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1.
Spectrochim Acta A Mol Biomol Spectrosc ; 324: 124955, 2025 Jan 05.
Article in English | MEDLINE | ID: mdl-39173323

ABSTRACT

Designing persistent dual-band afterglow materials with thermally activated delayed fluorescence (TADF) and room temperature phosphorescence (RTP) contributed to solving the problems of homogenization and singularity in long afterglow materials. Here, six aryl acetonitrile (CBM) and aryl dicyanoaniline (AMBT) derivatives, used as host and guest materials respectively, were successfully designed and synthesized based on the isomerization effect. Among of them, 0.1 % m-CBM/p-AMBT showed the longest dual-band TADF (540 ms) and RTP lifetimes (721 ms), as well as persistent afterglow over 8 s, whose fluorescence (ΦFL), TADF (ΦT) and RTP (ΦP) quantum yields were 0.11, 0.06 and 0.22 in sequence. More interestingly, some doping systems constructed by CBM and AMBT series compounds showed persistent triple-band emissions composed of TADF, unimolecular and aggregated AMBT series compounds. What's more, ΦFL, ΦT and ΦP of 1 % o-AMBT@PMMA film were up to 0.17, 0.17, 0.23 in turn, with TADF, RTP and afterglow lifetimes of 606 ms, 727 ms, and 10 s respectively. TADF and RTP emission of CBM/AMBT series doping systems was attributed to host sensitized guest emission. Besides, the comparison displayed AMBT series compounds had bigger intensity ratios between TADF and RTP emission in PMMA films compared to in CBM series compounds. Finally, a series of data encryption were successfully constructed based on different afterglow lifetimes of the doping systems, and a dynamic anti-counterfeiting pattern was prepared by using different temperature responses of TADF and RTP emissions.

2.
J Colloid Interface Sci ; 677(Pt B): 417-428, 2025 Jan.
Article in English | MEDLINE | ID: mdl-39153245

ABSTRACT

Synthesis of catalysts with high catalytic degradation activity for formaldehyde (HCHO) at room temperature is highly desirable for indoor air quality control. Herein, a novel K-Mn3O4@CeO2 catalyst with excellent catalytic oxidation activity toward HCHO at near room temperature was reported. In particular, the K addition in K-Mn3O4@CeO2 considerably enhanced the oxidation activity, and importantly, 99.3 % conversion of 10 mL of a 40 mg/L HCHO solution at 30 °C for 14 h was achieved, with simultaneous strong cycling stability. Moreover, the addition of K species considerably influenced the chemical valence state of Mn from +4 (ε-MnO2) to +8/3 (Mn3O4) on the surface of CeO2, which obviously changed the tunnel structure and the number of oxygen vacancies. One part of K species is uniformly dispersed on K-Mn3O4@CeO2, and the other part exists in the tunnel structure of Mn3O4@CeO2, which is mainly used to balance the negative charge of the tunnel and prevent collapse of the structure, providing enough active sites for the catalytic oxidation of HCHO. We observed a phase transition from tunneled KMnO2 to Mn3O4 to tunneled MnO2 with the decreasing K+ content, in which K-Mn3O4@CeO2 exhibited higher HCHO oxidation activity. In addition, K-Mn3O4@CeO2 exhibited lower oxygen vacancy formation and HCHO adsorption energies in aqueous solution based on density functional theory calculations. This is because the K species provide more active oxygen species and richer oxygen vacancies on the surface of K-Mn3O4@CeO2, promote the mobility of lattice oxygen and the room-temperature reduction properties of oxygen species, and enhance the ability of the catalyst to replenish the consumed oxygen species. Finally, a possible HCHO catalytic oxidation pathway on the surface of K-Mn3O4@CeO2 catalyst is proposed.

