Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 37
·12581-12589
·
IF 7.393
Yixuan Liu,Lulu Zhang,Xuemi Long,PanPan Jiang,Chong Geng,Shu Xu
Perovskite nanocrystals (PNCs) are promising luminescent materials but suffer severe stability issues due to their ionic surface nature. SiO2 encapsulation is widely adopted for stabilizing PNCs in LED lighting and display applications. However, PNCs commonly lose ligands during the SiO2 encapsulation process, leading to fluorescence quenching and agglomeration. Here, CsPbBr3 PNCs with lead-carboxylate capping motif, which shows extraordinary ethanol and moisture resistance, were developed to facilitate fast and controlled growth of PNC–SiO2 nanocrystals using ethanol to accelerate the hydrolysis of tetramethoxysilane. Surface analysis revealed the preservation of the original carboxylate ligands after the reaction. Carboxylate and SiO2 form uniform dual-encapsulation that provides PNCs with superior air and water resistance, excellent photoluminescence maintenance, and high miscibility in silicone resin. Finally, saturated green LED and white-light LED with a wide color gamut were fabricated through on-chip packaging of the PNC–SiO2 on the blue LED chip. LEDs retained >85% of their light intensity after continuous illumination for 1000 h, demonstrating the high potential of the encapsulation method and the materials in light-emitting applications.
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MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Ziqi Nie,Lu Huang,Cewei Ren,Xinlin Xiong,Wenqing Zhu,Weiguang Yang,Linjun Wang
The facile approach combined the halide mixture of chloride and bromide anions with the exchange of short-chain ligand Phenethylamine (PEA) was used to prepare hybrid perovskite PEA-MAPbBr 3-x Cl x quantum dots (PEA-QDs-Cl), which realized blue emissive quantum dots light-emitting diode (QLED) with wider gamut of Commission Internationale de l’Eclairage (CIE) coordinates (Δx = −0.04, Δy = 0.03) than National Television Systems Committee (NTSC) TV color standard. Compared to pristine MAPbBr 3 quantum dots (pristine-QDs) prepared by conventional long-chain ligands, the size of PEA-QDs-Cl was manipulated from 9 nm to 3 nm characterized by HRTEM, emissive spectra were blue shifted from 528 nm to 469 nm measured by photoluminescence (PL). Meanwhile, time-resolved PL (TRPL) decay lifetimes of perovskite quantum dots doped with chloride anions (QDs-Cl) were improved from 10.3 ns to 13.9 ns, because short-chain ligands were introduced to passivate defects on the surface of QDs-Cl. Furthermore, XPS results showed that the chloride content was decreased from 34.7% to 33.7% through chloride vacancies on the surface of QDs-Cl were passivated by PEA.
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Nanoscale
·
2021
·Vol. 13
·期 39
·16487-16498
·
IF 7.79
Jingwen Wang,Shoufu Cao,Likun Yang,Yan Zhang,Kun Xing,Xiaoqing Lu,Jun Xu
The incorporation of catalytic components is a promising strategy to promote redox reaction kinetics and suppress polysulfide shuttling for high-performance lithium–sulfur batteries (LSBs). In this work, metastable marcasite NiSe2 nanodendrites grown on carbon fiber clothes (m-NiSe2/CFC) were synthesized to improve chemical adsorption and electrocatalytic activity towards lithium polysulfides. The multifunctional m-NiSe2/CFC film was utilized as both the interlayer and the three-dimensional (3D) current collector in LSBs. In comparison with the stable pyrite NiSe2 nanodendrite–covered CFC (p-NiSe2/CFC) counterpart, the m-NiSe2/CFC film exhibits even stronger chemisorption, higher catalytic activity and faster reaction kinetics, thereby resulting in significantly improved lithium storage performance. The Al@S/rGO@m-NiSe2/CFC cell has a high reversible capacity of 1646 mA h g−1 at 0.2C, a high QL/QH ratio of 3.00 at 0.2C, a high rate capability of 900 mA h g−1 at 4C, and an outstanding cyclic stability exhibiting a low capacity decay of 0.028% per cycle for 600 cycles at 4C. Moreover, a symmetrically sandwiched cathode of m-NiSe2/CFC@S/rGO@m-NiSe2/CFC was designed for high sulfur loading LSBs (4.5 mg cm−2) with superior electrochemical performance of 3.73 mA h cm−2 after 100 cycles at 1C rate. Our work opens up a new opportunity to enhance the electrochemical performance of LSBs by phase engineering of NiSe2 catalysts in sandwiched structural cathodes.
