gelation, retaining its coatability for tape processing; after coating and oven drying, carboxyl–Al chelation establishes the tacky film, while UV curing polymerizes the pendant and terminal C=C groups, collapsing both the true interfacial contact area (Sa rising from ~1 to 12.75–18.28 μm) and the viscoelastic dissipation ( G′ increasing more than three orders of magnitude). The optimized adhesive delivers a 180° peel strength of 20.67 N/25 mm before UV curing, which drops to 0.01 N/25 mm after UV curing with no residue and no brittle fracture. By exploiting the intrinsic photoreactivity of a CO 2 ‐based polyol and an orthogonal dual‐curing chemistry, this design offers a sustainable, process‐compatible route to on‐demand peelable adhesives for advanced electronics manufacturing.