3.
Nanotechnology ; 2024 Oct 03.
Article in English | MEDLINE | ID: mdl-39362238

ABSTRACT

Two-dimensional material (2D material) MXene has great application potential in gas sensors because of its excellent controllable performance and vast specific surface area. In this study, we used a straightforward in-situ electrostatic self-assembly technique to create Fe(OH)3/Ti3C2Tx nanocomposites, which were then used to fabricate gas sensors for ammonia detection at room temperature (25 ℃). Several characterization methods were performed aimed at determining the surface appearance and construction of the nanocomposites, and the sensing characteristics and mechanism were also systematically examined. The findings demonstrate the effective incorporation of amorphous Fe(OH)3 nanoparticles on the surface of Ti3C2Tx. Additionally the nanocomposites of Fe(OH)3/Ti3C2Tx have considerably higher specific surface area than pure Ti3C2Tx, hence offering more active NH3 adsorption sites. The response of the sensor to 100 ppm NH3 was 48.6% at room temperature, which was 9.3 times more higher than that of pure Ti3C2Tx. The sensors also have the advantages of long-term stability (33 days), low NH3 detection limit (500 ppb), and rapid recovery time (85 s) and response times (78 s). It is anticipated that this work will be helpful for developing the new generation of wearable ammonia sensors at room temperature.

4.
Angew Chem Int Ed Engl ; : e202417593, 2024 Oct 09.
Article in English | MEDLINE | ID: mdl-39384546

ABSTRACT

Afterglow materials have garnered significant interest due to distinct photophysical characteristics. However, it is still difficult to achieve long afterglow phosphorescence from organic molecules due to aggregation-caused quenching (ACQ) and energy dissipation. In addition, most materials reported so far have long afterglow emission only at room or even low temperatures, and mainly use UV light as an excitation source. In this work, we report a strategy to achieve high temperature long afterglow emission through the assembly of isolated 0D metal-organic cages (MOCs). In which, both ACQ and phosphorescence quenching effects are effectively mitigated by altering the stacking mode of organic chromophores through orthogonally anchoring into the edges of cubic MOCs. Furthermore, improvement in molecular rigidity, promotion of spin-orbit coupling and broadening of the absorption range are achieved through the MOC- engineering strategy. As a result, we successfully synthesized MOCs that can produce afterglow emission even after excitation by WLEDs at high temperatures (380 K). Moreover, the MOCs are capable of generating afterglow emissions when excited by mobile phone flashlight at room temperature. Given these features, the potential applications of MOCs in the visual identification of explosives, information encryption and multicolor display are explored.

5.
Talanta ; 282: 126971, 2024 Sep 28.
Article in English | MEDLINE | ID: mdl-39366245

ABSTRACT

This work introduces an extremely easy method for preparing luminescent carbon dots (CDs) at ambient temperature using 1,2-naphthoquinone sulphonate and ethylenediamine as precursors via self-exothermic reaction without energy input. The as-obtained CDs have a high quantum yield (34.1 %), a production yield of 21.2 %, and a small size diameter (3.44 nm). Various techniques (NMR, TEM, EDX-mapping, XPS, XRD, FT-IR, fluorescence, and UV-visible spectroscopy) were used to characterize the prepared CDs. The CDs exhibited an excitation-independent emission with λex of 275 nm, demonstrating their homogeneity and high purity. The anticancer drug vincristine (VCR) quantitively quenched the fluorescent signal of the synthesized CDs, allowing their application as the first fluorescent nano-sensor to determine VCR. The quenching effect was linear within the range of 0.2-5.0 µg mL-1, enabling the determination of VCR in vials, plasma, and for content uniformity testing with a detection limit of 0.06 µg mL-1. Moreover, the synthesized CDs were employed as a bio-sensing platform to detect VCR in cancer cells owing to their good selectivity, excellent biocompatibility, minimal cytotoxicity, and high stability. The fabrication of CDs with excellent properties at room temperature under mild conditions paves the way for new advancements in the room temperature synthesis of CDs and offers a highly efficient alternative to traditional synthesis approaches.

6.
Mikrochim Acta ; 191(11): 655, 2024 Oct 08.
Article in English | MEDLINE | ID: mdl-39379669

ABSTRACT

Room temperature phosphorescent carbon dots (NCCDs@SiO2) were obtained by encapsulating hydrothermally synthesized CDs in a dense Si-O network structure after high-temperature calcination using silica as the matrix. This can avoid the quenching effect of dissolved oxygen in water and has a phosphorescence lifetime of up to 2.41 s. Using the phosphorescence property of NCCDs@SiO2, a phosphorescence quenching sensor was developed for the sensitive and selective detection of thiram with the assistance of Cu2+. Cu2+-thiram complexes led to a rapid phosphorescence quenching of NCCDs@SiO2 within 30 s through the inner filter effect. The linear range of phosphorescence for thiram was 0.5-100 µM with a detection limit of 0.121 µM. The proposed method was able to detect thiram in real samples and was validated by high-performance liquid chromatography (HPLC) confirming the potential of this phosphorescence sensing method for thiram detection. This work opens up a new avenue for the detection of thiram residues in fruits and vegetables and also provides a new idea for the design of a rapid detection platform using other room temperature phosphorescent materials.

