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1.
Small ; : e2310478, 2024 Feb 09.
Article in English | MEDLINE | ID: mdl-38334247

ABSTRACT

Addressing the challenge of lighting stability in perovskite white light emitting diodes (WLEDs) is crucial for their commercial viability. CsPbX3 (X = Cl, Br, I, or mixed) nanocrystals (NCs) are promising for next-generation lighting due to their superior optical and electronic properties. However, the inherent soft material structure of CsPbX3 NCs is particularly susceptible to the elevated temperatures associated with prolonged WLED operation. Additionally, these NCs face stability challenges in high humidity environments, leading to reduced lighting performance. This study introduces a two-step dual encapsulation method, resulting in CsPbBr3 @SiO2 /Al2 SiO5 composite fibers (CFs) with enhanced optical stability under extreme conditions. In testing, WLEDs incorporating these CFs, even under prolonged operation at high power (100 mA for 9 h), maintain consistent electroluminescence (EL) intensity and optoelectronic parameters, with surface temperatures reaching 84.2 °C. Crucially, when subjected to 85 °C and 85% relative humidity for 200 h, the WLEDs preserve 97% of their initial fluorescence efficiency. These findings underscore the efficacy of the dual encapsulation strategy in significantly improving perovskite material stability, marking a significant step toward their commercial application in optoelectronic lighting.

2.
Nanotechnology ; 34(27)2023 Apr 19.
Article in English | MEDLINE | ID: mdl-37011606

ABSTRACT

Perovskite nanocrystals (NCs) feature adjustable bandgap, wide absorption range, and great color purity for robust perovskite optoelectronic applications. Nevertheless, the absence of lasting stability under continues energization, is still a major hurdle to the widespread use of NCs in commercial applications. In particular, the reactivity of red-emitting perovskites to environmental surroundings is more sensitive than that of their green counterparts. Here, we present a simple synthesis of ultrathin ZrO2coated, Sr2+doped CsPbBrI2NCs. Introducing divalent Sr2+may significantly eliminate Pb° surface traps, whereas ZrO2encapsulation greatly improves environmental stability. The photoluminescence quantum yield of the Sr2+-doped CsPbBrI2/ZrO2NCs was increased from 50.2% to 87.2% as a direct consequence of the efficient elimination of Pb° surface defects. Moreover, the thickness of the ZrO2thin coating gives remarkable heat resistance and improved water stability. Combining CsPbSr0.3BrI2/ZrO2NCs in a white light emitting diode (LED) with an excellent optical efficiency (100.08 lm W-1), high and a broad gamut 141% (NTSC) standard. This work offers a potential method to suppress Pb° traps by doping with Sr2+and improves the performance of perovskite NCs by ultrathin coating structured ZrO2, consequently enabling their applicability in commercial optical displays.

3.
Nanotechnology ; 33(17)2022 Feb 03.
Article in English | MEDLINE | ID: mdl-35026753

ABSTRACT

In recent years, significant progress has been made in the red and green perovskite quantum dots (PQDs) based light-emitting devices. However, a scarcity of blue-emitting devices that are extremely efficient precludes their research and development for optoelectronic applications. Taking advantage of tunable bandgaps of PQDs over the entire visible spectrum, herein we tune optical properties of CSPbBr3by mixing Nd3+trivalent lanthanide halide cations for blue light-emitting devices. The CsPbBr3PQDs doped with Nd3+trivalent lanthanide halide cations emitted strong photoemission from green into the blue region. By adjusting their doping concentration, a tunable wavelength from (515 nm) to (450 nm) was achieved with FWHM from (37.83 nm) to (16.6 nm). We simultaneously observed PL linewidth broadening thermal quenching of PL and the blue shift of the optical bandgap from temperature-dependent PL studies. The Nd3+cations into CsPbBr3PQDs more efficiently reduced non-radiative recombination. As a result of the efficient removal of defects from PQDs, the photoluminescence quantum yield (PLQY) has been significantly increased to 91% in the blue-emitting region. Significantly, Nd3+PQDs exhibit excellent long-term stability against the external environment, including water, temperature, and ultraviolet light irradiation. Moreover, we successfully transformed Nd3+doped PQDs into highly fluorescent nanocomposites. Incorporating these findings, we fabricate and test a stable blue light-emitting LED with EL emission at (462 nm), (475 nm), and successfully produce white light emission from Nd3+doped nanocomposites with a CIE at (0.32, 0.34), respectively. The findings imply that low-cost Nd3+doped perovskites may be attractive as light converters in LCDs with a broad color gamut.

