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1.
Small ; 20(31): e2310431, 2024 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-38441366

RESUMEN

Innovative advances in the exploitation of effective electrocatalytic materials for the reduction of nitrogen (N2) to ammonia (NH3) are highly required for the sustainable production of fertilizers and zero-carbon emission fuel. In order to achieve zero-carbon footprints and renewable NH3 production, electrochemical N2 reduction reaction (NRR) provides a favorable energy-saving alternative but it requires more active, efficient, and selective catalysts. In current work, sulfur vacancy (Sv)-rich NiCo2S4@MnO2 heterostructures are efficaciously fabricated via a facile hydrothermal approach followed by heat treatment. The urchin-like Sv-NiCo2S4@MnO2 heterostructures serve as cathodes, which demonstrate an optimal NH3 yield of 57.31 µg h-1 mgcat -1 and Faradaic efficiency of 20.55% at -0.2 V versus reversible hydrogen electrode (RHE) in basic electrolyte owing to the synergistic interactions between Sv-NiCo2S4 and MnO2. Density functional theory (DFT) simulation further verifies that Co-sites of urchin-like Sv-NiCo2S4@MnO2 heterostructures are beneficial to lowering the energy threshold for N2 adsorption and successive protonation. Distinctive micro/nano-architectures exhibit high NRR electrocatalytic activities that might motivate researchers to explore and concentrate on the development of heterostructures for ambient electrocatalytic NH3 generation.

2.
Angew Chem Int Ed Engl ; 63(21): e202402634, 2024 May 21.
Artículo en Inglés | MEDLINE | ID: mdl-38466630

RESUMEN

Molecular ultralong room-temperature phosphorescence (RTP), exhibiting multiple stimuli-responsive characteristics, has garnered considerable attention due to its potential applications in light-emitting devices, sensors, and information safety. This work proposes the utilization of photochemical cascade processes (PCCPs) in molecular crystals to design a stepwise smart RTP switch. By harnessing the sequential dynamics of photo-burst movement (induced by [2+2] photocycloaddition) and photochromism (induced by photogenerated radicals) in a bismuth (Bi)-based metal-organic halide (MOH), a continuous and photo-responsive ultralong RTP can be achieved. Furthermore, utilizing the same Bi-based MOH, diverse application demonstrations, such as multi-mode anti-counterfeiting and information encryption, can be easily implemented. This work thus not only serves as a proof-of-concept for the development of solid-state PCCPs that integrate photosalient effect and photochromism with light-chemical-mechanical energy conversion, but also lays the groundwork for designing new Bi-based MOHs with dynamically responsive ultralong RTP.

3.
Angew Chem Int Ed Engl ; : e202412350, 2024 Aug 17.
Artículo en Inglés | MEDLINE | ID: mdl-39152766

RESUMEN

Zero-dimensional (0D) hybrid metal halides have been emerged as room-temperature phosphorescence (RTP) materials, but synchronous optimization of multiple phosphorescence performance in one structural platform remains less resolved, and stable RTP activity in aqueous medium is also unrealized due to serious instability toward water and oxygen. Herein, we demonstrated a photophysical tuning strategy in a new 0D hybrid zinc halide family of (BTPP)2ZnX4 (BTPP = benzyltriphenylphosphonium, X = Cl and Br). Infrequently, the delicate combination of organic and inorganic species enables this family to display multiple ultralong green afterglow and efficient self-trapped exciton (STE) associated cyan phosphorescence. Compared with inert luminescence of [BTPP]+ cation, incorporation of anionic [ZnX4]2- effectively enhance the spin-orbit coupling effect, which significantly boosts the photoluminescence quantum yield (PLQY) up to 30.66% and 54.62% for afterglow and phosphorescence, respectively. Synchronously, the corresponding luminescence lifetime extend to 143.94 ms and 0.308 µs surpassing the indiscernible phosphorescence of [BTPP]X salt. More importantly, this halide family presents robust RTP emission with nearly unattenuated PLQY in water and harsh condition (acid and basic aqueous solution) over half a year. The highly efficient integrated afterglow and STE phosphorescence as well as ultrahigh aqueous state RTP realize multiple anti-counterfeiting applications in wide chemical environments.

