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The one‐step efficient separation of high‐purity C2H4 from C2H4/C2H6 mixtures by hydrogen‐bonded organic frameworks (HOFs) faces two problems: lack of strategies for constructing stable pores in HOFs and how to obtain high C2H6 selectivity. Herein, we have developed a microporous Mortise‐Tenon‐type HOF (MTHOF‐1, MT is short for Mortise‐Tenon structure) with a new self‐assembly mode for C2H4/C2H6 separation. Unlike previous HOFs which usually possess discrete head‐to‐head hydrogen bonds, MTHOF‐1 is assembled by unique consecutive side‐by‐side hydrogen bonds, which result in mortise‐and‐tenon pores decorated with orderly arranged amide groups and benzene rings. As expected, MTHOF‐1 exhibits excellent stability under various conditions and shows clear separation trends for C2H6/C2H4. The IAST selectivity is as high as 2.15 at 298 K. More importantly, dynamic breakthrough experiments have demonstrated that MTHOF‐1 can effectively separate the C2H6/C2H4 feed gas to obtain polymer‐grade C2H4 in one step even under high‐humidity conditions. [ABSTRACT FROM AUTHOR]

H2O2 is a widely used eco‐friendly oxidant and a potential energy carrier. Photocatalytic H2O2 production from water and O2 is an ideal approach with the potential to address the current energy crisis and environmental issues. Three zig‐zag two‐dimensional coordination polymers (2D CPs), named CuX‐dptz, were synthesized by a rapid and facile method at room temperature, showing preeminent H2O2 photoproduction performance under pure water and open air without any additives. CuBr‐dptz exhibits a H2O2 production rate high up to 1874 μmol g−1 h−1, exceeding most reported photocatalysts under this condition, even comparable to those supported by sacrificial agents and O2. The coordination environment of Cu can be modulated by halogen atoms (X=Cl, Br, I), which in turn affects the electron transfer process and finally determines the reaction activity. This is the first time that 2D CPs have been used for photocatalytic H2O2 production in such challenging conditions, which provides a new pathway for the development of portable in situ H2O2 photosynthesis devices. [ABSTRACT FROM AUTHOR]

Ultra‐broadband near‐infrared (NIR) phosphor‐converted light‐emitting diodes (pc‐LEDs) have great application prospects in research and industrial fields. However, simultaneously achieving highly efficient and ultra‐broad NIR emission in phosphor material remains a challenge. Herein, an ultra‐broadband NIR emission in the range of 800–1200 nm with ultra‐high emission efficiency of up to 64.2% is first achieved by substituting the Sc3+ site in Cs2NaScCl6 perovskite single‐crystal with a Cr3+ ion. By combining the experimental results with first‐principles calculations, an efficient charge transfer sensitization process from host to Cr3+ is found to be the fundamental reason for the ultra‐high NIR emission efficiency. Benefiting from the excellent efficiency and superior chemical resistance to heat and UV radiation, an ultra‐broadband NIR pc‐LED made of this phosphor demonstrates great potential in biomedical imaging, nondestructive testing, and night‐vision devices. [ABSTRACT FROM AUTHOR]

For high‐power white light‐emitting diode devices (WLEDs), phosphor ceramics were widely used because of their high thermal conductivity and temperature resistance. In this study, Y2.998Al5O12: 0.002Ce3+ ceramics were prepared via vacuum reaction sintering and treated by silicon carbide (SiC) abrasives with particle sizes of 8.6, 20, 25, 34, and 50 μm to obtain a single textured surface. The transmittance, reflectance, luminous efficiency (LE) and photoluminescence (PL) intensity of the ceramics were investigated with various surface roughness and different placement. Compared with the double polished (DP) samples, the PL intensity and LE of the single‐surface textured ceramics were greatly improved. It was shown that the roughest ceramics placed with the single polished (SP) side facing the direction of the excitation light (the SP‐forward YAG: Ce ceramics) showed the best performance. [ABSTRACT FROM AUTHOR]

