ACS Nano
·
2023
·
IF 17.1
Shiang Li,Ziqi Wang,Yuhao Li,Chun-Jen Su,Yuang Fu,Yi Wang,Xinhui Lu
Due to their versatile applications, perovskite quantum dot (PQD)-based optoelectrical devices have garnered significant research attention. However, the fundamental packing behavior of PQDs in thin films and its impact on the device performance remain relatively unexplored. Drawing inspiration from theoretical models concerning packing density with size mixtures, this study presents an effective strategy, namely, binary-disperse mixing, aimed at enhancing the packing density of PQD films. Comprehensive grazing-incidence small-angle X-ray characterization suggested that the PQD film consists of three phases: two monosize phases and one binary mixing phase. The volume fraction and population of the binary-size phase can be tuned by mixing an appropriate amount of large and small PQDs. Furthermore, we performed multi-length-scale all-atom and coarse-grained molecular dynamics simulations to elucidate the distribution and conformation of organic surface ligands, highlighting their influence on PQD packing. Notably, the mixing of two PQDs of different sizes promotes closer face-to-face contact. The densely packed binary-disperse film exhibited largely suppressed trap-assisted recombination, much longer carrier lifetime, and thereby improved power conversion efficiency. Hence, this study provides fundamental understanding of the packing mechanism of perovskite quantum dots and highlights the significance of packing density for PQD-based solar cells.
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高影响因子
MOLECULES
·
2023
·Vol. 28
·期 21
·7310
·
IF 4.6
Yiting Gu,Xin Du,Feng Hua,Jianfeng Wen,Ming Li,Tao Tang
Inorganic halide perovskite CsPbI3is highly promising in the photocatalytic field for its strong absorption of UV and visible light. Among the crystal phases of CsPbI3, the δ-phase as the most aqueous stability; however, directly using it in water is still not applicable, thus limiting its dye photodegradation applications in aqueous solutions. Via adopting nitrogen-doped graphene quantum dots (NGQDs) as surfactants to prepare δ-phase CsPbI3nanocrystals, we obtained a water-stable material, NGQDs-CsPbI3. Such a material can be well dispersed in water for a month without obvious deterioration. High-resolution transmission electron microscopy and X-ray diffractometer characterizations showed that NGQDs-CsPbI3is also a δ-phase CsPbI3after NGQD coating. The ultraviolet-visible absorption spectra indicated that compared to δ-CsPbI3, NGQDs-CsPbI3has an obvious absorption enhancement of visible light, especially near the wavelength around 521 nm. The good dispersity and improved visible-light absorption of NGQDs-CsPbI3benefit their aqueous photocatalytic applications. NGQDs-CsPbI3alone can photodegrade 67% rhodamine B (RhB) in water, while after compositing with TiO2, NGQDs-CsPbI3/TiO2exhibits excellent visible-light photocatalytic ability, namely, it photodegraded 96% RhB in 4 h. The strong absorption of NGQDs-CsPbI3in the visible region and effective transfer of photogenerated carriers from NGQDs-CsPbI3to TiO2play the key roles in dye photodegradation. We highlight NGQDs-CsPbI3as a water-stable halide perovskite material and effective photocatalytic adjuvant.Keywords:nitrogen doping;graphene quantum dot;perovskite;photodegradation
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Sibo Zhao,Hengbin Mao,Weishan Ma,Mingliang Li,Shao Gang,Bingbing Fan,Hailong Wang,Hongliang Xu,Hongxia Lu
All-inorganic halide perovskite nanocrystals (NCs) have attracted much attention in many fields. However, the poor stability of NCs and the toxicity of Pb have greatly hindered their practical applications. Reducing the proportion of Pb with the concept of high-entropy and coating NCs with an outer layer have been regarded as effective strategies to solve the problems. Herein, We have successfully synthesized the all-inorganic high-entropy dual-phase Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Cd 1/5 )Br 3 /Cs(Pb 1/5 Mn 1/5 Ni 1/5 Zn 1/5 Cd 1/5 ) 2 Br 5 (Cs‘B’Br 3 /Cs‘B’ 2 Br 5 ) perovskite NCs with good luminescence properties by a high-energy ball milling method; On the basis of which, Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs are coated with SiO 2 and EVA resin. Due to the amorphous SiO 2 protection, the Cs‘B’Br 3 /Cs‘B 2 ’Br 5 @SiO 2 NCs maintained 93% of their emission intensity after 90 days compared to their uncoated counterparts. The PL intensity of Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs /EVA was significantly enhanced by a factor of 4.7 for compared to the uncoated NCs. In addition, the PL emission intensity of the Cs‘B’Br 3 /Cs‘B 2 ’Br 5 NCs /EVA remained 93.7% after 90 days, and the emission peak intensity remained approximately 63% after 8 h of placement in an enclosed environment at 80% humidity through the dense polymer chains and the hydrophobic nature of the film. Finally, the film could expand its application prospects in the field of flexible device.