4.
Anal Bioanal Chem ; 414(14): 4139-4147, 2022 Jun.
Article in English | MEDLINE | ID: mdl-35441261

ABSTRACT

Propyl gallate (PG) as one of the most important additives has been widely used to prevent or slow the oxidation of foods in the food industry. In this work, Cu3(PO4)2/BiVO4 composite is synthesized through two hydrothermal processes. With visible light irradiation, the Cu3(PO4)2/BiVO4 composites modified PEC platform displays a superior anode photocurrent signal. The PEC sensor showed a wide linear range from 1 × 10-10 to 1 × 10-3 mol L-1 with a detection limit as low as 0.05 × 10-10 mol L-1. The Cu3(PO4)2/BiVO4 photoelectrochemical (PEC) sensor is designed and characterized by electrochemical impedance. Compared with GCE/BiVO4 and GCE/Cu3(PO4)2, the GCE/Cu3(PO4)2/BiVO4 has a higher photocurrent response. In addition, the sensor is highly selective for samples containing other antioxidants. Furthermore, the sensor can be used to detect PG in edible oil samples with satisfactory results. The recoveries of propyl gallate in edible oil ranged from 95.5 to 101.8%. The results show that Cu3(PO4)2/BiVO4 composites can be used to analyze PG in different edible oil samples, which are beneficial for food quality monitoring and reduce the risk of PG overuse in food.


Subject(s)
Biosensing Techniques , Propyl Gallate , Antioxidants , Biosensing Techniques/methods , Electrochemical Techniques , Electrodes , Propyl Gallate/chemistry
5.
Anal Bioanal Chem ; 414(12): 3571-3580, 2022 May.
Article in English | MEDLINE | ID: mdl-34982179

ABSTRACT

Photoelectrochemical (PEC) detection as a potential development strategy for Cu2+ ion sensor has arisen extensive attention. Herein, CdS/Ti3C2 heterostructure was synthesized by electrostatically driven assembly and hydrothermal method. On the basis of a CdS/Ti3C2 heterostructure, a novel anodic PEC sensing platform was constructed for highly sensitive detection of trace amount of Cu2+. Carrier transport at the interface of CdS/Ti3C2 heterostructure was tremendously improved, due to the generation of effective Schottky junctions. Under visible light irradiation, the CdS/Ti3C2 heterostructure-modified PEC platform exhibits great anode photocurrent signal, and the formation of CuxS reduces the PEC response with the presence of Cu2+ as a representative analyte. Thus, the linear response of Cu2+ ranges from 0.1 nM to 10 µM and the limits of detection (LOD, 0.05 nM) are obtained, which is lower than that of WHO's Guidelines for Drinking-water Quality (30 µM). This idea of component reconstitution provides a new paradigm for the design of advanced PEC sensors.


Subject(s)
Biosensing Techniques , Electrochemical Techniques , Biosensing Techniques/methods , Electrodes , Light , Limit of Detection , Titanium/chemistry
6.
Nanotechnology ; 32(41)2021 Jul 19.
Article in English | MEDLINE | ID: mdl-34198279

ABSTRACT

Since visible-light (VL) accounting for massive solar radiation energy, a large amount of attention has been paid to the development of highly efficient visible-light-driven (VLD) semiconductor materials. However, despite recent efforts to construct VL active material, hollow structure-based silver iodide (AgI) with appropriate band gap and a large surface area are limited because of lack of a proper synthesis method. Herein, hollow AgI with p-type semiconductor behavior is constructed on the basis of micro-emulsion strategy, which enables admirable cathode photoelectrochemical (PEC) response. The as-prepared hollow AgI is applied to fabricate the PEC sensing platform and reveals a low limit of detection of 0.04 fM and a wide dynamic range up to 5 orders of magnitude toward H2S. The PEC sensing mechanism is supposed to the 'signal-off' pattern on account of the ultralow solubility product (Ksp) of Ag2S, derived from the precipitation reaction due to the high affinity between sulfide ion and Ag+. Besides, the hollow structure of AgI provides sufficient surface area forin situproducing Ag2S that serves as recombination center of carrier, thus causing the efficient quenching of photocurrent signals. This work broadens the horizon of structuring VLD semiconductor nanomaterials andKsp-based H2S sensing.

