▎ 摘　　要

The pH of sweat is the most common biochemical parameter monitored by integrated wearable devices. A crucial factor in sensing materials for wearable applications is strong contact both with the skin and with the electrode substrate. Currently, the deposition of many sensitive materials on a substrate relies on mixing a small amount of binder, which raises the issue of biocompatibility and the risk of detachment. Herein, we report self-adhesive tannin-graphene supramolecular aggregates for use in wearable potentiometric pH sensors. The abundant phenolic hydroxyl groups in tannin (TA) result in strong adhesion and are also the pH response sites. The graphene (reduced graphene oxide, RGO) induces the supramolecular formation of TA and promotes electron transfer based on the 7C-7C conjugation interaction. The pH sensor has a reversible and Nernstian response, and is not affected by potentially interfering ions. Owing to the strong adhesion of TA-RGO, a wearable pH device was directly fabricated using a dispensing printing technique. The sensor has been shown to be successful in monitoring the pH of sweat in real time. This work emphasizes the importance of the adhesion of sensing materials for use in wearable electrochemical sensors.