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Laser & Photonics Reviews
·
2023
·Vol. 18
·期 1
·2300809
·
IF 11
Xiankun Zheng,Lijin Wang,Jialin Bai,Han Zhang,Hanzhuang Zhang,Aiwei Tang,Wenyu Ji
Currently, the performance of quantum-dot light-emitting diodes (QLEDs) based on environmental-friendly Cu─In─Zn─S quantum dots (QDs) still lags far behind that of Cd-QDs-based devices. Here it is demonstrated that the unique trap-related recombination in Cu─In─Zn─S QDs is mainly responsible for the low device efficiency. The luminous efficiency of Cu─In─Zn─S-based QLEDs is rather sensitive to the temperature and hole-transporting layers (HTLs) due to the susceptible thermal-related trappingdetrapping processes of holes in radiative Cu-related traps. The holes in Cu-related traps can be quenched by escaping to the valence band of the QDs or/and transferring to the adjacent HTLs. An HTL with low highest occupied molecular orbitals is desired to enhance the hole injection and hinder the aforementioned hole transfer. As a result, a high device efficiency of 6.0 cd A −1 is achieved at room temperature, which is attributed to suppressed HTL-induced emission quenching and efficient valence-band-dominated hole injection from HTL to the QDs. The device efficiency is further increased to 13.2 cd A −1 at 150K by suppressing thermal-induced quenching.
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Frontiers of Optoelectronics
·
2023
·Vol. 16
·期 1
·1-10
·
IF 5.4
Zhao Xinzhao,Li Mingyu,Ma Tianjun,Yan Jun,Khalaf Gomaa Mohamed Gomaa,Chen Chao,Hsu Hsien-Yi,Song Haisheng,Tang Jiang
Infrared solar cells are more effective than normal bandgap solar cells at reducing the spectral loss in the near-infrared region, thus also at broadening the absorption spectra and improving power conversion efficiency. PbS colloidal quantum dots (QDs) with tunable bandgap are ideal infrared photovoltaic materials. However, QD solar cell production suffers from small-area-based spin-coating fabrication methods and unstable QD ink. Herein, the QD ink stability mechanism was fully investigated according to Lewis acid–base theory and colloid stability theory. We further studied a mixed solvent system using dimethylformamide and butylamine, compatible with the scalable manufacture of method-blade coating. Based on the ink system, 100 cm 2 of uniform and dense near-infrared PbS QDs (~ 0.96 eV) film was successfully prepared by blade coating. The average efficiencies of above absorber-based devices reached 11.14% under AM1.5G illumination, and the 800 nm-filtered efficiency achieved 4.28%. Both were the top values among blade coating method based devices. The newly developed ink showed excellent stability, and the device performance based on the ink stored for 7 h was similar to that of fresh ink. The matched solvent system for stable PbS QD ink represents a crucial step toward large area blade coating photoelectric devices. Graphical Abstract
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Zhaolun Yang,Xi Yuan,Yusheng Song,Mingyan Chen,Ke Xing,Sheng Cao,Jinju Zheng,Jialong Zhao
Mn-doped CsPbBr3 perovskite nanoplatelets (NPLs) with multicolor emission have very promising applications in light-emitting devices. However, the effects of NPL thickness on the Mn2+ luminescence properties remain to be investigated. Herein, a series of Mn-doped CsPbBr3 NPLs and nanocubes with different Mn/Pb molar ratios were synthesized by a supersaturated crystallization method at room temperature. The incorporation of Mn2+ ions into CsPbBr3 perovskites is attributed to the formation of the L2[Pb1–xMnx]Br4 intermediate structure in the precursor. The excitonic peak is tuned from 437 to 488 nm and the morphology evolves from NPLs to nanocubes with an increasing Mn2+ ion doping concentration due to the excess Br– from MnBr2. The photoluminescence quantum yields (PL QYs) of NPLs/nanocubes were greatly enhanced, achieving the maximum PL QYs of 88.7% at the Mn/Pb molar ratio of 3/1. The PL lifetime of Mn2+ emission is tuned from 0.19 to 0.44 ms due to the passivation of defect states and morphology transformation. Temperature-dependent steady-state and time-resolved PL spectra revealed that deep defect states in the NPLs/nanocubes were significantly reduced as the thickness increased. The Mn-doped CsPbBr3 NPLs/nanocubes show great potential for application in white light-emitting diodes.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 44
·15531-15540
·
IF 6.4
Yin Lv,Shuhua Tu,Min Chen
All-inorganic CsPbX3 (X = Cl, Br, I) perovskite quantum dots (PQDs)/polymer composite films have been used widely in light-emitting devices. Most methods of fabricating CsPbX3 PQDs/polymer composite films cannot meet the diverse requirements of real applications, particularly with regard to depositing or transferring films on different substrate types, including non-planar surfaces. It is still a challenge to prepare freestanding CsPbX3 PQDs/polymer composite films and deposit them on various substrates (especially non-planar substrates). Here, we report a facile way to prepare freestanding CsPbX3 PQDs/poly(styrene–ethylene–butylene–styrene) (SEBS) composite films via an interfacial-confinement (IC) strategy. The as-obtained films were applicable to various substrates (even curved and flexible substrates) and exhibited excellent stability against various environments. These freestanding CsPbX3 PQDs/SEBS composite films could be patterned readily for anti-counterfeiting and information-encryption applications. They also could be employed as color-conversion materials for white light-emitting diodes (LEDs).