When hydrogels are in environments with high water content, they usually undergo swelling, leading to a degradation of mechanical properties, which severely limits their application in underwater sensing. To solve this problem, we synthesized an anti-swelling, tough, double-crosslinked, dual-network hydrogel, P(AA-SMA)-CMC-Na, for underwater sensing. Due to the hydrophobic association and electrostatic interactions between the cationic surfactant N-Hexadecyltrimethylammonium chloride (CTAC) and poly (acrylate-methacrylate octadecyl ester) [P(AA-SMA)], as well as the dense network structure brought about by double cross-linking and the incorporation of CMC-Na, the hydrogel has excellent anti-swelling properties and mechanical properties (large stretchability of 955%, tensile strength of 252 kPa). Notably, after seven days of immersion in water (pH = 3, 5) and saline, stress and strain were elevated compared to the original hydrogel (strain up to 1460% and stress up to 805 kPa after immersion). The dynamic hydrophobic association of CTAC with SMA and the large number of hydrogen bonds within the hydrogel contributed to the excellent self-healing efficiency of the hydrogel (90%). The hydrogel was fabricated into a flexible strain sensor that showed keen sensitivity in the sensing range of 0–400% (GF values of 1.55, 2.87, and 5.03 for the ranges of 0–200%, 200–300% and 300–400%, respectively). It could accurately detect real-time signals of human movement in air, underwater, and seawater. Therefore, the P(AA-SMA)-CMC-Na hydrogel can meet the needs of underwater sensing and have great potential for applications in electronic skin, personal health detection, and flexible wearable electronics. [ABSTRACT FROM AUTHOR]

Crystal-field perturbation is theoretically the most direct and effective method of achieving highly efficient photoluminescence from trivalent lanthanide (Ln3+) ions through breaking the parity-forbidden nature of their 4f-transitions. However, exerting such crystal-field perturbation remains an arduous task even in well-developed Ln3+-doped luminescent nanocrystals (NCs). Herein, we report crystal-field perturbation through interstitial H+-doping in orthorhombic-phase NaMgF3:Ln3+ NCs and achieve a three-orders-of-magnitude emission amplification without a distinct lattice distortion. Mechanistic studies reveal that the interstitial H+ ions perturb the local charge density distribution, leading to anisotropic polarization of the F− ligand, which affects the highly symmetric Ln3+-substituted [MgF6]4− octahedral clusters. This effectively alleviates the parity-forbidden selective rule to enhance the 4f–4 f radiative transition rate of the Ln3+ emitter and is directly corroborated by the apparent shortening of the radiative recombination lifetime. The interstitially H+-doped NaMgF3:Yb/Er NCs are successfully used as bioimaging agents for real-time vascular imaging. These findings provide concrete evidence for crystal-field perturbation effects and promote the design of Ln3+-doped luminescent NCs with high brightness. Lanthanide-doped inorganic nanocrystals are promising for optical imaging and biomedical applications. Here authors show that interstitial H+ doping-induced crystal-field perturbation enhances the photoluminescence intensity of lanthanide-doped inorganic nanocrystals. [ABSTRACT FROM AUTHOR]

Self-trapped excitons (STEs) emission from halide perovskites with strong exciton-phonon coupling has attracted considerable attention due to the widespread application in optoelectronic devices. Nevertheless, the in-depth understanding of the relationship between exciton-phonon coupling and luminescence intensity remains incomplete. Herein, a doping-enhanced exciton-phonon coupling effect is observed in Cs3Cu2I5 nanocrystals (NCs), which leads to a remarkable increasement of their STEs emission efficiency. Mechanism study shows that the hetero-valent substitution of Cu+ with alkaline-earth metal ions (AE2+) causes a greater degree of Jahn–Teller distortion between the ground state and excited state structures of [Cu2I5]3− clusters as evidenced by our spectral analysis and first-principles calculations. As a consequence, an X-ray detector based on these Cs3Cu2I5:AE NCs delivers an X-ray imaging resolution of up to 10 lp·mm−1 and a low detection limit of 0.37 µGyair·s−1, disclosing the potential of doping-enhanced exciton-phonon coupling effect in improving STEs-emission and practical application for X-ray imaging. [ABSTRACT FROM AUTHOR]