7.
Adv Sci (Weinh) ; : e2410671, 2024 Oct 08.
Article in English | MEDLINE | ID: mdl-39377218

ABSTRACT

Chiral recognition is crucial for applications in chiral purity assessment and biomedical fields. However, achieving chiral recognition through visible room temperature phosphorescence remains challenging. Here, two chiral molecules, designated as host and guest are synthesized, which possess similar structural configurations. A viable strategy involving a chiral configuration-dependent energy transfer process to enable selective phosphorescence expression is proposed, thereby enabling chiral recognition in a host-guest doping system. The chiral and structural similarity between host and guest facilitates efficient Dexter energy transfer due to the reduced spatial distance between the molecules. This mechanism significantly enhances the intensity of red phosphorescence from the guest molecule, characterized by an emission peak at 612 nm and a prolonged lifetime of 32.7 ms. This work elucidates the mechanism of chiral-dependent energy transfer, demonstrating its potential for selectively expressing phosphorescence in chiral recognition.

8.
Adv Mater ; : e2407916, 2024 Oct 07.
Article in English | MEDLINE | ID: mdl-39374028

ABSTRACT

Scintillators have attracted significant attention due to their wide-ranging applications in both industrial and medical fields. However, one of the ongoing challenges is the efficient utilization of triplet excitons to achieve high radioluminescence efficiency. Here, a series of purely organic phosphors is presented for X-ray scintillation, employing a combined rigid and flexible host-guest doping strategy. The doped crystals exhibit a remarkable maximum phosphorescence efficiency of 99.4% under UV excitation. Furthermore, upon X-ray irradiation, the radioluminescence intensities of the doped phosphors are markedly higher compared to their single-component crystal counterparts. Through systematic investigations, it is demonstrated the crucial role of confining isolated chromophores in enhancing scintillation efficiency. Additionally, a transparent scintillator screen fabricated with the doped phosphor exhibits excellent X-ray imaging performance, achieving a high spatial resolution of 18.0 lp mm-1. This work not only offers valuable insights into suppressing non-radiative transitions of triplet excitons during scintillation but also opens a new avenue for designing highly efficient purely organic phosphorescent scintillators.

9.
Spectrochim Acta A Mol Biomol Spectrosc ; 326: 125247, 2024 Oct 05.
Article in English | MEDLINE | ID: mdl-39388937

ABSTRACT

Purely organic room temperature phosphorescence materials (RTP) have attracted much attention recently, but most of them are substituted with heavy atoms to enhance the intersystem crossing (ISC), which requires complicated design and synthesis. Herein, we report four chiral heavy-atom-free small molecules which integrate properties of aggregation and long-lifetime room temperature phosphorescence. The phosphorescence lifetime of synthesized chiral molecules is measured to be 150 ms, and the phosphorescence quantum yield reaches 15 % at room temperature. The twisted chiral conformation of four molecules not only affect aggregation photoluminescence properties but also can synergistically stabilize triplet exciton in the triplet excited states for excellent ISC efficiency. This strategy enriches the application fields of chiral aggregated long-lifetime room temperature phosphorescent materials.

10.
Chemistry ; : e202403326, 2024 Sep 29.
Article in English | MEDLINE | ID: mdl-39343748

ABSTRACT

As family members of polycyclic aromatic hydrocarbons, compound anthracene (Ant) and phenanthrene (Phe) as isomers are widely used in organic optical materials and electronic materials. But their photochemical and physical properties are very different. In this work, the room temperature phosphorescence (RTP) properties of PVA-B-Ant and PVA-B-Phe are discussed carefully which are prepared by B-O click reaction through polyvinyl alcohol (PVA) with 9-anthraceneboronic acid (B-Ant) and 9-phenanthrenylboronic acid (B-Phe), respectively. PVA-B-Phe 1% film exhibits excellent fluorescence (FL) emission at 374 nm and RTP emission at 523 nm with green afterglow and around 1.9 s phosphorescence lifetime. However, PVA-B-Ant 1% film only shows strong blue FL emission at 414 nm, and the emission intensity decreases seriously with the extension of irradiation time. Experimental and theoretical calculations results suggest that the photodimer of Ant which is formed in PVA matrix under the UV light irradiation would be competitive with the process of RTP emission. This work demonstrates that the RTP properties of organic molecules might be probably affected by the photostability of the organic phosphor under UV irradiation.