7.
Mikrochim Acta ; 186(12): 789, 2019 11 15.
Article in English | MEDLINE | ID: mdl-31732798

ABSTRACT

A corn-like CeO2/C coaxial cable textured by a cerium oxide shell and a carbon core was designed to sense NO. The carbon core possesses high electrical conductivity, and the CeO2 surface delivers excellent electrocatalytic activity. The sensor, typically operated at 0.8 V (vs. Ag/AgCl), exhibits a detection limit of 1.7 nM, which is 4-times lower than that of CeO2 nanotubes based one (at S/N = 3). It also displays wide linear response (up to 83 µM), a sensitivity of 0.81 µA µM-1 cm-2, and fast response (2 s). These values are highly competitive to that of a CeO2 tube (0.92 µA µM-1 cm-2 and 2 s). The sensor was used to quantify NO that is released by Aspergillus flavus. Graphical abstractSchematic representation of corn-like CeO2/C which can more sensitively and effectively detect NO released from A. flavus than when using CeO2 nanotubes, benefitting from its unique coaxial cable structure.

8.
Mikrochim Acta ; 185(2): 140, 2018 01 27.
Article in English | MEDLINE | ID: mdl-29594540

ABSTRACT

FePO4 is biocompatible and can act as a kind of promising enzyme mimetic. Unfortunately, the electrical conductivity of FePO4 is poor. In order to enhance its conductivity, FePO4 was embedded into nanofibers consisting of amorphous carbon and reduced graphene oxide (rGO) by an electrospinning technique. As a sensing material for monitoring superoxide anion (O2•-) and typically operated at 0.5 V (vs. SCE), it displays high sensitivity (9.6 µA⋅µM-1⋅cm-2), a low detection limit (9.7 nM at S/N = 3), a wide linear response range (10 nM to 10 µM), and fast response (1.6 s). Due to its low detection limit and fast response, the sensor in our perception has a large potential for detecting superoxide anions released by HeLa cancer cells. Graphical abstract Schematic of the microstructure of FePO4/C and FePO4/rGO-C nanofibers, a photograph of cancer cells (HeLa), and the electrochemical response towards O2-• of the sensor.


Subject(s)
Biomimetic Materials/chemistry , Ferric Compounds/chemistry , Graphite/chemistry , Nanofibers/chemistry , Superoxides/chemistry , Superoxides/metabolism , Cell Survival , Electric Conductivity , Electrochemistry , HeLa Cells , Human Umbilical Vein Endothelial Cells/metabolism , Humans , Limit of Detection , Oxidation-Reduction
9.
Angew Chem Int Ed Engl ; 57(7): 1963-1967, 2018 02 12.
Article in English | MEDLINE | ID: mdl-29247475

ABSTRACT

Transition-metal phosphides (TMPs) have emerged as promising catalyst candidates for the hydrogen evolution reaction (HER). Although numerous methods have been investigated to obtain TMPs, most rely on traditional synthetic methods that produce materials that are inherently deficient with respect to electrical conductivity. An electrospinning-based reduction approach is presented, which generates nickel phosphide nanoparticles in N-doped porous carbon nanofibers (Ni2 P@NPCNFs) in situ. Ni2 P nanoparticles are protected from irreversible fusion and aggregation in subsequent high-temperature pyrolysis. The resistivity of Ni2 P@NPCNFs (5.34â€…Ω cm) is greatly decreased by 104 times compared to Ni2 P (>104 â€…Ω cm) because N-doped carbon NFs are incorporated. As an electrocatalyst for HER, Ni2 P@NPCNFs reveal remarkable performance compared to other previously reported catalysts in acidic media. Additionally, it offers excellent catalytic ability and durability in both neutral and basic media. Encouraged by the excellent electrocatalytic performance of Ni2 P@NPCNFs, a series of pea-like Mx P@NPCNFs, including Fe2 P@NPCNFs, Co2 P@NPCNFs, and Cu3 P@NPCNFs, were synthesized by the same method. Detailed characterization suggests that the newly developed method could render combinations of ultrafine metal phosphides with porous carbon accessible; thereby, extending opportunities in electrocatalytic applications.

