53% Efficient Red Emissive Carbon Quantum Dots for High Color Rendering and Stable Warm White-Light-Emitting Diodes
TL;DR: An ultraviolet (UV)-pumped CQD phosphors-based warm white light-emitting diode (WLED) is realized for the first time and achieves a color rendering index of 97.
Abstract: Red emissive carbon quantum dots (R-CQDs) with quantum yield of 53% is successfully prepared. An ultraviolet (UV)-pumped CQD phosphors-based warm white light-emitting diode (WLED) is realized for the first time and achieves a color rendering index of 97. This work provides a new avenue for the exploration of low cost, environment-friendly, and high-performance CQD phosphors-based warm WLEDs.
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TL;DR: CPDs are revealed as an emerging class of CDs with distinctive polymer/carbon hybrid structures and properties, and critical insights into facilitating their potential in various application fields are proposed.
Abstract: Despite the various synthesis methods to obtain carbon dots (CDs), the bottom-up methods are still the most widely administrated route to afford large-scale and low-cost synthesis. However, as CDs are developed with increasing reports involved in producing many CDs, the structure and property features have changed enormously compared with the first generation of CDs, raising classification concerns. To this end, a new classification of CDs, named carbonized polymer dots (CPDs), is summarized according to the analysis of structure and property features. Here, CPDs are revealed as an emerging class of CDs with distinctive polymer/carbon hybrid structures and properties. Furthermore, deep insights into the effects of synthesis on the structure/property features of CDs are provided. Herein, the synthesis methods of CDs are also summarized in detail, and the effects of synthesis conditions of the bottom-up methods in terms of the structures and properties of CPDs are discussed and analyzed comprehensively. Insights into formation process and nucleation mechanism of CPDs are also offered. Finally, a perspective of the future development of CDs is proposed with critical insights into facilitating their potential in various application fields.
631 citations
TL;DR: This work demonstrates multicolored narrow bandwidth emission from triangular CQDs with a quantum yield up to 54–72% and synthesizes these dots showing tunable emission color, high fluorescence and a narrow FWHM of only 30 nanometers, which will set the stage for developing next-generation high-performance C QDs-based light-emitting diodes.
Abstract: Carbon quantum dots (CQDs) have emerged as promising materials for optoelectronic applications on account of carbon’s intrinsic merits of high stability, low cost, and environment-friendliness. However, the CQDs usually give broad emission with full width at half maximum exceeding 80 nm, which fundamentally limit their display applications. Here we demonstrate multicolored narrow bandwidth emission (full width at half maximum of 30 nm) from triangular CQDs with a quantum yield up to 54–72%. Detailed structural and optical characterizations together with theoretical calculations reveal that the molecular purity and crystalline perfection of the triangular CQDs are key to the high color-purity. Moreover, multicolored light-emitting diodes based on these CQDs display good stability, high color-purity, and high-performance with maximum luminance of 1882–4762 cd m−2 and current efficiency of 1.22–5.11 cd A−1. This work will set the stage for developing next-generation high-performance CQDs-based light-emitting diodes.
592 citations
TL;DR: Three strategies for structural engineering of CDs are presented and analyzed, in terms of the tuning of size and crystallinity, and the methodologies for surface modification and heteroatom doping, with a focus on the relationship among the synthesis methods, structure and properties of the concerned CDs.
Abstract: The emergence of carbon dots (CDs) has opened up an exciting new field in the science and technology of carbon nanomaterials and has attracted increasing interest in recent years. Due to their diverse physicochemical properties and favourable attributes, such as quantum confinement effects and abundant surface defects, CDs and their derived hybrids have shown exciting and indispensable prospects in the energy conversion and storage fields. Considering the latest developments, in this review, we comprehensively summarize the classification and structure of CDs. Three strategies for structural engineering of CDs are presented and analyzed, in terms of the tuning of size and crystallinity, and the methodologies for surface modification and heteroatom doping, with a focus on the relationship among the synthesis methods, structure and properties of the concerned CDs. More importantly, the recent advances in energy-oriented applications of CDs, including photo- and electro-catalysis, light-emitting diodes, photovoltaic cells, lithium/sodium ion batteries and supercapacitors, will be systematically highlighted. Finally, we discuss and outline the remaining major challenges and opportunities for CDs in the future.
476 citations
TL;DR: In this paper, the authors reviewed recent progress on CDs utilized for photocatalysis from different perspectives, including the following three parts: classification and synthesis, mechanism of CDs-derived photocatalysts as well as the applications for environmental issues (up-converted photoluminescence (PL) and energy conversion).
471 citations
TL;DR: The collective properties of the Mn‐CD assembly enable it to be utilized as an acidic H2O2‐driven oxygenerator to increase the oxygen concentration in hypoxic solid tumors for simultaneous bimodal FL/MR imaging and enhanced PDT.
