Wearable devices hold significant potential in healthcare and medical diagnostics. One major challenge in realizing this potential is the low barrier property of polymer substrates, which fail to withstand surrounding moisture and biofluids. In this work, a two-step strategy involving ALI followed by a UV-curing process is developed to fabricate a K48PDMS/Al2O3 ultra-barrier with high barrier property of 7.82 × 10-5 g m-2 day-1 under stretching strain, representing one of the highest values among current works. Moreover, the K48PDMS/Al2O3 barrier enables Ca-tested devices to exhibit extended operational lifetimes of up to 12 days in simulated rain. It also ensures the high sensitivity of strain sensors for real-time monitoring of health-related physiological signals, even when exposed to aggressive solutions such as PBS, KOH, and glucose. A clear "filling-cross-linking" mechanism is revealed, involving the filling of the void spaces within polymer chains followed by the cross-linking of polymer side chains to enhance the density of the hybrid layer. Adjusting porosity and functional group density ensures complete Al2O3 infiltration into the polymer. The cross-linking increases from 12.31% to 73.79% compared to the UV-curing process alone due to the presence of Al2O3, further enhancing the density of the hybrid layer and its barrier properties. The proposed strategy in our work shows great potential for providing highly reliable encapsulation for wearable electronics.
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