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Shuai Zhang,Linxiang Yang,Gaoyu Liu,Shengli Zhang,Qingsong Shan,Haibo Zeng
I–III–VI quantum dots (QDs) and derivatives (I, III, and VI are Ag+/Cu+, Ga3+/In3+, and S2–/Se2–, respectively) are the ideal candidates to replace II–VI (e.g., CdSe) and perovskite QDs due to their nontoxicity, pure color, high photoluminescence quantum yield (PLQY), and full visible coverage. However, the chaotic cation alignment in multielement systems can easily lead to the formation of multiple surface vacancies, highlighted as VI and VVI, leading to nonradiative recombination and nonequilibrium carrier distribution, which severely limit the performance improvement of materials and devices. Here, based on Zn–Ag–In–Ga–S QDs, we construct an ultrathin indium sulfide shell that can passivate electron vacancies and convert donor/acceptor level concentrations. The optimized In-rich 2-layer indium sulfide structure not only enhances the radiative recombination rate by preventing further VS formation but also achieves the typical DAP emission enhancement, achieving a significant increase in PLQY to 86.2% at 628 nm. Moreover, the optimized structure can mitigate the lattice distortion and make the carrier distribution in the interior of the QDs more balanced. On this basis, red QD light-emitting diodes (QLEDs) with the highest external quantum efficiency (EQE; 5.32%) to date were obtained, providing a novel scheme for improving I–III–VI QD-based QLED efficiency.
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Advanced Healthcare Materials
·
2023
·Vol. 12
·期 32
·2301559
·
IF 10
Guorong Jia,Tao Wang,Rou Li,Xiao Li,Gaofeng Sun,Wei Chen,Ye Peng,Chao Cheng,Jijin Yang,Changjing Zuo
In interventional treatment, materials are administered into the blood supply artery and directly delivered to tumors, offering proper scenarios for nanomedicine potential clinical applications. Transarterial chemoembolization (TACE) and transarterial radioembolization (TARE) are effective treatment methods for hepatocellular carcinoma (HCC), but postoperative residual tumor may result in intrahepatic recurrence and distant metastasis. The combination therapy of TACE and TARE based on multifunctional nanoparticles (NPs) is expected to overcome the drug resistance in hypoxic tumors and improve the therapeutic effect. Herein, BaGdF 5 NPs are synthesized and then coated with polydopamine (PDA), conjugated with the chemotherapeutic drug cis-diamminedichloride platinum (CDDP), radio-labeled with therapeutic radionuclide 131 I, yielding 131 I-BaGdF 5 @PDA-CDDP NPs. The in vitro anti-cancer effects of 131 I-BaGdF 5 @PDA-CDDP NPs are confirmed using CCK-8 and γ-H2AX assays in Huh7 cells. Mixed with Lipiodol, 131 I-BaGdF 5 @PDA-CDDP NPs are injected into the hepatic artery via a microcatheter to realize the TACE and TARE combination therapy in a rabbit VX2 liver tumor model. The results indicate that glucose metabolism is clearly decreased based on 18 F-FDG PET imaging and the apoptosis of tumor cells is increased. Furthermore, 131 I and BaGdF 5 NPs can be used for SPECT imaging and CT/MR imaging respectively, facilitating real-time monitoring of the in vivo biodistribution of 131 I-BaGdF 5 @PDA-CDDP NPs.