4.
Nat Commun ; 15(1): 5281, 2024 Jun 20.
Artículo en Inglés | MEDLINE | ID: mdl-38902239

RESUMEN

Long persistent luminescence (LPL) has gained considerable attention for the applications in decoration, emergency signage, information encryption and biomedicine. However, recently developed LPL materials - encompassing inorganics, organics and inorganic-organic hybrids - often display monochromatic afterglow with limited functionality. Furthermore, triplet exciton-based phosphors are prone to thermal quenching, significantly restricting their high emission efficiency. Here, we show a straightforward wet-chemistry approach for fabricating multimode LPL materials by introducing both anion (Br-) and cation (Sn2+) doping into hexagonal CsCdCl3 all-inorganic perovskites. This process involves establishing new trapping centers from [CdCl6-nBrn]4- and/or [Sn2-nCdnCl9]5- linker units, disrupting the local symmetry in the host framework. These halide perovskites demonstrate afterglow duration time ( > 2,000 s), nearly full-color coverage, high photoluminescence quantum yield ( ~ 84.47%), and the anti-thermal quenching temperature up to 377 K. Particularly, CsCdCl3:x%Br display temperature-dependent LPL and time-valve controllable time-dependent luminescence, while CsCdCl3:x%Sn exhibit forward and reverse excitation-dependent Janus-type luminescence. Combining both experimental and computational studies, this finding not only introduces a local-symmetry breaking strategy for simultaneously enhancing afterglow lifetime and efficiency, but also provides new insights into the multimode LPL materials with dynamic tunability for applications in luminescence, photonics, high-security anti-counterfeiting and information storage.

5.
Nat Commun ; 15(1): 5519, 2024 Jun 29.
Artículo en Inglés | MEDLINE | ID: mdl-38951508

RESUMEN

Dynamically responsive materials, capable of reversible changes in color appearance and/or photoemission upon external stimuli, have attracted substantial attention across various fields. This study presents an effective approach wherein switchable modulation of photochromism and ultralong phosphorescence can be achieved simultaneously in a zero-dimensional organic-inorganic halide hybrid glass doped with 4,4´-bipyridine. The facile fabrication of large-scale glasses is accomplished through a combined grinding-melting-quenching process. The persistent luminescence can be regulated through the photochromic switch induced by photo-generated radicals. Furthermore, the incorporation of the aggregation-induced chirality effect generates intriguing circularly polarized luminescence, with an optical dissymmetry factor (glum) reaching the order of 10-2. Exploiting the dynamic ultralong phosphorescence, this work further achieves promising applications, such as three-dimensional optical storage, rewritable photo-patterning, and multi-mode anti-counterfeiting with ease. Therefore, this study introduces a smart hybrid glass platform as a new photo-responsive switchable system, offering versatility for a wide array of photonic applications.

6.
Adv Sci (Weinh) ; 11(17): e2310262, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38425136

RESUMEN

Ensuring information security has emerged as a paramount concern in contemporary human society. Substantial advancements in this regard can be achieved by leveraging photonic signals as the primary information carriers, utilizing photonic logical gates capable of wavelength tunability across various time and spatial domains. However, the challenge remains in the rational design of materials possessing space-time-color multiple-resolution capabilities. In this work, a facile approach is proposed for crafting metal-organic halides (MOHs) that offer space-time-color resolution. These MOHs integrate time-resolved room temperature phosphorescence and color-resolved excitation wavelength dependencies with both space-resolved ex situ optical waveguides and in situ heterojunctions. Capitalizing on these multifaceted properties, MOHs-based two-dimensional (2D) optical waveguides and heterojunctions exhibit the ability to tune full-color emissions across the spectra from blue to red, operating within different spatial and temporal scales. Therefore, this work introduces an effective methodology for engineering space-time-color resolved MOH microstructures, holding significant promise for the development of high-density photonic logical devices.

7.
Chem Sci ; 15(10): 3625-3632, 2024 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-38455006

RESUMEN

Color-tunable room temperature phosphorescent (RTP) materials have raised wide interest due to their potential application in the fields of encryption and anti-counterfeiting. Herein, a series of CdX2-organic hybrid perovskitoids, (H-apim)CdX3 and (apim)CdX2 (denoted as CdX-apim1 and CdX-apim2, apim = 1-(3-aminopropyl)imidazole, X = Cl, Br), were synthesized using apim with both rigid and flexible groups as ligands, which exhibit naked-eye detectable RTP with different durations and colors (from cyan to red) by virtue of different halogen atoms, coordination modes and the coplanar configuration of flexible groups. Interestingly, CdCl-apim1 and CdX-apim2 both exhibit excitation wavelength-dependent RTP properties, which can be attributed to the multiple excitation of imidazole/apim, the diverse interactions with halogen atoms, and aggregated state of imidazoles. Structural analysis and theoretical calculations confirm that the aminopropyl groups in CdCl-apim1 do not participate in luminescence, while those in CdCl-apim2 are involved in luminescence including both metal/halogen to ligand charge transfer and twisted intramolecular charge transfer. Furthermore, we demonstrate that these perovskitoids can be applied in multi-step anti-counterfeiting, information encryption and smart ink fields. This work not only develops a new type of perovskitoid with full-color persistent luminescence, but also provides new insight into the effect of flexible ligands and halogen engineering on the wide-range modulation of RTP properties.

