Soft Matter
·
2022
·Vol. 18
·期 19
·3762-3770
·
IF 4.046
Jilei Chen,Wenrong Fu,Jiaqiang Xiong,Wei Zhang,Feng-Lei Jiang,Liuchun Zheng,Yi Liu,Peng Jiang
Three-dimensional (3D) self-assembled quantum dot (QD) aerogels have attracted attention due to the combined properties of both QDs and porous materials. However, the difficulty and complexity of structural composition control limit the practical application of 3D self-assembled QDs. Hence, convenient, available and multifunction QD aerogels need to be explored to promote broader practical applications. Herein, we propose a universal and facile self-assembly method of copper indium selenium (CISe) QD aerogels based on coordination interaction between Zn2+ and carboxyl. Both experiments and Monte Carlo simulations indicate that QDs are aggregated into oligomers by Zn2+, and then the oligomers are gradually interconnected to each other to form a 3D network as the concentration of Zn2+ increases. Moreover, Zn2+-induced 3D self-assembled aerogel could be depolymerized by EDTA reversibly. In combination with CISe QDs, Zn-CISe aerogel has been successfully applied in green pollution-free environment-friendly anti-counterfeiting and encryption systems.
研究领域:
材料科学
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纳米技术
·
化学工程
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DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Pengtao Sheng,Youyang Xie,Shuyu Han,Yanling Li,Weili Li
Manganese ion-doped quantum dots (QDs) with wide band gaps have been widely investigated to modify their electronic, magnetic, and photophysical properties. The research on Mn-doped Cu-In-Se QDs with narrow band gaps has been minimal due to the profound differences in the reaction reactivity of cations. In this work, photoluminescent and magnetic Cu-In-Se QD nanoprobes were designed and synthesized by introducing Zn 2+ ions, which function as an intermediate acid that can regulate metal ion acidity to enhance the doping efficiency of Mn 2+ ions in a facile phosphine-free hot-injection protocol. The emission peaks of Zn-doped Cu-In-Se QDs and MnZn-doped Cu-In-Se QDs exhibit significant composition-dependent shifts. Moreover, incorporating manganese ions confers a paramagnetic character to MnZn-doped Cu-In-Se QDs and provides a quasi-core shell structure with an Mn-rich alloy shell layer, as demonstrated by the micro-structural surface analysis and electron paramagnetic resonance spectroscopy . Analyzing the decay lifetime and quantum yield reveals that this host-dopant coupling involves a preferential energy transfer from the host material to the dopant (Mn 2+ ions), wherein photogenerated electrons nonradiatively transfer to the 4 T 1 level of Mn dopant and then recombine with the Cu x state above the valance band of host QDs. The ability to serve as nanoprobes for the visualization of tumors through fluorescence and magnetic resonance dual-modality imaging makes these ternary MnZn-doped Cu-In-Se QDs strong candidates for practical applications in biology/biomedicine field.
研究领域:
材料科学
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生物医学工程
·
光学
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DOI
高影响因子
Advanced Electronic Materials
·
2020
·Vol. 6
·期 5
·2000035
·
IF 6.593
Ruiqi Guo,Linxing Zhang,Jie Meng,Aqiang Liu,Jifeng Yuan,Kaibo Zheng,Jianjun Tian
Compared to analogous bulk materials, colloidal nanocrystals have presented a powerful platform for building up electronic devices on the nano/micrometer scale and flexible portable electronic apparatus with the benefits of solution-based processing approach at room temperature. Herein, memristors based on CuInSe 2 (CISe) colloidal nanocrystals prepared using a solution-based process at room temperature are constructed. The memristors exhibit obvious bipolar resistive switching performance with a high–low resistance ratio larger than 5.7 and a steady retention time over 10 4 s. This is attributed to the copper ion redox reaction and the migration of these ions under an applied electric field. When the SET voltage is reached, the ions are separated from one of the electrodes, and the memristor changes from a low-resistance state (LRS) to a high-resistance state (HRS). Conversely, when the voltage reaches the RESET voltage, the memristor switches from a HRS to a LRS. In addition, the flexible memristor can be fabricated by spincoating nanocrystal solution onto polyethylene terephthalate (PET) at room temperature, showing excellent reproducibility of the performance including 100 times of continuous operation, 10 4 s of reproducible reading, 600 times of antifatigue testing, and thermal stability up to 95 °C. The flexible devices demonstrate promising applications for portable electronic devices.