Abstract: Recent studies indicate that carbon dots (CDs) can efficiently generate singlet oxygen (1 O2 ) for photodynamic therapy (PDT) of cancer. However, the hypoxic tumor microenvironment and rapid consumption of oxygen in the PDT process will severely limit therapeutic effects of CDs due to the oxygen-dependent PDT. Thus, it is becoming particularly important to develop a novel CD as an in situ tumor oxygenerator for overcoming hypoxia and substantially enhancing the PDT efficacy. Herein, for the first time, magnetofluorescent Mn-CDs are successfully prepared using manganese(II) phthalocyanine as a precursor. After cooperative self-assembly with DSPE-PEG, the obtained Mn-CD assembly can be applied as a smart contrast agent for both near-infrared fluorescence (FL) (maximum peak at 745 nm) and T1 -weighted magnetic resonance (MR) (relaxivity value of 6.97 mM-1 s-1 ) imaging. More interestingly, the Mn-CD assembly can not only effectively produce 1 O2 (quantum yield of 0.40) but also highly catalyze H2 O2 to generate oxygen. These collective properties of the Mn-CD assembly enable it to be utilized as an acidic H2 O2 -driven oxygenerator to increase the oxygen concentration in hypoxic solid tumors for simultaneous bimodal FL/MR imaging and enhanced PDT. This work explores a new biomedical use of CDs and provides a versatile carbon nanomaterial candidate for multifunctional nanotheranostic applications.
398 citations
References
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TL;DR: It is reported that nanoscale carbon particles (carbon dots) upon simple surface passivation are strongly photoluminescent in both solution and the solid state.
Abstract: We report that nanoscale carbon particles (carbon dots) upon simple surface passivation are strongly photoluminescent in both solution and the solid state. The luminescence emission of the carbon dots is stable against photobleaching, and there is no blinking effect. These strongly emissive carbon dots may find applications similar to or beyond those of their widely pursued silicon counterparts.
3,817 citations
TL;DR: A facile and highoutput strategy for the fabrication of CDs, which is suitable for industrial-scale production and is almost equal to fluorescent dyes, is discussed.
Abstract: Fluorescent carbon-based materials have drawn increasing attention in recent years owing to exceptional advantages such as high optical absorptivity, chemical stability, biocompatibility, and low toxicity. These materials primarily include carbon dots (CDs), nanodiamonds, carbon nanotubes, fullerene, and fluorescent graphene. The superior properties of fluorescent carbon-based materials distinguish them from traditional fluorescent materials, and make them promising candidates for numerous exciting applications, such as bioimaging, medical diagnosis, catalysis, and photovoltaic devices. Among all of these materials, CDs have drawn the most extensive notice, owing to their early discovery and adjustable parameters. However, many scientific issues with CDs still await further investigation. Currently, a broad series of methods for obtaining CD-based materials have been developed, but efficient one-step strategies for the fabrication of CDs on a large scale are still a challenge in this field. Current synthetic methods are mainly deficient in accurate control of lateral dimensions and the resulting surface chemistry, as well as in obtaining fluorescent materials with high quantum yields (QY). Moreover, it is important to expand these kinds of materials to novel applications. Herein, a facile and highoutput strategy for the fabrication of CDs, which is suitable for industrial-scale production (yield is ca. 58%), is discussed. The QY was as high as ca. 80%, which is the highest value recorded for fluorescent carbon-based materials, and is almost equal to fluorescent dyes. The polymer-like CDs were converted into carbogenic CDs by a change from low to high synthesis temperature. The photoluminescence (PL) mechanism (high QY/PL quenching) was investigated in detail by ultrafast spectroscopy. The CDs were applied as printing ink on the macro/micro scale and nanocomposites were also prepared by polymerizing CDs with certain polymers. Additionally, the CDs could be utilized as a biosensor reagent for the detection of Fe in biosystems. The CDs were prepared by a hydrothermal method, which is described in the Supporting Information (Figure 1a; see also the Supporting Information, Figure S1). The reaction was conducted by first condensing citric acid and ethylenediamine, whereupon they formed polymer-like CDs, which were then carbonized to form the CDs. The morphology and structure of CDs were confirmed by analysis. Figure 1b shows transmission electron microscopy (TEM) images of the CDs, which can be seen to have a uniform dispersion without apparent aggregation and particle diameters of 2–6 nm. The sizes of CDs were also measured by atomic force microscopy (AFM; Figure S2), and the average height was 2.81 nm. From the high-resolution TEM, most particles are observed to be amorphous carbon particles without any lattices; rare particles possess well-resolved lattice fringes. With such a low carbon-lattice-structure content, no obvious D or G bands were detected in the Raman spectra of the CDs (Figure S3). The XRD