10.
Analyst ; 141(4): 1279-85, 2016 Feb 21.
Article in English | MEDLINE | ID: mdl-26765273

ABSTRACT

Metal-organic frameworks (MOFs) have recently attracted much interest in electrochemical fields due to their controlled porosity, large internal surface area, and countless structural topologies. However, the direct application of single component MOFs is limited since they also exhibit poor electronic conductivity, low mechanical stability, and inferior electrocatalytic ability. To overcome these problems, we implanted multi-walled carbon nanotubes (MWCNTs) into manganese-based metal-organic frameworks (Mn-BDC) using a one-step solvothermal method and found that the introduction of MWCNTs can initiate the splitting of bulky Mn-BDC into thin layers. This splitting is highly significant in that it enhances the electronic conductivity and electrocatalytic ability of Mn-BDC. The constructed Mn-BDC@MWCNT composites were utilized as an electrode modifying material in the fabrication of an electrochemical sensor and then were used successfully for the determination of biomolecules in human body fluid. The sensor displayed successful detection performance with wide linear detection ranges (0.1-1150, 0.01-500, and 0.02-1100 µM for AA, DA and UA, respectively) and low limits of detection (0.01, 0.002, and 0.005 µM for AA, DA and UA, respectively); thus, this preliminary study presents an electrochemical biosensor constructed with a novel electrode modifying material that exhibits superior potential for the practical detection of AA, DA and UA in urine samples.


Subject(s)
Ascorbic Acid/urine , Dopamine/urine , Manganese/chemistry , Nanotubes, Carbon/chemistry , Organometallic Compounds/chemistry , Uric Acid/urine , Urinalysis/methods , Electrochemistry , Electrodes , Humans , Hydrogen-Ion Concentration , Limit of Detection , Nanocomposites/chemistry , Temperature , Time Factors
11.
Phys Chem Chem Phys ; 18(27): 18219-26, 2016 Jul 21.
Article in English | MEDLINE | ID: mdl-27332751

ABSTRACT

Although reduced graphene oxide (rGO)-based photocatalyst composites have been intensively developed during the past few years, the influence of reduction extent of rGO on the photocatalytic performance of the rGO-based composite has virtually not been investigated due to some technical limitations, such as the poor water dispersibility of rGO and low reduction selectivity of the hydrothermal method, which make it difficult to control the reduction extent of rGO in these composites. Herein, we used a facile room-temperature method to synthesize Ag/AgX (X = Cl, Br)/rGO photocatalyst composites as a model to study the effect of reduction extent of rGO on the photocatalytic performance of the photocatalyst. It was found that the photocatalytic activities of both Ag/AgCl/PrGO and Ag/AgBr/PrGO systems had an optimized threshold of the reduction extent of photoreduced GO (PrGO). More importantly, due to the different conductive band values of AgCl and AgBr, the optimized thresholds in the two systems were at different PrGO reduction extents, based on which we proposed that the favorable energy band matching between AgX and PrGO in the two systems played a crucial role in obtaining high photocatalysis performance. Besides, the photocatalytic reaction of the Ag/AgBr based system was confirmed to be a pseudo-second-order kinetics reaction rather than pseudo-first-order kinetics reaction. The new insights presented in this work provided useful information on the design and development of a more sophisticated photocatalyst, and can also be applied to many other applications.