研究领域:
材料科学
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纳米技术
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电子工程
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DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 46
·e202404170
·
IF 1.9
Pengtao Sheng,Haiyan Xu,Yaqi Zhang,Haiyue Xia,Haipeng Liu,Weili Li
Graphical We present a surfactant-associated controlled synthesis of copper (Cu)-deficient zinc (Zn)-doped Cu-indium (In)-selenium (Se) QDs, followed by a mechanistic investigation of their photophysical properties using surfactants. The findings described here are expected to provide a general strategy for enhancing the tunability of photophysical properties in other QDs systems. The shape and size-controlled synthesis of colloidal I−III−VI quantum dots (QDs) can be attained only by a few synthesis strategies via the introduction of various high-boiling-point organic surfactants. To further investigate this strategy, in this study, we present a surfactant-associated controlled synthesis of copper (Cu)-deficient, zinc (Zn)-doped Cu─indium (In)─selenium (Se) QDs, followed by a mechanistic investigation of their photophysical properties using surfactants, such as oleylamine (OLA), oleic acid (OA), and diphenylphosphine (DPP). OLA significantly promoted the quantum size effect-resultant emission wavelength red-shift, while OA controlled the homogeneous growth of QDs and improved the quantum yields. Moreover, Gaussian deconvolution of the photoluminescence spectra and the bandgap derived from the absorption spectra, by fitting, supported the fact that the radiative transition channels, especially for surface-trap-state-related transitions, are also dependent on the surfactants. Specifically, the conduction band electron-intragap state transitions and donor-acceptor transitions were present in all the prepared samples but accounted for different percentages. Furthermore, the surface-trap-state-related transitions significantly faded upon adding (i) OLA/OA as the sole surfactant to the cationic precursor and (ii) the OA + OLA + DPP mixture to the anionic precursor. The findings described here are expected to provide a general strategy for enhancing the tunability of photophysical properties in other QDs systems.
研究领域:
材料科学
·
化学
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DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Jilei Chen,Lu Zhang,Shulan Li,Feng-Lei Jiang,Peng Jiang,Yi Liu
Copper indium selenide (CISe) quantum dots (QDs) are a class of extremely appealing candidates for various biological applications due to their composition- and size-dependent photoluminescence and low toxicity. However, the synthesis of high-quality water-soluble CISe QDs with controlled composition in the aqueous phase is still a great challenge, which limits their biological applications. Moreover, the effects of the copper content in CISe QDs on the fluorescence and the corresponding mechanism are still subject to debate. Herein, a composition-tunable aqueous synthesis of high-quality Cu-deficient CISe QDs was presented, and the effects of the copper content on the fluorescence of CISe QDs was studied by the time-resolved fluorescence. The composition of CISe QDs could be flexibly controlled by manipulating the reaction temperature, the reaction time, and the Cu/In precursor ratio. The time-resolved fluorescence of CISe QDs with different Cu/In ratios suggested that the donor–acceptor pair (DAP) recombination was enhanced gradually with the increase of copper vacancies, resulting in the enhancement of fluorescence. However, if copper vacancies achieved an excessive concentration, the fluorescence would decrease possibly due to Auger recombination. The optimized CISe QDs with the maximum quantum yield of 10.3% were obtained with the Cu/In ratio, reaction temperature, and reaction time of 1/5, 170 °C, and 1 h, respectively. Based on the intense emission of the Cu-deficient CISe QDs, a highly sensitive “turn-on” fluorescent probe was developed for the detection of adenosine triphosphate (ATP) in living cells with a limit of detection of 56 nM. This work provides a paradigm for the aqueous-phase synthesis and applications of ternary I–III–VI QDs.