patterns of the CDs (Figure 1c) also displayed a broad peak centered at 258 (0.34 nm), which is also attributed to highly disordered carbon atoms. Moreover, NMR spectroscopy (H and C) was employed to distinguish sp-hybridized carbon atoms from sp-hybridized carbon atoms (Figure S4). In the H NMR spectrum, sp carbons were detected. In the C NMR spectrum, signals in the range of 30–45 ppm, which correspond to aliphatic (sp) carbon atoms, and signals from 100–185 ppm, which are indicative of sp carbon atoms, were observed. Signals in the range of 170– 185 ppm, which correspond to carboxyl/amide groups, were also present. In the FTIR analysis of CDs, the following were observed: stretching vibrations of C OH at 3430 cm 1 and C H at 2923 cm 1 and 2850 cm , asymmetric stretching vibrations of C-NH-C at 1126 cm , bending vibrations of N H at 1570 cm , and the vibrational absorption band of C=O at 1635 cm 1 (Figure S5). Moreover, the surface groups were also investigated by XPS analysis (Figure 1d). C1s analysis revealed three different types of carbon atoms: graphitic or aliphatic (C=C and C C), oxygenated, and nitrous (Table S1). In the UV/Vis spectra, the peak was focused on 344 nm in an aqueous solution of CDs. In the fluorescence spectra, CDs have optimal excitation and emission wavelengths at 360 nm and 443 nm, and show a blue color under a hand-held UV lamp (Figure 2a). Excitation-dependent PL behavior was [*] S. Zhu, Q. Meng, Prof. J. Zhang, Y. Song, Prof. K. Zhang, Prof. B. Yang State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University Changchun, 130012 (P. R. China) E-mail: byangchem@jlu.edu.cn
3,095 citations
TL;DR: Carbon dots with tunable photoluminescence (PL) and a quantum yield of up to 35% in water were hydrothermally synthesized in one pot and separated via silica column chromatography, and these separated CDs emitted bright and stable luminescence in gradient colors under a single-wavelength UV light.
Abstract: Carbon dots (CDs) with tunable photoluminescence (PL) and a quantum yield of up to 35% in water were hydrothermally synthesized in one pot and separated via silica column chromatography. These separated CDs emitted bright and stable luminescence in gradient colors from blue to red under a single-wavelength UV light. They exhibited high optical uniformity; that is, every sample showed only one peak in the PL excitation spectrum, only one peak in the excitation-independent PL emission spectrum, and similar monoexponential fluorescence lifetimes. Although these samples had similar distributions of particle size and graphite structure in their carbon cores, the surface state gradually varied among the samples, especially the degree of oxidation. Therefore, the observed red shift in their emission peaks from 440 to 625 nm was ascribed to a gradual reduction in their band gaps with the increasing incorporation of oxygen species into their surface structures. These energy bands were found to depend on the surfac...
1,707 citations
TL;DR: The facile preparation and unique optical features make these CDs potentially useful in numerous applications such as light-emitting diodes, full-color displays, and multiplexed (UC)PL bioimaging.
Abstract: A facile approach for preparation of photoluminescent (PL) carbon dots (CDs) is reported. The three resulting CDs emit bright and stable red, green and blue (RGB) colors of luminescence, under a single ultraviolet-light excitation. Alterations of PL emission of these CDs are tentatively proposed to result from the difference in their particle size and nitrogen content. Interestingly, up-conversion (UC)PL of these CDs is also observed. Moreover, flexible full-color emissive PVA films can be achieved through mixing two or three CDs in the appropriate ratios. These CDs also show low cytotoxicity and excellent cellular imaging capability. The facile preparation and unique optical features make these CDs potentially useful in numerous applications such as light-emitting diodes, full-color displays, and multiplexed (UC)PL bioimaging.
1,504 citations
TL;DR: In this article, recent exciting progresses on CD and GQD-based optoelectronic and energy devices, such as light emitting diodes (LEDs), solar cells (SCs), photodetctors (PDs), photocatalysis, batteries, and supercapacitors are highlighted.
Abstract: As new members of carbon material family, carbon and graphene quantum dots (CDs, GQDs) have attracted tremendous attentions for their potentials for biological, optoelectronic, and energy related applications. Among these applications, bio-imaging has been intensively studied, but optoelectronic and energy devices are rapidly rising. In this Feature Article, recent exciting progresses on CD- and GQD-based optoelectronic and energy devices, such as light emitting diodes (LEDs), solar cells (SCs), photodetctors (PDs), photocatalysis, batteries, and supercapacitors are highlighted. The recent understanding on their microstructure and optical properties are briefly introduced in the first part. Some important progresses on optoelectronic and energy devices are then addressed as the main part of this Feature Article. Finally, a brief outlook is given, pointing out that CDs and GQDs could play more important roles in communication- and energy-functional devices in the near future.
1,023 citations