Molecule–Graphene Hybrid Materials with Tunable Mechanoresponse: Highly Sensitive Pressure Sensors for Health Monitoring

The development of pressure sensors is crucial for the implementation of electronic skins and for health monitoring integrated into novel wearable devices. Tremendous effort is devoted toward improving their sensitivity, e.g., by employing microstructured electrodes or active materials through cumbersome processes. Here, a radically new type of piezoresistive pressure sensor based on a millefeuille‐like architecture of reduced graphene oxide (rGO) intercalated by covalently tethered molecular pillars holding on‐demand mechanical properties are fabricated. By applying a tiny pressure to the multilayer structure, the electron tunnelling ruling the charge transport between successive rGO sheets yields a colossal decrease in the material's electrical resistance. Significantly, the intrinsic rigidity of the molecular pillars employed enables the fine‐tuning of the sensor's sensitivity, reaching sensitivities as high as 0.82 kPa−1 in the low pressure region (0–0.6 kPa), with short response times (≈24 ms) and detection limit (7 Pa). The pressure sensors enable efficient heartbeat monitoring and can be easily transformed into a matrix capable of providing a 3D map of the pressure exerted by different objects. Toward highly performing piezoresistive pressure sensors, a radically new type of sensor based on reduced graphene oxide is demonstrated. Functionalization of graphene oxide with flexible molecular springs allows generation of devices featuring high sensitivity, short response time, and ultralow detection limit, which can be applied to health monitoring and 3D mapping of the pressure.