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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Dongxue Xiang,Feng Niu,Jing Ji,Junhui Liang,Huayu Chen,Laishun Qin,Yuexiang Huang,Da Chen
Lead halide perovskites (LHPs) quantum dots (QDs) has been deemed as a promising material for photocatalytic conversion (e.g., CO 2 reduction or water splitting) due to their remarkable photoelectrical properties. However, the severe carrier recombination and low charge transfer efficiency largely restrain their photocatalytic performance. Herein, a series of graphene supported dual-phase perovskite QDs photocatalysts were designed by a facile hot-injection strategy for highly efficient photocatalytic CO 2 reduction. Catalytic results showed that under a 5 W white LED irradiation, the CsPbBr 3 /Cs 4 PbBr 6 @G 5% composite with 5 wt% graphene loading exhibited an optimum CO yield of 18.76 μmol g −1 with a selectivity of 52.99% towards the product of CO for photocatalytic CO 2 reduction. The enhanced photocatalytic CO 2 reduction performance over the composites compared with that of CsPbBr 3 , Cs 4 PbBr 6 and CsPbBr 3 /Cs 4 PbBr 6 QDs could be ascribed to the type-I heterojunction structure and graphene support as the electron acceptor in the composite, which could stepwise accelerate the charge separation, suppresses recombination process, and provide more active sites for CO 2 adsorption and reaction. This work would bring new insight in designing novel efficient perovskite-based catalysts for photocatalytic CO 2 transformation.
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JOURNAL OF LUMINESCENCE
·
2023
·
IF 3.6
Ya Chu,Weiqiang Zhang,Yurong Guo,Guangjiu Zhao
Silica-coated perovskite quantum dots (QDs), which exhibit exceptional photophysical properties, hold great promise for various optoelectronic applications. Nonetheless, the issue of insufficient stability poses a significant challenge to their continued advancement and widespread adoption. Herein, we present a novel approach for the synthesis of silica-coated CH 3 NH 3 PbBr 3 (CH 3 NH 3 = MA) QDs with exceptional stability and luminescence, which utilized hydrophobic ionic liquids (ILs) with unlike alkyl chain lengths as surface ligands. As the alkyl chain length of the hydrophobic ILs increased, we observed a blue-shift in the wavelength and a reduction in the time required to reach maximum fluorescence for the silica-coated perovskite QDs . It not only effectively prevents QD aggregation but also accelerates the formation rate of the SiO 2 shell. The introduction of ILs generated the enhancement of photoluminescence quantum yield (PLQY) from 85% for the pristine sample to 92.83% for ILs treated C 16 -QDs@SiO 2 . Furthermore, the stability of the ILs-treated C 16 -QDs@SiO 2 was notably enhanced, with the fluorescence intensity retaining 80.5% after 40 days of storage. The as-prepared white light emitting diode (LED) displayed a high color rendering index (CRI) of 75.3 and a correlated color temperature (CCT) of 7529 K. This work provides an alternative strategy to solve the challenging stability issue of silica-coated perovskite QDs and promote the silica-coated perovskite QDs to the practical application in solid-state LEDs.
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ADVANCED MATERIALS
·
2023
·
IF 29.4
Jingxuan Chen,Donglin Jia,Rongshan Zhuang,Yong Hua,Xiaoliang Zhang
Perovskite quantum dots (PQDs) have emerged as one of the most promising candidates for next-generation solar cells owing to its remarkable optoelectronic properties and solution processability. However, the optoelectronic properties of PQDs suffer from severe degradation in storage due to the dynamically binding ligands, predominantly affecting photovoltaic applications. Herein, an in situ defect healing treatment (DHT) is reported to effectively rejuvenate aged PQDs. Systematically, experimental studies and theoretical calculations are performed to fundamentally understand the causes leading to the recovered optoelectronic properties of aged PQDs. The results reveal that the I 3 − anions produced from tetra- n -octylammonium iodide and iodine could strongly anchor on the surface matrix defects of aged PQDs, substantially diminishing the nonradiative recombination of photogenerated charge carriers. Meanwhile, an DHT could also renovate the morphology of aged PQDs and thus improve the stacking orientation of PQD solids, substantially ameliorating charge carrier transport within PQD solids. Consequently, by using a DHT, the PQD solar cell (PQDSC) yields a high efficiency of up to 15.88%, which is comparable with the PQDSCs fabricated using fresh PQDs. Meanwhile, the stability of PQDSCs fabricated using the rejuvenated PQDs is also largely improved.
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