The rising demand for radiation detection materials in many applications has led to extensive research on scintillators. The ability of a scintillator to absorb high-energy (kiloelectronvolt-scale) X-ray photons and convert the absorbed energy into low-energy visible photons is critical for applications in radiation exposure monitoring, security inspection, X-ray astronomy and medical radiography. However, conventional scintillators are generally synthesized by crystallization at a high temperature and their radioluminescence is difficult to tune across the visible spectrum. Here we describe experimental investigations of a series of all-inorganic perovskite nanocrystals comprising caesium and lead atoms and their response to X-ray irradiation. These nanocrystal scintillators exhibit strong X-ray absorption and intense radioluminescence at visible wavelengths. Unlike bulk inorganic scintillators, these perovskite nanomaterials are solution-processable at a relatively low temperature and can generate X-ray-induced emissions that are easily tunable across the visible spectrum by tailoring the anionic component of colloidal precursors during their synthesis. These features allow the fabrication of flexible and highly sensitive X-ray detectors with a detection limit of 13 nanograys per second, which is about 400 times lower than typical medical imaging doses. We show that these colour-tunable perovskite nanocrystal scintillators can provide a convenient visualization tool for X-ray radiography, as the associated image can be directly recorded by standard digital cameras. We also demonstrate their direct integration with commercial flat-panel imagers and their utility in examining electronic circuit boards under low-dose X-ray illumination.
The components with soft nature in the metal halide perovskite absorber usually generate lead (Pb)0 and iodine (I)0 defects during device fabrication and operation. These defects serve as not only recombination centers to deteriorate device efficiency but also degradation initiators to hamper device lifetimes. We show that the europium ion pair Eu3+-Eu2+ acts as the “redox shuttle” that selectively oxidized Pb0 and reduced I0 defects simultaneously in a cyclical transition. The resultant device achieves a power conversion efficiency (PCE) of 21.52% (certified 20.52%) with substantially improved long-term durability. The devices retained 92% and 89% of the peak PCE under 1-sun continuous illumination or heating at 85°C for 1500 hours and 91% of the original stable PCE after maximum power point tracking for 500 hours, respectively.
Electrocatalysis by atomic catalysts is a major focus of chemical and energy conversion effort. Although transition-metal-based bulk electrocatalysts for electrochemical application on energy conversion processes have been reported frequently, anchoring the stable transition-metal atoms (e.g. nickel and iron) still remains a practical challenge. Here we report a strategy for fabrication of ACs comprising only isolated nickel/iron atoms anchored on graphdiyne. Our findings identify the very narrow size distributions of both nickel (1.23 Å) and iron (1.02 Å), typical sizes of single-atom nickel and iron. The precision of this method motivates us to develop a general approach in the field of single-atom transition-metal catalysis. Such atomic catalysts have high catalytic activity and stability for hydrogen evolution reactions.
Current X-ray imaging technologies involving flat-panel detectors have difficulty in imaging three-dimensional (3D) objects because fabrication of large-area, flexible silicon-based photodetectors on highly curved surfaces remains a challenge 1-3 . Here we demonstrate ultralong-lived X-ray trapping for flat-panel-free, high-resolution 3D imaging using a series of solution-processable, lanthanide-doped nanoscintillators. Corroborated with quantum mechanical simulation, our experimental characterizations show that a thermally activated slow-hopping of trapped electrons, due to radiation-induced anionic migration in host lattices, induces more than 30 days of persistent radioluminescence. We further demonstrate X-ray luminescence extension imaging (Xr-LEI) with >20-lp/mm resolution and >15-day optical memory. These findings provide insight into mechanisms underlying X-ray energy conversion through enduring electron trapping and also offer a new paradigm to motivate future research in wearable X-ray detectors for patient-centered radiography and mammogram, imaging-guided therapeutics, high-energy physics, and deep learning in radiology.
The emergence of zerovalent atom catalysts has been highly attractive for catalytic science. For many years, scientists have explored the stability of zerovalent atom catalysts and demonstrated their unique properties. Here, we describe an atom catalyst (AC) with atomically dispersed zerovalent molybdenum atoms on graphdiyne (Mo 0 /GDY) with a high mass content of Mo atoms (up to 7.5 wt %) that was synthesized via a facile and scalable process. The catalyst shows both excellent selectivity and activity in the electrochemical reduction of nitrogen and in the hydrogen evolution reaction in aqueous solutions at room temperature and pressure. It is noted that this catalyst is the first bifunctional AC for highly efficient and selective ammonia and hydrogen generation. The catalytic process of our catalyst is well understood, the structure is defined, and the performance is excellent, providing a solid foundation for the generation and application of the new generation of catalysts.
Pursuing active and durable water splitting electrocatalysts is of vital significance for solving the sluggish kinetics of the oxygen evolution reaction (OER) process in energy supply. Herein, theoretical calculations identify that the local distortion-strain effect in amorphous RuTe2 system abnormally sensitizes the Te-pπ coupling capability and enhances the electron-transfer of Ru-sites, in which the excellent inter-orbital p-d transfers determine strong electronic activities for boosting OER performance. Thus, a robust electrocatalyst based on amorphous RuTe2 porous nanorods (PNRs) is successfully fabricated. In the acidic water splitting, a-RuTe2 PNRs exhibit a superior performance, which only require a cell voltage of 1.52 V to reach a current density of 10 mA cm−2. Detailed investigations show that the high density of defects combine with oxygen atoms to form RuOxHy species, which are conducive to the OER. This work offers valuable insights for constructing robust electrocatalysts based on theoretical calculations guided by rational design and amorphous materials.
Simultaneous realization of improved activity, enhanced stability, and reduced cost remains a desirable yet challenging goal in the search of electrocatalysis oxygen evolution reaction (OER) in acid. Herein, we report a novel strategy to prepare iridium single-atoms (Ir-SAs) on ultrathin NiCo2O4 porous nanosheets (Ir–NiCo2O4 NSs) by the co-electrodeposition method. The surface-exposed Ir-SAs couplings with oxygen vacancies (VO) exhibit boosting the catalysts OER activity and stability in acid media. They display superior OER performance with an ultralow overpotential of 240 mV at j = 10 mA cm–2 and long-term stability of 70 h in acid media. The TOFs of 1.13 and 6.70 s–1 at an overpotential of 300 and 370 mV also confirm their remarkable performance. Density functional theory (DFT) calculations reveal that the prominent OER performance arises from the surface electronic exchange-and-transfer activities contributed by atomic Ir incorporation on the intrinsic VO existed NiCo2O4 surface. The atomic Ir sites substantially elevate the electronic activity of surface lower coordinated Co sites nearby VO, which facilitate the surface electronic exchange-and-transfer capabilities. With this trend, the preferred H2O activation and stabilized *O have been reached toward competitively lower overpotential. This is a generalized key for optimally boosting OER performance.
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