8.
Mater Horiz ; 2024 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-39045671

RESUMEN

Ultralong room-temperature phosphorescence (RTP) and thermally activated delayed fluorescence (TADF) materials provide exciting opportunities for the rational design of persistent luminescence owing to their long-lived excitons. However, conventional rare-earth-based all-inorganic emitters involve high cost and harsh synthesis conditions, and purely organic systems may require complicated synthesis routes and tedious purification. Therefore, it is highly desirable to develop a cost-effective and easily manufacturable method for achieving color-tunable RTP-TADF with a long afterglow. Herein, we demonstrate a rational strategy to introduce different anions (Cl-, Br- and OAc- ions) into a Zn-based metal-organic scaffold, which can improve the crystal rigidity and achieve a well-balanced RTP-TADF. Both theoretical and experimental studies have demonstrated that the adjustment of different anions can effectively modulate the spin-orbit coupling (SOC) and the energy gap of singlet-triplet states (ΔEST) and then tailor the afterglow lifetime. Moreover, we prepared dye-doped metal-organic hybrid glasses with remarkable potential for the color-tunable afterglow. Therefore, this work not only provides a new horizon for modulating crystal and glass states with color/lifetime-tunable persistent luminescence, but also contributes to optical information storage and anti-counterfeiting technology.

9.
Chem Sci ; 15(12): 4222-4237, 2024 Mar 20.
Artículo en Inglés | MEDLINE | ID: mdl-38516079

RESUMEN

Organic room-temperature phosphorescence (RTP) materials have attracted considerable attention for their extended afterglow at ambient conditions, eco-friendliness, and wide-ranging applications in bio-imaging, data storage, security inks, and emergency illumination. Significant advancements have been achieved in recent years in developing highly efficient RTP materials by manipulating the intermolecular interactions. In this perspective, we have summarized recent advances in ion-regulated organic RTP materials based on the roles and interactions of ions, including the ion-π interactions, electrostatic interactions, and coordinate interactions. Subsequently, the current challenges and prospects of utilizing ionic interactions for inducing and modulating the phosphorescent properties are presented. It is anticipated that this perspective will provide basic guidelines for fabricating novel ionic RTP materials and further extend their application potential.

10.
Chem Sci ; 15(3): 953-963, 2024 Jan 17.
Artículo en Inglés | MEDLINE | ID: mdl-38239673

RESUMEN

Zero-dimensional (0D) hybrid metal halides have emerged as highly efficient luminescent materials, but integrated multifunction in a structural platform remains a significant challenge. Herein, a new hybrid 0D indium halide of (Im-BDMPA)InCl6·H2O was designed as a highly efficient luminescent emitter and X-ray scintillator toward multiple optoelectronic applications. Specifically, it displays strong broadband yellow light emission with near-unity photoluminescence quantum yield (PLQY) through Sb3+ doping, acting as a down-conversion phosphor to fabricate high-performance white light emitting diodes (WLEDs). Benefiting from the high PLQY and negligible self-absorption characteristics, this halide exhibits extraordinary X-ray scintillation performance with a high light yield of 55 320 photons per MeV, which represents a new scintillator in 0D hybrid indium halides. Further combined merits of a low detection limit (0.0853 µGyair s-1), ultra-high spatial resolution of 17.25 lp per mm and negligible afterglow time (0.48 ms) demonstrate its excellent application prospects in X-ray imaging. In addition, this 0D halide also exhibits reversible luminescence off-on switching toward tribromomethane (TBM) but fails in any other organic solvents with an ultra-low detection limit of 0.1 ppm, acting as a perfect real-time fluorescent probe to detect TBM with ultrahigh sensitivity, selectivity and repeatability. Therefore, this work highlights the multiple optoelectronic applications of 0D hybrid lead-free halides in white LEDs, X-ray scintillation, fluorescence sensors, etc.

11.
Sci Bull (Beijing) ; 69(12): 1806-1808, 2024 Jun 30.
Artículo en Inglés | MEDLINE | ID: mdl-38644129
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