Although perovskite nanocrystals have attracted considerable interests as emerging semiconductors in optoelectronic devices, design and fabrication of a deformable structure with high stability and flexibility while meeting the charge transport requirements remain a huge challenge. Herein, a combined soft‐hard strategy is demonstrated to fabricate intrinsically flexible all‐inorganic perovskite layers for photodetection via ligand cross‐linking. Perfluorodecyltrichlorosilane (FDTS) is employed as the capping ligand and passivating agent bound to the CsPbBr3 surface via Pb‐F and Br‐F interactions. The SiCl head groups of FDTS are hydrolyzed to produce SiOH groups which subsequently condense to form the SiOSi network. The CsPbBr3@FDTS nanocrystals (NCs) are monodispersed cubes with an average particle size of 13.03 nm and exhibit excellent optical stability. Furthermore, the residual hydroxyl groups on the surface of the CsPbBr3@FDTS render the NCs tightly packed and cross‐linked to each other to form a dense and elastic CsPbBr3@FDTS film with soft and hard components. The photodetector based on the flexible CsPbBr3@FDTS film exhibits outstanding mechanical flexibility and robust stability after 5000 bending cycles.
Shear stiffening gel (SSG) with prominent rate-dependent mechanical properties is promising for impact protection, but conventional boron-based SSG suffers from toxicity and corrosion arising from boric acid. Here, we design a boron-free supramolecular dynamic reversible network of polytitanosiloxane (PTS) based on the metal-ion-mediated hydrogen bonding enhancement strategy. Different oxidation states of Ti atoms in the network influence the charge distribution of the adjacent hydroxyl groups (Ti-OH). The electrostatic potential of the H-bond donor and acceptor could be effectively modulated by the Ti4+ and Ti3+ cations, thereby enhancing the H-bond strength. The resulting PTS SSG exhibits exceptional shear stiffening (~2800 times, 0.1–100 Hz), negligible corrosion, and low cytotoxicity (Grade 1). The PTS SSG is further explored for impact protection materials and flexible mechanical sensors in practice. The hydrogen bonding enhancement strategy also paves the way for developing dynamic reversible networks to fabricate next-generation smart materials.
15 July 2024 in ACS Applied Materials & Interfaces