研究领域:
生物化学
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纳米医学
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分析化学
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DOI
高影响因子
NANO
·
2020
·
IF 1.566
Weili Li,Hongchao Geng,Lu Yao,Haiyan Xu,Yongjun Han,Pengtao Sheng
Oil phase CuInSe 2 quantum dots (CISe QDs) were synthesized via a hot-injection method, exhibiting a near-infrared (NIR) emission wavelength of 710 nm with poor fluorescence intensity. Therefore, we address this challenge by introducing two strategies: doping and ligand exchange. First, Zn was used as a dopant to improve the fluorescent properties of CISe QDs synthesized by the same method. The PL peak position of the resulting Zn–CuInSe (ZnCISe) QDs could be tuned from 600 nm to 662 nm, and the PL intensity of the QDs was greatly improved. Except that, this Zn doping strategy can help to improve the fluorescence lifetime and reduce defects, leading to increased quantum yield. Next, the aqueous phase transfer of ZnCISe QDs was achieved through an efficient ligand exchange strategy using glutathione (GSH) as the bifunctional ligand. Mercaptoacetic acid (MPA) was also used as an essential additive for GSH ligand exchange. With this method, we obtained high-quality hydrophilic ZnCISe QDs with particle sizes less than 3 nm and good monodispersity. In addition, DLS measurements showed a unimodal peak shape of the hydrated ZnCISe QDs in ultrapure water with particle sizes ranging from 7 nm to 40 nm. Finally, the cytotoxicity studies revealed that the viabilities of the cells incubated with ZnCISe QDs from 1 μ g/mL to 18 μ g/mL remained at levels greater than 90%, which indicates that QDs with good biocompatibility are promising fluorescent probes.
研究领域:
材料科学
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生物医学
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DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2020
·Vol. 412
·期 30
·8379-8389
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IF 3.637
Geng Hongchao,Qiao Yan,Jiang Ning,Li Chenyi,Zhu Xingqi,Li Weili,Cai Qingyun
Bacteria are everywhere and pose severe threats to human health and safety. The rapid classification and sensitive detection of bacteria are vital steps of bacterial community research and the treatment of infection. Herein, we developed optical property–superior and heavy metal–free ZnCuInSe quantum dots (QDs) for achieving rapid discrimination of Gram-positive/Gram-negative bacteria by the naked eye; driven by the structural differences of bacteria, ZnCuInSe QDs are effective in binding to Gram-positive bacteria, especially Staphylococcus aureus ( S . aureus ), in comparison with Gram-negative bacteria and give discernable color viewed by the naked eye. Meanwhile, based on its distinctive fluorescence response, the accurate quantification of S . aureus was investigated with a photoluminescence system in the concentration ranges of 1 × 10 3 to 1 × 10 11 CFU/mL, with a limit of detection of 1 × 10 3 CFU/mL. Furthermore, we demonstrated the feasibility of ZnCuInSe QDs as a fluorescence probe for imaging S . aureus . This simple strategy based on ZnCuInSe QDs provides an unprecedented step for rapid and effective bacterial discrimination, detection, and imaging.