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Crystals
·
2021
·Vol. 11
·期 9
·1132
·
IF 2.589
Lianxing Liao,Kunhua Quan,Xiangshi Bin,Ruosheng Zeng,Tao Lin
Bandgap tunability through ion substitution is a key feature of lead halide perovskite nanocrystals (LHP-NCs). However, the low stability and low luminescent performance of CsPbCl3hinder their full-color applications. In this work, quantum confinement effect (QCE) was utilized to control the bandgap of CsPbBr3NCs instead of using unstable CsPbCl3, which possess much higher emission efficiency in blue spectra region. Studies of microstructures, optical spectra and carrier dynamics revealed that tuning the reaction temperature was an effective way of controlling the NC sizes as well as QCE. Furthermore, the obtained CsPbBr3NCs were encapsulated in a PDMS matrix while maintaining their size distribution and quantum-confined optoelectronic properties. The encapsulated samples showed long-term air and water stability. These results provide valuable guidance for both applications of LHP-NCs and principal investigation related to the carrier transition in LHP-NCs.Keywords:lead halide perovskites;nanocrystals;quantum confinement effect;carrier lifetimes
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Wei Wei,Wen Chen,Xizhu Zhao,Zifan Yang,Yueli Liu
All-inorganic CsPbI 3 quantum dots perovskite solar cells (QDPSCs) have wide potential application due to their excellent photoelectric properties with high environmental stability. However, the poor interface contact between the light absorption layer and hole transport layer (HTL) results in the serious carrier recombination and the large open-circuit voltage ( V OC ) loss. Herein, we introduce the insulating PMMA (poly(methyl methacrylate)) buffer layer into CsPbI 3 quantum dots (QDs)/Cu 12 Sb 4 S 13 QDs HTL interface in all-inorganic QDPSCs with the structure of FTO/c-TiO 2 /m-TiO 2 /CsPbI 3 QDs/Cu 12 Sb 4 S 13 QDs/Au. The interface carrier recombination is obviously suppressed and the significant V OC improvement from 1.04 V to 1.14 V is obtained with the incorporated PMMA buffer layer. The devices with PMMA buffer layer show the enhanced power conversion efficiency (PCE) of 10.99%, and the improvement of 9.71% is achieved compared to that of the control devices (10.02%). The stability is significantly enhanced due to the intrinsic hydrophobic characteristic of PMMA, and the devices retain 62.69% of their initial PCE after stored in air condition for 15 days, which is greatly improved compared with the control device without PMMA.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-15
·
IF 14.919
Qin Xing,Wu Chu,Niu Dechao,Qin Limei,Wang Xia,Wang Qigang,Li Yongsheng
Peroxisome, a special cytoplasmic organelle, possesses one or more kinds of oxidases for hydrogen peroxide (H 2 O 2 ) production and catalase for H 2 O 2 degradation, which serves as an intracellular H 2 O 2 regulator to degrade toxic peroxides to water. Inspired by this biochemical pathway, we demonstrate the reactive oxygen species (ROS) induced tumor therapy by integrating lactate oxidase (LOx) and catalase (CAT) into Fe 3 O 4 nanoparticle/indocyanine green (ICG) co-loaded hybrid nanogels (designated as FIGs-LC). Based on the O 2 redistribution and H 2 O 2 activation by cascading LOx and CAT catalytic metabolic regulation, hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) production can be modulated for glutathione (GSH)-activated chemodynamic therapy (CDT) and NIR-triggered photodynamic therapy (PDT), by manipulating the ratio of LOx and CAT to catalyze endogenous lactate to produce H 2 O 2 and further cascade decomposing H 2 O 2 into O 2 . The regulation reactions of FIGs-LC significantly elevate the intracellular ROS level and cause fatal damage to cancer cells inducing the effective inhibition of tumor growth. Such enzyme complex loaded hybrid nanogel present potential for biomedical ROS regulation, especially for the tumors with different redox state, size, and subcutaneous depth.
