ACS Applied Nano Materials
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2023
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IF 5.9
Yifang Sun,Liangliang Zhang,Ying Lv,Qinghui Zeng,Xiaoyang Guo,Wenyu Ji,Xingyuan Liu
AgIn5S8/ZnS (AIS/ZS) core/shell quantum dots (QDs) have been synthesized using a hot injection method at relatively low temperature without any protection using inert gas. The QDs were characterized with UV visible electronic absorption spectroscopy, PL spectroscopy, Fourier transform infrared (FT-IR) spectroscopy, transmission electron microscopy (TEM), and temperature-dependent time-resolved PL (TRPL). The average size of the QDs was determined to be 1.73 ± 0.29 nm. The QDs exhibit a major excitonic absorption band peaked at 479–573 nm and emission bands peaked from 548 to 666 nm with excitation at 410 nm with the peak position dependent on the synthesis temperature that affects the QD size. Upon the addition of trioctylphosphine (TOP) as a ligand, the PL quantum yield (PLQY) increased to 74.1% compared to 56.7% without TOP. The QDs show high stability after hours of ultraviolet (UV) light exposure or repetitive treatment with a significant amount of polar solvents, which is attributed to surface passivation by the ligands and ZnS shell. The luminescence mechanism of the core/shell AIS/ZS QDs is ascribed to donor–acceptor pair (DAP) recombination. TRPL results suggest that the binding energy of DAP increases and the DAP recombination probability is enhanced after passivation with TOP, leading to the high PLQY. Furthermore, prototype highly pure white light-emitting diodes (LEDs) based on these AIS/ZS QDs have been successfully demonstrated, yielding ideal 1931 CIE coordinates of (0.327, 0.335).
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Journal of Physical Chemistry C
·
2023
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IF 3.7
Yongqi Zhang,Hongrui Cheng,Xin Chen,Yuanhui Zheng
Two-dimensional (2D) Sn-based perovskites have emerged as a promising alternative to Pb-based perovskites due to their nontoxic nature. However, Sn2+ ions tend to get oxidized to Sn4+ during the synthesis process, leading to crystalline defects and rapid nonradiative transitions, which limits their applications. In this study, we present a facile molecular doping strategy for (C18H35NH3)2SnBr4 perovskite by introducing o-phenylenediamine (oPD) in the precursor solution. The oPD serves a dual role: it not only acts as an electron donor, creating a reducing environment to suppress the oxidation of Sn2+, but also functions as a chelating agent, forming stable compounds with Sn2+. This approach results in 20% oPD doped (C18H35NH3)2SnBr4 perovskite, which exhibits a high photoluminescence quantum yield (PLQY) of 95.3% and excellent stability against oxygen. Furthermore, UV-pumped orange and white light-emitting diodes (LEDs) with a CIE coordinate (0.562, 0.431, 0.327, and 0.346) were produced using oPD-doped 2D tin-based perovskite powders, respectively. These findings suggest that the doping strategy has great potential to enhance the stability of 2D Sn-based perovskites and facilitate their application in the field of lighting devices.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 11
·期 1
·71-84
·
IF 7
Xing-Yao Zhao,Xiao-Song Zhang,Xiao-Kai Gong,Xiu-Rong Yuan,Min-Xing Chen,Shu-Wei Huang,Bao-zeng Zhou,Jian-Ping Xu,Lan Li
Lead-halide perovskites exhibit excellent photovoltaic properties. However, lead's toxicity and limited stability under ambient conditions limit its further commercialization. This paper reports a Bi3+-doped lead-free metal halide, Cs2ZnCl4:Bi3+ nanocrystals (NCs). After doping with Bi3+, the pristine weakly luminescent nanocrystals showed highly efficient broadband blue emission with a peak position of 445 nm, a full width at half-maximum (FWHM) of 92 nm, and a significant increase in the photoluminescence quantum yield (PLQY) to 57.71%. The formation of a water-induced protective layer of BiOCl ensures good water stability. The luminescence mechanism of Cs2ZnCl4:Bi3+ NCs has been investigated by optical characterization and density-functional theory (DFT) calculations, and it has been concluded that the emission of triple-state self-trapped excitons (STEs) induced by Bi3+ doping is the source of broadband blue light emission. Combining nanocrystals as a luminescence down-shifting (LDS) layer with commercial GaAs solar cell devices has solved the problem of the solar cell's weak absorption of short waves, augmenting the photovoltaic conversion efficiency (PCE) by approximately 1%. Additionally, the integration of Cs2ZnCl4:Bi3+ NCs with 365 nm commercial LED chips enables the creation of broadband blue-emitting LED devices. Therefore, we believe that Cs2ZnCl4:Bi3+ NCs have great potential for future optoelectronic applications.
