SCIENCE CHINA Materials•2026•DOI: 10.1007/s40843-026-4498-7
Two-dimensional porphyrin-based hypercrosslinked polymers (TPP-HCPs) were synthesized via room-temperature interfacial polymerization using 5,10,15,20-tetraphenylporphyrin and 1,3,5-trioxane. The resulting TPP-HCPs exhibited a BET surface area of 548 m2 g-1 and a CO2 uptake of 7.97 wt% at 1 bar and 298 K. CuO/TPP-HCPs nanospheres were fabricated by thermal conversion of Cu(NO3)2·3H2O in DMF at 135 °C, using TPP-HCPs as dynamic templates. This in-situ strategy generated CuO nanoparticles within the conjugated porous matrix, facilitating electron transfer and enhancing CO2 access to catalytic centers. In CO2 electroreduction, the composite achieved a total gas Faradaic efficiency exceeding 90% at ~500 mA cm-2 (-1.4 V vs. RHE), with 40.9% for C2H4, 8.2% for CH4, 31.9% for CO, and 12.3% for H2. The catalyst maintained stability over 24 h in an H-cell. These results demonstrate that 2D conjugated polymer-templated catalysts can sustain high-rate CO2 conversion to value-added products, offering a viable route for industrial CO2 utilization.
SCIENCE CHINA Materials•2025•DOI: 10.1007/s40843-025-3593-5
Organic ultrathin crystals, comprising monolayers or a few molecular layers, exhibit outstanding optoelectronic properties and have shown great promise for constructing advanced functional neuromorphic devices. However, scalable growth of high-quality organic ultrathin crystals and their seamless concurrent integration with charge trapping layers for multi-mode neuromorphic devices, that required in future high-density neuromorphic integration, remain challenging. Here, we present a scalable one-step fabrication strategy based on solution shearing, where spontaneous vertical phase separation of a small-molecule/polymer (Ph-BTBT-10/PS) blend enables the simultaneous formation of high-quality ultrathin Ph-BTBT-10 crystals and an electret PS charge-trapping layer. The PS electret layer serves a dual function: it facilitates the formation of ultrathin, highly ordered Ph-BTBT-10 crystals; meanwhile, its gate-tunable electron-trapping capability enables dynamic switching between photo-switching and photo-synaptic modes within a single device. As a photodetector, the device exhibits exceptional performance, including a responsivity of 4.7 × 10^4 A/W, specific detectivity of 2.2 × 10^17 Jones, and photosensitivity of 1.5 × 10^8. Under negative gate bias, light-triggered switching behavior enables logic gate demonstration, while under positive gate modulation, photonic synaptic behavior successfully emulates key biological functions, including excitatory post-synaptic current (EPSC), paired-pulse facilitation (PPF), short-term plasticity (STP) to long-term plasticity (LTP) transition, dynamic learning-forgetting processes, and image processing. Moreover, the system exhibits excellent compatibility with low-voltage flexible substrates and further demonstrates its application in low-consumption flexible neuromorphic devices. This work provides a scalable route toward high-performance, multifunctional neuromorphic optoelectronics based on organic ultrathin crystals, and advances the integration of flexible electronics and brain-inspired computing.