11.
ACS Sens ; 2024 Sep 29.
Article in English | MEDLINE | ID: mdl-39344131

ABSTRACT

Detecting H2S in oxygen-deficient conditions is vital for identifying leaks in SF6-insulated electrical equipment. Current infrared-based detection methods are expensive and sensitive to environmental conditions, highlighting the necessity for cost-effective and stable gas sensors. Existing gas sensors based on semiconducting metal oxides (SMOXs) are limited by redox reactions with oxygen and require high operating temperatures. Here, we introduce a room-temperature (RT) H2S sensor for oxygen-deficient environments using the intrinsic conducting two-dimensional (2D) metal-organic framework (MOF), Co1.8Ni1.2(hexaiminotriphenylene)2 [Co1.8Ni1.2(HITP)2], overcoming the limitations of SMOX gas sensors. Remarkably, Co1.8Ni1.2(HITP)2 sensors exhibit exceptional selectivity for H2S with negligible cross-responses and a sensitivity drift of less than 4.13% in an SF6 atmosphere over 60 days. The Co1.8Ni1.2(HITP)2 gas sensor shows significant promise for real-time and stable monitoring of H2S gas in oxygen-deficient environments.

12.
ChemSusChem ; : e202400763, 2024 Sep 30.
Article in English | MEDLINE | ID: mdl-39344878

ABSTRACT

Surfactant-free colloidal syntheses in aqueous media are attractive to develop nanomaterials relevant for various applications, e.g. catalysis or medicine. However, controlled green syntheses without surfactants of metal nanoparticles in aqueous media remain scarce. Here, room temperature syntheses of gold (Au) nanoparticles (NPs) that require only HAuCl4, alkaline water and an alcohol, i.e. relatively benign chemicals and mild reaction conditions, are developed. The findings of a comprehensive multi-parameters screening performed in small volumes (< 3 mL) over 1000+ experiments pave the way to greener high throughput screenings of large parametric spaces and lead to scalable (100 mL) synthetic strategies. A rational selection of the alcohol is proposed. The influence of lights with defined wavelengths (222-690 nm) is investigated. It is found that lights with lower wavelengths favor the formation of smaller 5 nm NPs. Different kinetics and formation pathways are observed for different alcohols and for lights with different wavelengths. The sensitivity to various experimental parameters increases in the order glycerol < ethylene glycol < ethanol < methanol. New strategies for a rational fine size control, and to some extend shape control, are identified. The results lead to more sustainable and reproducible surfactant-free colloidal syntheses of NPs.

13.
Angew Chem Int Ed Engl ; : e202416189, 2024 Sep 26.
Article in English | MEDLINE | ID: mdl-39325535

ABSTRACT

Controlling multicolor persistent room-temperature phosphorescence (RTP) through photoirradiation holds fundamental significance but remains a significant challenge. In this study, we engineered a wavelength-selective photoresponsive system utilizing the Förster resonance energy transfer strategy. This system integrates a photoactivated long-lived luminescent material as the energy donor with a fluorescent photoswitch as the energy acceptor, facilitating programmable persistent luminescence switches. Distinct afterglow color states, such as initial nonemissive, green, yellow, and orange, were achieved through irradiation at 400 nm, 365 nm, and 254 nm, respectively. Based on this capability, we established an interacting network for multistate afterglow color switching among these four emissive states. In addition, we demonstrate the potential of this wavelength-selective photoresponsive system in the photo-controlled rewritable printing of multicolor afterglow images on a single thin film. This work represents a substantial step towards the fabrication of sophisticated wavelength-selective photoresponsive systems, potentially revolutionizing applications in optical data storage, security labeling, and smart displays by enabling precise control over photoresponsive behaviors under various photoirradiation wavelengths.