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CRYSTAL GROWTH & DESIGN
·
2023
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IF 3.8
Wei Wan,Yifei Zhao,Shuai Zhang,Fangrui Cheng,Shi Ye
Cesium lead halide (CsPbX3, where X is Cl, Br, or I) perovskite quantum dots (QDs) hold great potential for applications in various devices, on account of their superior electronic and optical properties. However, the poor stability has severely restricted their applications. Herein, by exfoliating K4Nb6O17 into niobate nanosheets (KNO NSs) and utilizing the flocculation of KNO NSs as building blocks, the CsPbBr3/K4–xNb6O17 (CsPbBr3/KNO) nanocomposites were obtained via evaporation of a dimethyl sulfoxide (DMSO) solution and crystallization of CsPbBr3 nanocrystals. The as-synthesized CsPbBr3/KNO nanocomposites possess sandwich-like and scroll-like heterostructures, which consist of restacked KNO NSs and CsPbBr3 in the internanosheet gallery. CsPbBr3/KNO nanocomposites exhibit better exciton emission of CsPbBr3 with a prolonged emission decay time with reference to the value of CsPbBr3 QDs. In addition, the strong interaction at the interfaces of CsPbBr3 and KNO NSs endows CsPbBr3/KNO nanocomposites with significantly improved resistance to alcohol over bare CsPbBr3 QDs. This work paves a new way for utilizing oxide nanosheets as building blocks to synthesize stable all-inorganic perovskite QDs.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Xing-Yao Zhao,Xiao-Song Zhang,Xin Liu,Xiao-Kai Gong,Xiu-Rong Yuan,Bao-zeng Zhou,Jian-Ping Xu,Li-Na Kong,Lan Li
Lead-based perovskite quantum dots (QDs) have promising applications in optoelectronic devices , but commercial applications are limited by the potential toxicity and poor stability of lead. Meanwhile, there are lattice, polarity, and thermal expansion coefficient mismatches in integrating semiconductor materials onto the surface of photoelectronic circuit devices, resulting in high-density defects limiting the reliability of photoelectronic devices. Therefore, there is a need to investigate perovskite alternatives that are non-toxic, stable, and can be effectively coupled to silicon photonic circuits. In this paper, lead-free perovskite Cs 3 Bi 2 Br 9 /SiO 2 QDs were synthesized. The emission wavelength falls within the 400–560 nm range, exhibiting vibrant blue photoluminescence and demonstrating exceptional air stability for a duration exceeding 60 days. Optical tests and density-functional theory (DFT) calculations show that the silica shell layer effectively binds the electron and hole wave functions, prevents photon-generated carriers from escaping, reduces surface defects , and improves the carrier recombination probability. Meanwhile, using Cs 3 Bi 2 Br 9 /SiO 2 QDs as a luminescent down-shifting (LDS) layer in combination with a conventional silicon solar cell , the photovoltaic conversion power was increased by 1.82%. Hence, the core-shell structure is designed by the green environmental protection method to control the improvement of the PL characteristics of QDs , which opens a window for the synthesis of new barrier materials in ethanol and water systems, making the Cs 3 Bi 2 Br 9 /SiO 2 QDs have great potential for the application of novel optoelectronic devices in the future.
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OPTICS EXPRESS
·
2023
·Vol. 31
·期 25
·42400-42412
·
IF 3.8
Yajun Lou,Boyuan Ge,Yue Cai,Xinhai Zhang
Passive mode-locking based on saturable absorbers (SAs) is an effective way to generate ultrafast pulses, while the spatiotemporal mode-locking (STML) based on SAs are rarely studied. We construct an all-fiber laser with InP quantum dots (QDs) SA, and realize multi-mode Q-switching (MMQS) and STML. In addition, by adjusting the polarization controller (PC) in the laser cavity, we obtain two different single-pulse STML states. The narrowest pulse widths of the two states are 57 ps and 32 ps, respectively, and the pulse width can be tuned continuously with increasing the pump power. By decoupling the effects of the PC and the SA in our experiment, we find that the polarization plays a key role in the selection of transverse modes. The effect of independent polarization on spatiotemporal mode-locked pulses has not been investigated before. To further analyze and understand the experimental results, we numerically solve the nonlinear Schrodinger equation, and compare the numerical simulation with the experimental results. In addition to passively adjusting cavity loss, the InP QD SA can balance the large walk off between different transverse modes, due to the spatial and spectral filtering effects. Our work has important implications for the design and application of all-fiber STML lasers.
