Flexible devices are garnering substantial interest owing to their potential for wearable and portable applications. Here, flexible and self‐powered photodetector arrays based on all‐inorganic perovskite quantum dots (QDs) are reported. CsBr/KBr‐mediated CsPbBr3 QDs possess improved surface morphology and crystallinity with reduced defect densities, in comparison with the pristine ones. Systematic material characterizations reveal enhanced carrier transport, photoluminescence efficiency, and carrier lifetime of the CsBr/KBr‐mediated CsPbBr3 QDs. Flexible photodetector arrays fabricated with an optimum CsBr/KBr treatment demonstrate a high open‐circuit voltage of 1.3 V, responsivity of 10.1 A W−1, specific detectivity of 9.35 × 1013 Jones, and on/off ratio up to ≈104. Particularly, such performance is achieved under the self‐powered operation mode. Furthermore, outstanding flexibility and electrical stability with negligible degradation after 1600 bending cycles (up to 60°) are demonstrated. More importantly, the flexible detector arrays exhibit uniform photoresponse distribution, which is of much significance for practical imaging systems, and thus promotes the practical deployment of perovskite products.
A facile and controllable low-temperature (450 °C) route is reported to produce ultra-small Co3O4/Co nanoparticles in nitrogen-doped hyperporous graphenic networks (Co3O4/Co@N-G-450). Firstly, a monolayer of ZIF-67 nanocrystals is directly grown in thermal-shock exfoliated graphene networks (EGO) of suitable porosity and pore-widths. Later, the ZIF-67 is etched by targeting the small concentrations of residual oxygen functionalities on EGO (≈13 atom%) under a nitrogen atmosphere at 450 °C. Therefore, the partial gasification of ZIF-67 followed by oxidation of the resultant open cobalt metal centres produces a highly active nanophase of Co3O4/Co@N-G in a mass yield of >65 wt%. The as-synthesised Co3O4/Co@N-G-450 catalyst, without any further acid washing or oxidation process, exhibits an outstanding ORR performance with a high onset (0.962 V vs. RHE) and half-wave (0.808 V vs. RHE) potential as well as limiting current density (5.2 mA cm−2) in 0.1 M KOH solution. These merits are comparable to those of commercial Pt/C and many ZIF-derived catalysts, synthesised under extended and complex chemical treatment. Moreover, the catalyst also exhibits fast reaction kinetics with a dominant 4-electron reaction pathway and high durability.
Methane, the main component of natural and shale gas, is a significant carbon source for chemical synthesis. The direct partial oxidation of methane to liquid oxygenates under mild conditions1–3 is an attractive pathway, but the inertness of the molecule makes it challenging to achieve simultaneously high conversion and high selectivity towards a single target product. This difficulty is amplified when aiming for more valuable products that require C–C coupling4,5. Whereas selective partial methane oxidation processes1–3,6–9 have thus typically generated C1 oxygenates6,7, recent reports have documented photocatalytic methane conversion to the C2 oxygenate ethanol with low conversions but good-to-high selectivities4,5,8–12. Here we show that the intramolecular junction photocatalyst covalent triazine-based framework-1 with alternating benzene and triazine motifs13,14 drives methane coupling and oxidation to ethanol with a high selectivity and significantly improved conversion. The heterojunction architecture not only enables efficient and long-lived separation of charges after their generation, but also preferential adsorption of H2O and O2 to the triazine and benzene units, respectively. This dual-site feature separates C–C coupling to form ethane intermediates from the sites where •OH radicals are formed, thereby avoiding over-oxidation. When loaded with Pt to further boost performance, the molecular heterojunction photocatalyst generates ethanol in a packed-bed flow reactor with greatly improved conversion that results in an apparent quantum efficiency of 9.4%. We anticipate that further developing the ‘intramolecular junction’ approach will deliver efficient and selective catalysts for C–C coupling, pertaining, but not limited, to methane conversion to C2+ chemicals.
Robust superhydrophobic surfaces were fabricated via aerosol-assisted CVD of epoxy resins and PDMS polymer films. The as-obtained surfaces showed thermo-triggered healing of the superhydrophobicity by recovery of roughness structures.