One of the key challenges in two-dimensional (2D) materials is to go beyond graphene, a prototype 2D polymer (2DP), and to synthesize its organic analogues with structural control at the atomic- or molecular-level. Here we show the successful preparation of porphyrin-containing monolayer and multilayer 2DPs through Schiff-base polycondensation reaction at an air–water and liquid–liquid interface, respectively. Both the monolayer and multilayer 2DPs have crystalline structures as indicated by selected area electron diffraction. The monolayer 2DP has a thickness of∼0.7 nm with a lateral size of 4-inch wafer, and it has a Young’s modulus of 267±30 GPa. Notably, the monolayer 2DP functions as an active semiconducting layer in a thin film transistor, while the multilayer 2DP from cobalt-porphyrin monomer efficiently catalyses hydrogen generation from water. This work presents an advance in the synthesis of novel 2D materials for electronics and energy-related applications.

We boost the ORR performance of Fe–N–C electrocatalysts in acids by engineering highly accessible and dense surface single metal FeN₄ active sites.

Engineering conducting polymer thin films with morphological homogeneity and long-range molecular ordering is intriguing to achieve high-performance organic electronics. Polyaniline (PANI) has attracted considerable interest due to its appealing electrical conductivity and diverse chemistry. However, the synthesis of large-area PANI thin film and the control of its crystallinity and thickness remain challenging because of the complex intermolecular interactions of aniline oligomers. Here we report a facile route combining air-water interface and surfactant monolayer as templates to synthesize crystalline quasi-two-dimensional (q2D) PANI with lateral size ~50 cm² and tunable thickness (2.6–30 nm). The achieved q2D PANI exhibits anisotropic charge transport and a lateral conductivity up to 160 S cm⁻¹ doped by hydrogen chloride (HCl). Moreover, the q2D PANI displays superior chemiresistive sensing toward ammonia (30 ppb), and volatile organic compounds (10 ppm). Our work highlights the q2D PANI as promising electroactive materials for thin-film organic electronics.