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Although ferroelectric materials exhibit large pyroelectric coefficients, their pyroelectric figures of merit (FOMs) are severely limited by their high dielectric constants because of the inverse relationship between FOMs and dielectric constant. Here, we report the molecular ferroelectric [Hdabco]ClO4 and [Hdabco]BF4 (dabco = diazabicyclo[2.2.2]octane) exhibiting improper ferroelectric behavior and pyroelectric FOMs outperforming the current ferroelectrics. Concurrently, the improper molecular ferroelectrics have pyroelectric coefficients that are more than one order of magnitude greater than the state-of-the-art pyroelectric Pb(Mg1/3Nb2/3)O3-PbTiO3. Our first-principles and thermodynamic calculations show that the strong coupling between the order parameters, i.e., the rotation angle of anions and polarization, is responsible for the colossal pyroelectric coefficient of the molecular ferroelectrics. Along with the facile preparation and self-poling features, the improper molecular ferroelectrics hold great promise for high-performance pyroelectric devices.

Currently, various electronic devices make our life more and more safe, healthy, and comfortable, but at the same time, they produce a large amount of nondegradable and nonrecyclable electronic waste that threatens our environment. In this work, we explore an environmentally friendly and flexible mechanical sensor that is biodegradable and recyclable. The sensor consists of a bacterial cellulose (BC) hydrogel as the matrix and imidazolium perchlorate (ImClO 4 ) molecular ferroelectric as the functional element, the hybrid of which possesses a high sensitivity of 4 mV kPa −1 and a wide operational range from 0.2 to 31.25 kPa, outperforming those of most devices based on conventional functional biomaterials. Moreover, the BC hydrogel can be fully degraded into glucose and oligosaccharides, while ImClO 4 can be recyclable and reused for the same devices, leaving no environmentally hazardous electronic waste.