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ACS Applied Nano Materials
·
2021
·
IF 5.097
Longhui Lin,Linghang Qiu,Feiming Li,Chaoyu You,Yimeng Zhu,Qiuhong Yao,Yibo Zeng,Yiru Wang,Jianfeng Li,Xi Chen
Lead halide perovskite nanocrystals (PNCs) have led to a growing number of studies focusing on electrochemiluminescence (ECL) due to their excellent optical characteristics, making them promising candidates as ECL emitters for high performance. However, because of their ionic salt nature, PNCs even protected by ligands will be dissolved rapidly in polar solvents as electrolytes. Meanwhile, the contact of interfaces among PNCs, the electrode, and the electrolyte (three-phase interface) is required to guarantee effective carrier transfer and sufficient excited-state species, leading to stable ECL signals and ultrasensitivity. Herein, a fast and convenient preparation method is first proposed for fabricating abundant three-phase interfaces by anchoring CsPbBr3 PNCs to graphene oxide (GO) functionalized with amino groups, which stabilizes the PNC structure and provides carrier transfer pathways. Consequently, the GO-assisted CsPbBr3 PNC three-phase interfaces exhibit brilliant ECL intensity in acetonitrile containing 10 mM tripropylamine (TPrA) and remain stable after more than 1 h continuous cyclic potential scans with an RSD of 6%. Finally, the method has been applied to detect cupric oleate with the detection limit down to the attomolar (10–18 M) level. This work further validates the vital role of interface state in PNCs’ ECL response and has potential in ultrasensitive analysis.
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FARADAY DISCUSSIONS
·
2021
·Vol. 233
·232-243
·
IF 4.008
Pengfei Yao,Jing Cao,Mingbo Ruan,Ping Song,Xue Gong,Ce Han,Weilin Xu
Achieving a highly efficient and durable methanol electro-oxidation catalyst in acid media is critical for the practical utilization of direct methanol fuel cells (DMFCs) at the commercial scale. Herein, we report a facile and effective one-pot strategy for the synthesis of carbon-supported PtCu alloy nanoparticles (PtCu NPs) with a Pt-rich surface, small particle size and uniform dispersion. The as-prepared PtCu NPs with the optimal alloy composition (Pt2Cu) exhibit a significantly improved electrochemical methanol oxidation reaction performance in terms of a high activity, superior CO tolerance and remarkable durability, in contrast to those of commercial Pt/C catalysts in acid media. Particularly, the Pt2Cu/C catalyst exerts a 4.5 times enhancement in the mass activity and a larger If/Ib value compared to those of commercial Pt/C (Pt/Ccomm). The enhanced catalytic activities can be ascribed to the high utilization of Pt and the high index facets of the surface. Also, the addition of Cu downshifts the d-band center of Pt and improves the CO tolerance during the methanol oxidation reaction process. This work provides an efficient strategy for designing desired Pt-based alloys for various catalytic reactions.
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高影响因子
FUEL
·
2021
·
IF 6.609
Jianwu Zou,Yankun Du,Rongjia Fang,Xiaoshuang Duan,Yangjia Liu,Jia Mao,Lingyun Yu,Xiang Xu,Zheng Zeng,Liqing Li
The PtCo 3 nanoparticles (NPs of 2–5 nm) were synthesized by the organic phase reduction method and the PtCo 3 -C samples were obtained by physically loading the bimetallic NPs on the carbon black. The catalytic activity and stability of PtCo 3 -C for toluene oxidation under different reaction conditions were studied. The PtCo 3 -C can completely oxidize and decompose 1000 ppm toluene at 238 ℃ for at least 120 h, which has excellent low-temperature catalytic activity and thermal stability. In addition, PtCo 3 -C displays a great water and CO 2 resistance when 3.5 to 20 vol% water vapor (at least 110 h) or 3.5 to 10 vol% CO 2 (at least 60 h) is introduced into the reaction gas at 238 ℃. Moreover, the adsorption energy of toluene (−73.68 kJ mol −1 ) is much higher than that of water (−24.5 kJ mol −1 ) and CO 2 (−37.56 kJ mol −1 ), which were calculated by the density functional theory (DFT). Furthermore, catalytic mechanism of the oxidation of toluene over the PtCo 3 -C catalyst was also proposed. This study presents a good catalyst candidate obtaining high catalytic activity and stability with great water and CO 2 resistance for the removal of toluene.