14.
Nanomaterials (Basel) ; 14(18)2024 Sep 22.
Article in English | MEDLINE | ID: mdl-39330690

ABSTRACT

Silver nanodendrites (AgNDs) were effectively synthesized utilizing a phytantriol template at ambient temperature without electrodeposition. In comparison to AgNDs, the phytantriol-templated silver nanodendrites (P/AgNDs) exhibited a smoother structure with the well-ordered growth of smaller particles around 51 nm. Moreover, the P/AgNDs exhibited uniform elemental distribution, forming chemical bonds with functional groups, crystallite size around 42 nm, and high transmittance around 95%. These experimental findings indicate that room temperature-based hierarchical P/AgNDs have considerable potential for diverse applications, specifically in sensing.

15.
Adv Sci (Weinh) ; : e2408096, 2024 Sep 28.
Article in English | MEDLINE | ID: mdl-39340830

ABSTRACT

La-decorated Bi2O2CO3 (BCO-La) microspheres are synthesized using a facile wet chemical strategy for sensing low-concentration nonanal (C9H18O) at room temperature. These BCO-La gas sensors are applied to evaluate agricultural product quality, specifically for cooked rice. The sensitivity of the BCO-6La sensor significantly surpassed that of the pure BCO sensor, achieving a response value of 174.6 when detecting 30 ppm nonanal gas. Notably, the BCO-6La sensor demonstrated a faster response time (36 s) when exposed to 18 ppm of nonanal. Additionally, the selectivity toward nonanal gas detection is higher (approximately 4-24 times) compared to interfering gases (1-octanol, geranyl acetone, linalool, hexanal, 2-pentyfuran, and 1-octen-3-ol) during cooked rice quality detection. The gas sensing mechanism and the factors contributing to the enhanced sensing performance of the BCO-La microspheres are demonstrated through in situ FT-IR spectra and DFT analysis while the realistic detection scenario is carried out. In a broader context, the reported sensors here represent a novel platform for the detection and monitoring of gases released by agricultural products during storage.

16.
Front Chem ; 12: 1441452, 2024.
Article in English | MEDLINE | ID: mdl-39345861

ABSTRACT

The long-lived room-temperature phosphorescence (RTP) originating from thiophene boronate polyvinyl alcohol (PVA) has enabled the creation of metal-ion-responsive RTP films doped with spirolactam ring-containing rhodamine 6G (1). In this study, RTP-active PVA films, namely, TDB@PVA and ATB@PVA, were prepared through boronate esterification of thiophene-2,5-diboronic acid (TDB) and 5-acetylthiophene-2-boronic acid (ATB) with the diol units of PVA. The delayed emission properties were evaluated, revealing an emission band at 477 nm with a turquoise afterglow for TDB@PVA and at 510 nm with a green afterglow for ATB@PVA after UV light irradiation ceased. The photophysical properties were assessed using TD-DFT and DFT calculations at the B3LYP/cc-pVDZ level. N-(rhodamine-6G)lactam dye with a salicylimine unit (1) was doped into the RTP-based PVA films, producing a multicolored afterglow upon the addition of metal ions. This phenomenon is explained by a triplet-to-singlet Förster-type resonance energy transfer process from the cross-linked thiophene boronate in PVA to the metal-ion-activated colored form of 1. This photophysical feature finds applicability in encryption techniques. Notably, the reversible metal-ligand coordination of 1 in the PVA system enabled a write/erase information process.

17.
Nano Lett ; 2024 Sep 25.
Article in English | MEDLINE | ID: mdl-39320324

ABSTRACT

We engineered a two-dimensional Pt/WSe2/Ni avalanche photodetector (APD) optimized for ultraweak signal detection at room temperature. By fine-tuning the work functions, we achieved an ultralow dark current of 10-14 A under small bias, with a noise equivalent power (NEP) of 8.09 fW/Hz1/2. This performance is driven by effective dark barrier blocking and a record-long electron mean free path (123 nm) in intrinsic WSe2, minimizing dark carrier replenishment and suppressing noise under an ultralow electric field. Our APD exhibits a high gain of 5 × 105 at a modulation frequency of 20 kHz, effectively balancing gain and bandwidth, a common challenge in traditional photovoltaic-based APDs. By addressing the typical challenges of high noise and low gain and minimizing dependence on high electric fields, this work highlights the potential of 2D materials in developing efficient, low-power, and ultrasensitive photodetections.