Hexagonal-phase NaYF4 (β-NaYF4) has been acknowledged to be one of the most efficient doping hosts to prepare bright lanthanide-doped luminescent nano-bioprobes for various biomedical applications. However, to date, it remains a great challenge to synthesize ultra-bright lanthanide-doped β-NaYF4 nano-bioprobes under a low reaction temperature by using conventional synthetic methods. Herein, we first develop an acetic acid (HAc)-mediated coprecipitation method for the preparation of ultra-bright lanthanide-doped β-NaYF4 nanoprobes under a low reaction temperature at 200 °C. Based on a series of comparative spectroscopic investigations, we show that the use of HAc in the reaction environment can not only promote the rapid α–β phase transformation of NaYF4 host at 200 °C within 1 h but also boost the absolute photoluminescence quantum yield (PLQY) of NaYF4 nanocrystals to 30.68% for near-infrared emission and to 3.79% for upconversion luminescence, both of which are amongst the highest values for diverse lanthanide-doped luminescent nanocrystals ever reported. By virtue of their superior near-infrared luminescence, we achieve optical-guided dynamic vasculature imaging in vivo of the whole body at a high spatial resolution (23.8 µm) under 980 nm excitation, indicating its potential for the diagnosis and treatment evaluation of vasculature-related diseases. [ABSTRACT FROM AUTHOR]

Thermally activated delayed fluorescence (TADF) materials hold great promise as next‐generation efficient emitters due to their theoretical 100% internal quantum efficiency. However, such an intriguing photophysical mechanism is extremely rare in perovskites or their derivatives. Herein, the colloidal synthesis of two‐dimensional CsAgCl2 nanocrystals (NCs) with typical TADF feature is reported first. The TADF mechanism is investigated in detail by combining first‐principles calculations with experimental results, including temperature‐dependent spectral analysis and fs‐transient absorption spectra. A small singlet−triplet state splitting energy (0.082 eV) and a large spatial separation of charge density |Ψ|2 of valence band maximum and conduction band minimum are observed, which are prerequisites for TADF. Moreover, these CsAgCl2 NCs deliver an ultralow X‐ray detection limit of 170.5 nGyair s−1 and a high imaging resolution of 11.5 lp mm−1, much superior to the commercial scintillators. [ABSTRACT FROM AUTHOR]

Zero‐dimensional (0D) copper‐based perovskite‐derivative nano‐scintillators (NSs), as a promising non‐toxic alternative to lead‐based halide perovskite, have shown great potential in flexible X‐ray detection and imaging. However, their practical applications are still impeded by low X‐ray imaging resolution associated with inadequate radioluminescence (RL) and poor environmental stability. Herein, for the first time a simple but valid Mn2+‐activation strategy is proposed to highly enhance the RL and stability of 0D Cs3Cu2I5 NSs, where the Mn2+ ions are embedded into the highly localized [Cu2I5]3− units by utilizing a modified hot‐injection method. As such, a newly emerged emission band of Mn2+ ion centered at ≈562 nm coupled with much improved intrinsic self‐trapped excitons (STE) emission of the 0D Cs3Cu2I5 host peaking at ≈445 nm can be achieved in these resultant Mn2+‐activated 0D Cs3Cu2I5 NSs, thereby delivering a light yield of 71 000 photons MeV−1 that is much superior to their lead‐based perovskite counterparts and commercial scintillators. As a consequence, X‐ray detectors made of these Mn2+‐activated NSs implement an ultrahigh X‐ray imaging resolution of 16.2 line pairs mm−1 and an ultra‐low detection limit of 127.5 nGyair s−1, highlighting their potential as promising candidates for flexible X‐ray detection and imaging. [ABSTRACT FROM AUTHOR]