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INORGANIC CHEMISTRY
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2023
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IF 4.6
Lingfeng Li,Zutao Fan,Jie Zhang,Dianyuan Fan,Xiaogang Liu,Yu Wang
Recently, low-dimensional copper(I)-based perovskite or derivatives have gained extensive attention in scintillator applications because of their environmental friendliness and good stabilities. However, the unsatisfactory scintillation performance and complex fabrication processes hindered their practical applications. Herein, efficient yellow emissive CsCu2I3 nanocrystals (NCs) were successfully prepared via a simple Mn2+-assisted hot-injection method. The added Mn2+ effectively induced the phase transformation from Cs3Cu2I5 to CsCu2I3, leading to the preparation of single-phase CsCu2I3 NCs with few defects and a high fluorescence performance. The as-prepared “optimal CsCu2I3 NCs” exhibited superior photoluminescence (PL) performance with a record-high PL quantum yield (PLQY) of 61.9%. The excellent fluorescence originated from the radiative recombination of strongly localized one-dimension (1D) self-trapped excitons (STEs), which was systematically investigated via the wavelength-dependent PL excitation, PL emission, and temperature-dependent PL spectra. These CsCu2I3 NCs also exhibited outstanding X-ray scintillation properties with a high light yield (32000 photons MeV–1) and an ultralow detection limit (80.2 nGyair s–1). Eventually, the CsCu2I3 NCs scintillator film achieved an ultrahigh (16.6 lp mm–1) spatial resolution in X-ray imaging. The CsCu2I3 NCs also exhibited good stabilities against X-ray irradiation, heat, and environmental storage, indicating their great application potential in flexible X-ray detection and imaging.
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Micromachines
·
2023
·Vol. 14
·期 12
·2186
·
IF 3.4
Yuezhu Wang,Xiaotong Xu,Wenchao Yang,Yawen Wei,Junsheng Wang
All-inorganic lead halide perovskite has emerged as an attractive semiconducting material due to its unique optoelectronic properties. However, its poor environmental stability restricts its broad application. Here, a simple method for the fabrication of CsPb2Br5/TiO2is investigated. The introduction of p-aminobenzoic acid, which has two functional groups, is critical for the capping of amorphous TiO2on CsPb2Br5. After calcination at 300 °C, amorphous TiO2crystallizes into the anatase phase. The CsPb2Br5/TiO2NCs show high long-term stability in water and enhanced stability against ultraviolet radiation and heat treatment, owing to the chemical stability of TiO2. More importantly, photo-electrochemical characterizations indicate that the formation of TiO2shells can increase the charge separation efficiency. Hence, CsPb2Br5/TiO2exhibits improved photoelectric activity owing to the electrical conductivity of the TiO2in water. This study provides a new route for the fabrication of optoelectronic devices and photocatalysts based on perovskite NCs in the aqueous phase. Furthermore, the present results demonstrate that CsPb2Br5/TiO2NCs has considerable potential to be used as a photoelectric material in optical sensing and monitoring.Keywords:TiO2;CsPb2Br5;p-aminobenzoic acid;environmental stability
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ACS Nano
·
2023
·
IF 17.1
Mingze Lu,Haoan Wu,Di Liu,Fei Wang,Yan Wang,Mengjun Wang,Qiannan Cui,He Zhang,Fengchao Zang,Ming Ma,Jun Ma,Fangfang Shi,Yu Zhang
Chemodynamic therapy based on the Fenton-like catalysis ability of Fe3O4 has the advantages of no involvement of chemical drugs and minimal adverse effects as well as the limitation of depletable efficacy. Radiotherapy based on high-energy radiation offers the convenience of treatment and cost-effectiveness but lacks precision and cellular adaptation of tumor cells. Approaching such dilemmas from a nanoscale materials perspective, we aim to bridge the weaknesses of both treatment methods by combining the principles of two therapeutics reciprocally. We have designed a camouflaged Fe3O4@HfO2 composite nanoreactor (FHCM), which combines a chemodynamic therapeutic agent Fe3O4 and a radiosensitizer HfO2 that both has passed clinical trials and was inspired by a cell membrane biomimetic technique. FHCM is employed as conceived radiotherapy-adjuvant chemodynamic synergistic therapy of malignant tumors, which has undergone dual scrutiny from both the physical and biological aspects. Experimental results obtained at different levels, including theory, material characterizations, and in vitro and in vivo verifications, suggest that FHCM effectively impaired tumor cells through physical and molecular biological mechanisms involving a HfO2–Fe3O4 photoelectron–electron transfer chain and DNA damage-ferroptosis-immunity chain. It is worth noting that compared to single therapies such as only chemodynamic therapy or radiotherapy, FHCM-mediated radiotherapy-adjuvant chemodynamic synergistic therapy exhibits stronger tumor inhibition efficacy. It significantly addresses the inherent limitations of chemodynamic therapy and radiotherapy and underscores the feasibility and importance of using existing clinical weapons, such as radiotherapy, as auxiliary strategies to overcome certain flaws of emerging antitumor therapeutics like chemodynamic therapy.