18.
Data Brief ; 57: 110879, 2024 Dec.
Article in English | MEDLINE | ID: mdl-39290431

ABSTRACT

The data presented here is the characteristics of biopellets and its raw materials. The raw materials of lignocellulosic waste (coffee skin, corncob, patchouli waste) and shrubs (Leucaena leucocephala and Gliricidia sepium) were collected from certain districts in Indonesia which provided quite abundant stocks of these raw materials. The raw material preparation and pelletization at room temperature (25 °C) using a manual press machine were carried out at Hasanuddin University, Makassar, Indonesia. Meanwhile, pelletization at high temperatures (225 °C) was carried out at The Integrated Laboratory of Forest Research and Development, Bogor, Indonesia. The evaluation of density, moisture content, volatile matter content, ash content, and amount of fixed carbon were also carried out at the laboratory. Meanwhile, evaluation of mineral content (sulfur, Na2O, K2O, Cl) and calorivic value was carried out at the Livestock Research Institute, Bogor, Indonesia. The results show that pelletization at high temperature produces better quality biopellets compared to pelletization at room temperature. Pelletization of L. leucocephala at high temperature produces the best quality biopellets with the highest density (1.17 g/cm3) and calorific value (4726 kcal/kg) and the lowest moisture content (4.87 %) and mineral content (0.01 % of S, 0.0014 % of Na2O, 1.53 % of K2O, and 0.17 % of Cl) among the other raw materials tested. This dataset is expected to be a primary source in comparing and determining the proper type of raw material for biopellet production as an alternative renewable energy source, especially those originating from shrubs and similar lignocellulosic waste.

19.
J Colloid Interface Sci ; 678(Pt B): 1125-1134, 2024 Sep 12.
Article in English | MEDLINE | ID: mdl-39278038

ABSTRACT

Room temperature sodium-sulfur (RT Na-S) batteries are considered as advanced energy storage technology due to their low cost and high theoretical energy density. However, challenges such as the growth of sodium dendrite and dissolution of sodium polysulfides significantly hinder the electrochemical performance. Herein, we developed a propylene carbonate (PC)-based electrolyte with Methyl 2-Fluoroisobutyrate (MFB) as an additive. The ester group in the MFB additive is capable of participating in and reconfiguring the coordination of their Na+ solvated structures, thereby lowering the desolvation barrier and regulating the Na anode's interfacial reaction and nucleation behavior. The polar C-F bond at the other end helps to reduce the lowest unoccupied molecular orbital (LUMO) energy of the MFB additive, enabling the preferential decomposition of MFB to form the F-rich inorganic phase strong polar solid electrolyte interphase (SEI), contributing to the inhibition of Na dendrite growth, the accumulation of dead Na. In addition, NaF-riched cathode electrolyte interphase (CEI) was also observed on sulfur-based cathode, which can effectively inhibited the shuttle effect. Consequently, the developed RT Na-S battery exhibit excellent electrochemical performance.

20.
J Biotechnol ; 395: 71-79, 2024 Sep 17.
Article in English | MEDLINE | ID: mdl-39299520

ABSTRACT

Macrolactins have attracted considerable attention due to their value and application in medicine and agriculture. However, poor yields severely hinder their broader application in these fields. This study aimed to improve macrolactins production in Bacillus siamensis using a combined atmospheric and room-temperature plasma mutagenesis and a microbial microdroplet culture system. After 25 days of treatment, a desirable strain with macrolactins production 3.0-fold higher than that of the parental strain was successfully selected. The addition of 30 mg/L ZnSO4 further increased macrolactins production to 503 ± 37.6 µg/mL, representing a 30.9 % improvement in production compared to controls. Based on transcriptome analysis, the synthesis pathways of amino acids, fengycin, and surfactin were found to be downregulated in IMD4036. Further fermentation experiments confirmed that inhibition of the comparative fengycin synthesis pathway was potentially driving the increased production of macrolactins. The strategies and possible mechanisms detailed in this study can provide insight into enhancing the production of other secondary metabolites toxic to the producer strains.

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