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NANO LETTERS
·
2021
·
IF 11.189
Chen Li,Shuai Zhou,Jing Nie,Jie Huang,Xiaoping Ouyang,Qiang Xu
Because of the extraordinary properties including high atomic numbers and large μτ products, metal halide perovskites have been widely employed and used for radiation detecting. Cs4PbI6 material has a high X-ray attenuation coefficient and excellent electrical properties that have a good potential in X-ray detection applications. Here, we have designed a flexible polymer-encapsulated Au/Cs4PbI6/Au X-ray detector with outstanding sensitivity of 256.20 μC Gy–1 cm–2 irradiated by 30 keV X-ray at 10 V bias, long-time stability, and durable flexibility without obvious degradation after bending for 600 cycles. These features demonstrate that this polymer-encapsulated durable flexible and sensitive X-ray detector could open a new possibility for next-generation radiation applications in dosimeter, imaging technologies.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2021
·
IF 3.171
Yingzhen Zhang,Yonggang Lei,Tianxue Zhu,Zengxing Li,Shen Xu,Jianying Huang,Xiao Li,Weilong Cai,Yuekun Lai,Xiaojun Bao
Exploring efficient and stable photoanode materials is a necessary link to realize the practical application of solar-driven photoelectrochemical (PEC) water splitting. Hence, we prepared rutile TiO 2 nanorods , with a width of 50 nm, which was growth in situ on carbon cloth (TiO 2 @CC) by hydrothermal reaction. And then, Ag nanoparticles (NPs) and biomass N,S-C NPs were chosen for the additional modification of the fabricated TiO 2 nanorods to produce broccoli-like Ag-N,S-C/TiO 2 @CC nanocomposites . According to the result of ultraviolet–visible diffuse reflectance spectroscopy (UV–vis) and PEC water splitting performance tests, Ag-N,S-C/TiO 2 @CC broadens the absorption region of TiO 2 @CC from the ultraviolet region to the visible region. Under AM 1.5G solar light irradiation, the photocurrent density of Ag-N,S-C/TiO 2 @CC is 89.8 μA·cm −2 , which is 11.8 times higher than TiO 2 @CC. Under visible light irradiation, the photocurrent density of Ag-N,S-C/TiO 2 @CC reaches to 12.6 μA·cm −2 , which is 21.0 times higher than TiO 2 @CC. Moreover, Ag-N,S-C/TiO 2 @CC shows a photocurrent responses in full pH range. It can be found that Ag NPs and N, S-C NPs play key roles in broaden the absorption range of TiO 2 nanorods to the visible light region and, promote the occurrence of PEC water oxidation reaction due to the surface plasmon resonance effect of Ag NPs and the synergistic effect of N,S-C NPs. The mechanism demonstrated that Ag-N,S-C/TiO 2 @CC can separate the photogenerated electron-hole pairs effectively and transfer the photogenerated electrons to the photocathode (Pt plate) in time. This research provides a new strategy for exploration surface plasma metal coupled biomass carbon materials in the field of PEC water splitting.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 46
·17281-17289
·
IF 4.39
Dayu Huang,Yue Liu,Qiuyun Ouyang,Hongzhou Lian,Jun Lin
The stability of perovskite quantum dots (PQDs) plays a vital role in practical devices. Besides silica coating, embedding PQDs in zeolites is another strategy to improve their stability significantly. Although the zeolite rigid framework has been reported to protect PQDs, there are few reports on the in situ synthesis of PQDs in zeolites. In this work, cubic phase CsPbX3 (X = Br, I) nanocrystals were successfully prepared by the ion exchange method combined with a non-polar organic trigger. Dropping a certain amount of ZnM2 (M = Br, I) solution into the intermediate product Cs4PbCl6 nanocrystals resulted in the formation of the final CsPbX3 nanocrystals. The ZnM2 solutions were prepared in non-polar solvents (hexane, octane, or chloroform). The highest photoluminescence quantum yield (PLQY) of the synthesized CsPbX3@zeolite composites can reach 83%, with a lifetime of 1.37 μs. The stability of the CsPbX3@zeolite composites thin film against damage from air and light is significantly improved. We fabricated white light-emitting diodes (WLEDs) using CsPbBr3@zeolite as the green light source and CsPbI3@zeolite as the red light source to further emphasize the practical application effect of the CsPbX3@zeolite composites. This work not only provides a new method for the synthesis of CsPbX3 nanocrystals but also involves the in situ synthesis of high stability CsPbX3@zeolite composites within the zeolite.
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