研究领域:
微生物学
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生物医学工程
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光学
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DOI
PubMed
高影响因子
Nanoscale Advances
·
2021
·Vol. 3
·期 8
·2334-2342
·
IF 4.553
Senlin Qu,Xin Yuan,Yu Li,Xingyang Li,Xiujuan Zhou,Xiaogang Xue,Kexiang Zhang,Juan Xu,Changlai Yuan
The composition and defect tolerance of CuInSe2 (CISe) quantum dots (QDs) provide a scaffold to design defects via tailoring the elemental ratio or distributions for boosting photocatalytic H2 evolution (PHE). Herein, a ligand-assisted two-step aqueous method was developed to prepare defect CISe quantum dots for the first time. UV-vis, XPS, HRTEM, and HADDF investigations confirmed the typical double-absorption edges of copper vacancy defects and indium substituted at copper site defects in the structure constructed through initial synthesis tuned by Cu/In ratio and the ensued coarsening. The steady-transient PL suggested that the D–A recombination with prolonged PL lifetime dominated the emission of composition-optimized CuInSe2 with the Cu/In ratio of 1/4 (CISe-1/4). Further transient photocurrent and electrochemical impedance spectroscopy investigations demonstrated that surface defects in the structure favor the carriers' separation/transportation. The CISe-1/4 exhibited a superior PHE rate of 722 μmol g−1 h−1, about 23 times higher than that of the initially synthesized CISe-1/4 nucleus (31 μmol g−1 h−1), with a maximum apparent quantum efficiency (AQE) of 1.3%. The analysis of energy levels and the coulombic interaction energy of electron–hole (Je/h) based on Raman, extending UV-vis spectra investigations suggested that surface defects resulted in decreased Je/h of CISe-1/4, favoring the enhanced PHE of this structure. This work is expected to provide a reference for designing effective non-noble metal I–III–VI photocatalysts.
研究领域:
材料科学
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化学
·
能源科学
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DOI
PubMed
高影响因子
Journal of Materials Chemistry C
·
2025
·
IF 5.1
Lizhao Nie,Linqi Chen,Jingzhou Li,Yijing Wang,Xiaoxia Wang,Long Zhang,Hongxing Dong,Anlian Pan
Copper indium selenide (CISe) quantum dots (QDs), a class of narrow bandgap and environmentally friendly QDs, have been developed rapidly for application in the fields of biomedicine, solar cells, and telecommunications. However, synthesizing CISe QDs that emit beyond 800 nm while maintaining high photoluminescence quantum yields (PLQY) remains a significant challenge. Herein, we employed a hot injection solution method to synthesize high-quality core–shell structure Zn:CuInSe2/ZnS QDs by adjusting the stoichiometric ratio of the CISe core and doping with Zn2+. The fabricated QDs exhibit a high PLQY of 62.7% at an emission wavelength of 810 nm with excellent photochemical stability and a large Stokes shift (150 nm). This can be attributed to pre-doping, which suppresses the cation exchange between Zn2+ and Cu+ or In3+ during the shelling process, and the passivation effects of ZnS on surface defects of the QDs. Furthermore, we demonstrate their application by using a home-built optical wireless communication (OWC) test platform, and the prepared QDs exhibit a modulation bandwidth of 3.23 MHz. With a bit error rate (BER) below the forward error correction (FEC) threshold of 0.0038, the system is capable of achieving a maximum data transmission rate of 14 Mbps. The synthesized high-efficiency PLQY Zn:CuInSe2/ZnS QDs could be expected to promote the development of near-infrared (NIR) wireless communications.
研究领域:
材料科学
·
光电子学
·
通信工程
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DOI
高影响因子
GREEN CHEMISTRY
·
2015
·Vol. 17
·期 8
·4482-4488
·
IF 8.02
Xiaojiao Kang,Yanchun Yang,Lijian Huang,Ying Tao,Lan Wang,Daocheng Pan
Water-soluble CuInSe2/ZnS (CISe/ZnS) and AgInSe2/ZnS (AISe/ZnS) core/shell quantum dots (QDs) on a multigram scale have been synthesized by using gelatin and thioglycolic acid as dual stabilizers in an electric pressure cooker. The core/shell QDs present composition-tunable emission in the range of 582 nm to 686 nm with a maximum PLQY of 23.3%. The core/shell QDs also exhibit good water/buffer stability. The red-emitting CISe/ZnS QDs are applied as wavelength converters to achieve warm white light-emitting diodes.