12.
Phys Chem Chem Phys ; 16(10): 4561-8, 2014 Mar 14.
Article in English | MEDLINE | ID: mdl-24457425

ABSTRACT

In this work, we report that the Ag-graphene composite (AGC) can effectively enhance the light harvesting and photoluminescence (PL) quenching efficiency of poly[2-methoxy-5-(2-ethylhexyloxy)-1,4-phenylene-vinylene] (MEH-PPV). Loading the AGC on MEH-PPV leads to improved light absorption ability and PL quenching efficiency, which is due to the strong interaction between localized surface plasmon resonance (LSPR)-activated Ag nanoparticles and the MEH-PPV molecule. Control experiment reveals that the combination of graphene and Ag nanoparticles achieves superior light absorptivity and PL quenching ability compared with individual graphene and Ag NPs. The exponential shape of the Stern-Volmer plot implies that both Ag and graphene in the AGC can offer the quenching pathway for the PL quenching process. We also found that the AGC with a broader LSPR absorption range is competitive in enhancing the light absorption ability and PL quenching efficiency of the MEH-PPV-AGC composite, because it can expand LSPR-induced light harvesting and PL quenching response to a wider absorption range.


Subject(s)
Graphite/chemistry , Nanoparticles/chemistry , Polymers/chemistry , Silver/chemistry , Vinyl Compounds/chemistry , Light , Luminescence , Nanoparticles/ultrastructure , Surface Plasmon Resonance
13.
Nanoscale ; 16(23): 11310-11317, 2024 Jun 13.
Article in English | MEDLINE | ID: mdl-38804052

ABSTRACT

Room temperature phosphorescent (RTP) carbon dot (CD) materials have been widely used in various fields, but it is difficult to achieve a long lifetime, high stability and easy synthesis. In particular, realizing the phosphorescence emission of CDs using a metal oxide (MO) matrix is a challenge. Here, solid gels are synthesized via in situ hydrolysis, and then RTP CDs are synthesized based on a SiO2 matrix (CDs@SiO2) and hybridized with a MO matrix (CDs@SiO2-MO) by high-temperature calcination. Among the materials synthesized, Al2O3 matrix RTP CDs (CDs@SiO2-Al2O3) have a long phosphorescence lifetime of 689 ms and can exhibit yellow-green light visible to the naked eye for 9 s after the UV light (365 nm) is turned off. Compared with the green phosphorescence of CDs@SiO2, the yellow-green phosphorescence lifetime of CDs@SiO2-Al2O3 is enhanced by 420 ms. In addition, CDs@SiO2-Al2O3 maintains good stability of phosphorescence emission in water, strongly oxidizing solutions and organic solvents. As a result, CDs@SiO2-Al2O3 can be applied to the field of information encryption and security anti-counterfeiting, and this work provides a new, easy and efficient synthesis method for MO as an RTP CD matrix.

14.
Nat Nanotechnol ; 19(3): 330-337, 2024 Mar.
Article in English | MEDLINE | ID: mdl-37770648

ABSTRACT

Personalized monitoring of female hormones (for example, oestradiol) is of great interest in fertility and women's health. However, existing approaches usually require invasive blood draws and/or bulky analytical laboratory equipment, making them hard to implement at home. Here we report a skin-interfaced wearable aptamer nanobiosensor based on target-induced strand displacement for automatic and non-invasive monitoring of oestradiol via in situ sweat analysis. The reagentless, amplification-free and 'signal-on' detection approach coupled with a gold nanoparticle-MXene-based detection electrode offers extraordinary sensitivity with an ultra-low limit of detection of 0.14 pM. This fully integrated system is capable of autonomous sweat induction at rest via iontophoresis, precise microfluidic sweat sampling controlled via capillary bursting valves, real-time oestradiol analysis and calibration with simultaneously collected multivariate information (that is, temperature, pH and ionic strength), as well as signal processing and wireless communication with a user interface (for example, smartphone). We validated the technology in human participants. Our data indicate a cyclical fluctuation in sweat oestradiol during menstrual cycles, and a high correlation between sweat and blood oestradiol was identified. Our study opens up the potential for wearable sensors for non-invasive, personalized reproductive hormone monitoring.