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Materials
·
2023
·Vol. 16
·期 21
·7007
·
IF 3.4
Yuzhe Wang,Yueqi Zhong,Jiangzhi Zi,Zichao Lian
Conventional single-component quantum dots (QDs) suffer from low recombination rates of photogenerated electrons and holes, which hinders their ability to meet the requirements for LED and laser applications. Therefore, it is urgent to design multicomponent heterojunction nanocrystals with these properties. Herein, we used CdSe quantum dot nanocrystals as a typical model, which were synthesized by means of a colloidal chemistry method at high temperatures. Then, CdS with a wide band gap was used to encapsulate the CdSe QDs, forming a CdSe@CdS core@shell heterojunction. Finally, the CdSe@CdS core@shell was modified through the growth of the ZnS shell to obtain CdSe@CdS@ZnS heterojunction nanocrystal hybrids. The morphologies, phases, structures and performance characteristics of CdSe@CdS@ZnS were evaluated using various analytical techniques, including transmission electron microscopy, X-ray diffraction, UV-vis absorption spectroscopy, fluorescence spectroscopy and time-resolved transient photoluminescence spectroscopy. The results show that the energy band structure is transformed from type II to type I after the ZnS growth. The photoluminescence lifetime increases from 41.4 ns to 88.8 ns and the photoluminescence quantum efficiency reaches 17.05% compared with that of pristine CdSe QDs. This paper provides a fundamental study and a new route for studying light-emitting devices and biological imaging based on multicomponent QDs.
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ChemElectroChem
·
2023
·
IF 4
Hailong Wei,Fangwei Gu,Yongsheng Wang,Jinyuan Hao,Wei Zhu,Zhongbin Zhuang
Graphical This work reports the synthesis of pure phase Ni 2 P nanowires for efficient hydrogen evolution reaction via the solution-based phosphidation method, demonstrating the effect of phosphorus ligand. Developing facile and low-cost synthetic methods of high-active platinum group metal-free electrocatalysts is essential for green hydrogen production primarily based on water electrolysis. We adopted a facile solution-based synthetic approach to prepare nickel phosphide nanoparticles (NP) and systematically studied the role of phosphorus ligands in the synthesis. Pure-phase Ni 2 P NPs were obtained by selecting the proper phosphorus ligands, which tuned the structures of the product. The Ni 2 P nanowire, prepared using triphenyl phosphite, exhibited the best activity and stability in acidic, neutral, and alkaline media for hydrogen evolution reaction (HER), indicating the advantages of the nanowire structure to the performance. In the acidic medium, it only required overpotential values of 100 and 167 mV to achieve the HER current densities of 10 and 100 mA cm −2 , respectively. Furthermore, the overpotential increased only by 26 mV during the 50-hour stability test, indicating potential for device application. It was also demonstrated that the on-site generation of insoluble nickel salts (e. g., hydroxides, phosphates, etc.) on the surface resulted in lower activity and stability in neutral and alkaline media than in acid.
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Regenerative Biomaterials
·
2023
·
IF 6.7
Zhong Jun,Zheng Xiang,Wen Yuan,Li Yuewei,Zhang Jianting,Kankala Ranjith Kumar,Wang Shibin,Chen Aizheng
The inadequate quantity of hydrogen peroxide (H2O2) in cancer cells promptly results in the constrained success of chemodynamic therapy (CDT). Significant efforts made throughout the years, nevertheless, researchers are still facing the great challenge of designing a CDT agent and securing H2O2 supply within the tumor cell. In this study, taking advantage of H2O2 level maintenance mechanism in cancer cells, a nanozyme-based bimetallic metal-organic frameworks (MOFs) tandem reactor is fabricated to elevate intracellular H2O2 levels, thereby enhancing CDT. In addition, under near-infrared excitation, the upconversion nanoparticles (UCNPs) loaded into the MOFs can perform photocatalysis and generate hydrogen, which increases cellular susceptibility to radicals induced from H2O2, inhibits cancer cell energy, causes DNA damages and induces tumor cell apoptosis, thus improving CDT therapeutic efficacy synergistically. The proposed nanozyme-based bimetallic MOFs-mediated CDT and UCNPs-mediated hydrogen therapy act as combined therapy with high efficacy and low toxicity.
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