Although three-dimensional metal halide perovskite (ABX3) single crystals are promising next-generation materials for radiation detection, state-of-the-art perovskite X-ray detectors include methylammonium as A-site cations, limiting the operational stability. Previous efforts to improve the stability using formamidinium–caesium-alloyed A-site cations usually sacrifice the detection performance because of high trap densities. Here we successfully solve this trade-off between stability and detection performance by synergistic composition engineering, where we include A-site alloys to decrease the trap density and B-site dopants to release the microstrain induced by A-site alloying. As such, we develop high-performance perovskite X-ray detectors with excellent stability. Our X-ray detectors exhibit high sensitivity of (2.6 ± 0.1) × 104 μC Gyair−1 cm−2 under 1 V cm−1 and ultralow limit of detection of 7.09 nGyair s−1. In addition, they feature long-term operational stability over half a year and impressive thermal stability up to 125 °C. We further demonstrate the promise of our perovskite X-ray detectors for low-bias portable applications with high-quality X-ray imaging and monitoring prototypes.

The 8-layered shifted hexagonal perovskite compound Ba8ZnNb6O24 was isolated via controlling the ZnO volatilization, which features long-range B-cation ordering with nanometer-scale separation by ∼1.9 nm of octahedral d(10) cationic (Zn(2+)) layers within the purely corner-sharing octahedral d(0) cationic (Nb(5+)) host. The long-range ordering of the B-site vacancy and out-of-center distortion of the highly-charged d(0) Nb(5+) that is assisted by the second-order Jahn-Teller effect contribute to this unusual B-cation ordering in Ba8ZnNb6O24. A small amount (∼15%) of d(10) Sb(5+) substitution for Nb(5+) in Ba8ZnNb6-xSbxO24 dramatically transformed the shifted structure to a twinned structure, in contrast with the Ba8ZnNb6-xTaxO24 case requiring 50% d(0) Ta(5+) substitution for Nb(5+) for such a shift-to-twin transformation. Multiple factors including B-cationic sizes, electrostatic repulsion forces, long-range ordering of B-site vacancies, and bonding preferences arising from a covalent contribution to the B-O bonding that includes out-of-center octahedral distortion and the B-O-B bonding angle could subtly contribute to the twin-shift phase competition of B-site deficient 8-layered hexagonal perovskites Ba8B7O24. The ceramics of new shifted Ba8ZnNb6O24 and twinned Ba8ZnNb5.1Sb0.9O24 compounds exhibited good microwave dielectric properties (εr ∼ 35, Qf ∼ 36 200-43 400 GHz and τf ∼ 38-44 ppm/°C).

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Novel PtCu alloy yolk-shell cubes were fabricated via the disproportionation and displacement reactions in Cu2O yolk-shell cubes, and they exhibit significantly improved catalytic activity and durability for methanol electrooxidation.

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