Subject(s)
Biosensing Techniques , Metal Nanoparticles , Wearable Electronic Devices , Humans , Female , Gold , Skin , Estradiol
15.
Article in English | MEDLINE | ID: mdl-38598608

ABSTRACT

The core-shell structure is an effective means to improve the stability and optoelectronic properties of cesium lead halide (CsPbX3 (X = Cl, Br, I)) perovskite quantum dots (QDs). However, confined by the ionic radius differences, developing a core-shell packaging strategy suitable for the entire CsPbX3 system remains a challenge. In this study, we introduce an optimized hot-injection method for the epitaxial growth of the CsPb2X5 substrate on CsPbX3 surfaces, achieved by precisely controlling the reaction time and the ratio of lead halide precursors. The synthesized CsPbX3/CsPb2X5 composite microplates exhibit an emission light spectrum that covers the entire visible range. Crystallographic analyses and density functional theory (DFT) calculations reveal a minimal lattice mismatch between the (002) plane of CsPb2X5 and the (11¯0) plane of CsPbX3, facilitating the formation of high-quality type-I heterojunctions. Furthermore, introducing Cl- and I- significantly alters the surface energy of CsPb2X5's (110) plane, leading to an evolutionary morphological shift of grains from circular to square microplates. Benefiting from the passivation of CsPb2X5, the composites exhibit enhanced optical properties and stability. Subsequently, the white light-emitting diode prepared using the CsPbX3/CsPb2X5 composite microplates has a high luminescence efficiency of 136.76 lm/W and the PL intensity decays by only 3.6% after 24 h of continuous operation.

16.
J Chem Phys ; 139(16): 164713, 2013 Oct 28.
Article in English | MEDLINE | ID: mdl-24182070

ABSTRACT

The plasmonic optical properties of nanostructures including a dimer, a linear chain, a T-shaped nanostructure, and a 2D array consisting of Ag nanocubes have been investigated using the discrete dipole approximation method. The simulation results indicate that both the interparticle gap and polarization have an important impact on far-field and near-field characteristics. With decreasing interparticle distance for four nanostructures, the plasmon resonance peak is monotonically red-shifted and the electric intensity enhancement factor increases rapidly due to increased interparticle coupling interaction. Moreover, we also find that a T-shaped nanostructure has the largest electric intensity enhancement factor compared with other three nanostructures due to the coupling interaction at the intersection. This coupling is caused by the radiative interference between subradiant and superradiant resulting in Fano resonance. These results show how nanostructure arrangement design, gap adjustment, and polarization control can be used to achieve high field enhancements.

17.
ACS Appl Mater Interfaces ; 15(9): 12383-12392, 2023 Mar 08.
Article in English | MEDLINE | ID: mdl-36821493

ABSTRACT

Lead-free double perovskites (DP) have the potential to become a rising star in the next generation of lighting markets by addressing the toxicity and instability issues associated with traditional lead-based perovskites. However, high concentrations of hydrochloric acid (HCl) were often employed as a solvent in the preparation of most DPs, accompanied by slow crystallization at high temperatures, which not only raised the risk and cost in the preparation process, but also had a potential threat to the environment. Here, an in situ fabrication strategy was proposed to realize the crystallization of DP in the polymer at low temperature with a mild dimethyl sulfoxide (DMSO) solvent, and subsequently obtained optically well-behaved Cs2Na0.8Ag0.2BiCl6/PMMA composite films (CFs) by doping with Ag+, generating bright orange luminescence with a photoluminescence quantum yield (PLQY) of up to 21.52%. Moreover, the growth dynamics of Cs2Na0.8Ag0.2BiCl6/PMMA CFs was further investigated by in situ optical transformation, which was extended to other DP-based polymer CFs. Finally, these CFs exhibited excellent performance in optoelectronic devices and anticounterfeit printing, the results of which provide a new pathway to advance the development of lead-free DP materials in the optical field.