研究领域:
材料科学
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光学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
·
2023
·Vol. 26
·期 24
·e202300303
·
IF 2.3
Youyang Xie,Pengtao Sheng,Weili Li,Yanling Li,Songtian Li
Graphical By changing Cu/In molar ratios of Cu−In−Se QDs from 0.3 : 1 to 0.9 : 1, the photoluminescence spectra displayed a remarkable red-shift from 700 nm to 1050 nm. Although there was a blue-shift after the introduction of Zn 2+ dopants. in Cu−In−Se QDs, a significant red-shift occurred from 660 nm to 760 nm when the Zn/Cu molar ratios decreased from 0.7 : 0.3 to 0.3 : 0.7. These results confirmed the strong effect of the Cu/In and Zn/Cu molar ratios on the intrinsic and dopants states related-transition channels, including the band-edge, conduction band-intragap acceptor, as well as the donor-acceptor. The large structural tolerance of I–III–VI group quantum dots (QDs) to off-stoichiometry allows their photoluminescence properties to be adjusted via doping, thereby enabling application in different fields. However, the photophysical processes underlying their photoluminescence mechanism remain significantly unknown. In particular, the transition channels of CuInSe 2 QDs, which are altered by intrinsic and extrinsic intragap states, remain poorly reported. Herein, we investigated the photophysical processes associated with intragap states via electrochemical and optical techniques by using copper deficient Cu−In−Se QDs as well as Zn doped Cu−In−Se QDs. When the Cu/In molar ratios of Cu−In−Se QDs increased from 0.3 : 1 to 0.9 : 1, the photoluminescence spectra displayed a red-shift from 700 nm to 1050 nm. Although there was a blue-shift after the introduction of Zn 2+ dopants in Cu−In−Se QDs, a significant red-shift occurred (from 660 nm to 760 nm) when the Zn/Cu molar ratios decreased from 0.7 : 0.3 to 0.3 : 0.7. The Gaussian deconvolution results of the photoluminescence spectra and the band gap derived from absorption spectra by fitting supported the fact that the optical transition channels are dependent on the Cu/In and Zn/Cu molar ratios. After the introduction of the Zn 2+ ions, the alloyed-resultant blue-shift of the emission spectra was observed, primarily due to the enlarged band gap; however, the radiative recombination of prominent intrinsic intragap states is still observed; and only a small proportion of the band-edge exciton undergoes recombination for the sample with low Zn content. Cyclic voltammetry measurements revealed well-defined extrinsic Zn Cu intragap states (Zn substitution on Cu sites) and intrinsic Cu x (x= 1+/2+) states in the band gap. The results presented here provide a better understanding of the varying effects of dopant on photoluminescence in terms of I–III–VI group QDs.
研究领域:
材料科学
·
光学
·
物理化学
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DOI
高影响因子
CRYSTENGCOMM
·
2016
·Vol. 18
·期 36
·6860-6866
·
IF 3.849
Hui Liu,Jiaxin Zhang,Xuerong Zheng,Gang Liu,Huilin Hu,Wenli Pan,Caichi Liu,Qiuyan Hao,Hongjian Chen
A mixed solvent of monoethanolamine and thioglycolic acid is successfully used to dissolve Se powder to prepare a highly reactive and soluble Se solution at room temperature in air. The as-prepared Se solution is very stable for more than half a year without any observed precipitation even in air. We used the Se precursor solution to synthesize various metal selenide nanomaterials such as Sb2Se3 nanorods, CuSe nanoplates and CuInSe2 nanocrystals by using a facile and environmentally-friendly triethylene glycol process. The structure, morphology, chemical composition and optical properties of the synthesized metal selenide nanomaterials are characterized. Moreover, the CuInSe2 nanocrystals are used to prepare ethanol-based colloidal ink and then deposited thin films by a dip-coating process. The synthesized CuInSe2 nanocrystal thin films are annealed at 550 °C in a selenizing atmosphere. A power conversion efficiency of 2.65% has been achieved by using the CuInSe2 thin films after selenization as a light-absorbing layer under AM 1.5 illumination.
研究领域:
材料科学
·
纳米技术
·
光伏应用
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）