18.
Nanoscale ; 15(26): 11190-11198, 2023 Jul 06.
Article in English | MEDLINE | ID: mdl-37340973

ABSTRACT

The thermal stability of phosphor materials had long been a bottleneck in their commercialization. Nowadays, cesium lead halide perovskite CsPbBr3 has been considered a potential replacement for the next generation of optoelectronic devices due to its excellent optical and electronic properties, however, the devices inevitably generate high temperatures on the surface under prolonged energization conditions in practical applications, which can be fatal to CsPbBr3. Despite the various strategies that have been employed to improve the thermal stability of CsPbBr3, systematic studies of the thermal stability of the basis CsPbBr3 are lacking. In this study, CsPbBr3 with different dimensions (0D quantum dots (QDs), 1D nanowires (NWs), 2D nanoplate (NPs), 3D micron crystals (MCs)) was prepared by traditional high-temperature thermal injection, and a systematic study was carried out on their optical properties and thermal stability. The results revealed that the dimensional change will directly influence the optical properties as well as the thermal stability of CsPbBr3. In particular, 3D CsPbBr3 MCs maintained relatively high thermal stability under high-temperature environments, which will bring interest for the commercialization of next-generation perovskite optoelectronic devices.

19.
Adv Mater ; 35(35): e2212161, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37159949

ABSTRACT

Wearable sweat sensors have the potential to revolutionize precision medicine as they can non-invasively collect molecular information closely associated with an individual's health status. However, the majority of clinically relevant biomarkers cannot be continuously detected in situ using existing wearable approaches. Molecularly imprinted polymers (MIPs) are a promising candidate to address this challenge but haven't yet gained widespread use due to their complex design and optimization process yielding variable selectivity. Here, QuantumDock is introduced, an automated computational framework for universal MIP development toward wearable applications. QuantumDock utilizes density functional theory to probe molecular interactions between monomers and the target/interferent molecules to optimize selectivity, a fundamentally limiting factor for MIP development toward wearable sensing. A molecular docking approach is employed to explore a wide range of known and unknown monomers, and to identify the optimal monomer/cross-linker choice for subsequent MIP fabrication. Using an essential amino acid phenylalanine as the exemplar, experimental validation of QuantumDock is performed successfully using solution-synthesized MIP nanoparticles coupled with ultraviolet-visible spectroscopy. Moreover, a QuantumDock-optimized graphene-based wearable device is designed that can perform autonomous sweat induction, sampling, and sensing. For the first time, wearable non-invasive phenylalanine monitoring is demonstrated in human subjects toward personalized healthcare applications.


Subject(s)
Biosensing Techniques , Graphite , Wearable Electronic Devices , Humans , Molecular Docking Simulation , Biosensing Techniques/methods , Sweat/chemistry , Graphite/chemistry
20.
Nanomaterials (Basel) ; 13(19)2023 Oct 04.
Article in English | MEDLINE | ID: mdl-37836344

ABSTRACT

Perovskite nanocrystals (PeNCs) have emerged as a promising class of luminescent materials offering size and composition-tunable luminescence with high efficiency and color purity in the visible range. PeNCs doped with Yb3+ ions, known for their near-infrared (NIR) emission properties, have gained significant attention due to their potential applications. However, these materials still face challenges with weak NIR electroluminescence (EL) emission and low external quantum efficiency (EQE), primarily due to undesired resonance energy transfer (RET) occurring between the host and Yb3+ ions, which adversely affects their emission efficiency and device performance. Herein, we report the synergistic enhancement of NIR emission in a CsPbCl3 host through co-doping with Yb3+/Nd3+ ions for perovskite LEDs (PeLEDs). The co-doping of Yb3+/Nd3+ ions in a CsPbCl3 host resulted in enhanced NIR emission above 1000 nm, which is highly desirable for NIR optoelectronic applications. This cooperative energy transfer between Yb3+ and Nd3+ can enhance the overall efficiency of energy conversion. Furthermore, the PeLEDs incorporating the co-doped CsPbCl3/Yb3+/Nd3+ PeNCs as an emitting layer exhibited significantly enhanced NIR EL compared to the single doped PeLEDs. The optimized co-doped PeLEDs showed improved device performance, including increased EQE of 6.2% at 1035 nm wavelength and low turn-on voltage. Our findings highlight the potential of co-doping with Yb3+ and Nd3+ ions as a strategy for achieving synergistic enhancement of NIR emission in CsPbCl3 perovskite materials, which could pave the way for the development of highly efficient perovskite LEDs for NIR optoelectronic applications.

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