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1.
Inorg Chem ; 63(31): 14755-14760, 2024 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-39042421

RESUMO

The efficient single-step purification of ethylene from ternary C2 mixtures containing ethane and acetylene is challenging and demanding. Herein, we introduce a novel cerium-based metal-organic framework (MOF) of Ce-NTB-rtk synthesized via a ligand-conformer strategy. The Ce-NTB-rtk features a rare tetranuclear cerium cluster and 2D kgd layers pillared by a 3D rtl framework concomitant with an extraordinary (3,3,12)-c network. The compound encompasses microporous cavities replete with a nonpolar microenvironment. Gas sorption and breakthrough experiments demonstrate its superior affinity for C2H6 and C2H2 over C2H4, enabling effective single-step ethylene purification. Computational simulations reveal that preferential adsorptions are facilitated by different interaction strengths of C-H···O hydrogen bonds. The performance of Ce-NTB-rtk in separation selectivity and regeneration capacity makes it a promising candidate for sustainable and cost-effective ethylene purification, showcasing the potential of MOFs in advanced gas separation applications.

2.
Inorg Chem ; 62(44): 18014-18019, 2023 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-37862124

RESUMO

Due to their intrinsic structural features, the design and synthesis of a new type of zeolite-like metal-organic frameworks (ZMOFs) is highly desirable but challenging. Herein, solvothermal reactions between an angular dicarboxylate linker and rare-earth (RE) ions afforded two RE-MOFs, namely, Tb-ZMOF-2 and Tb-ZMOF-3, respectively. Structural analyses reveal that Tb-ZMOF-2 encompasses a novel [446482] cage, while Tb-ZMOF-3 contains nonanuclear (i.e., D6R) and hexanuclear (i.e., D4R) RE clusters simultaneously, subsequently resulting in two new zeolitic topologies. Thanks to its high surface area and pore volume, Tb-ZMOF-2 demonstrates considerably high gravimetric and volumetric methane storage working capacities.

3.
Phys Chem Chem Phys ; 18(7): 5614-21, 2016 Feb 21.
Artigo em Inglês | MEDLINE | ID: mdl-26862710

RESUMO

Direct fabrication of semiconductor light emitting devices on metal foils is beneficial, because it brings flexibility and good heat sink in the devices. In this work, we have grown ZnO on the commercially available stainless steel foils by metal-organic chemical vapor deposition for the first time. With the increase of growth temperature, the morphology changes from a thin film structure to closely stacked columns, and eventually to nanorods. The change in the migration ability of adatoms due to the increase of growth temperature plays an important role in the evolution of morphology. The samples with nanorod morphology exhibit relatively better crystallinity and optical quality. A PEDOT: PSS/PMMA/ZnO device was fabricated based on the grown ZnO nanorods. The metal-insulator-semiconductor type device shows an uncommon symmetric I-V curve. Under reverse bias, the device emits fairly pure UV light, which comes from the near band edge emission of ZnO. The working mechanism of the devices has been discussed, and a model mainly based on the Poole-Frenkel effect is proposed to describe the charge transportation of the devices.

4.
Phys Chem Chem Phys ; 17(21): 13813-20, 2015 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-25803480

RESUMO

Vertically aligned ZnO/MgO coaxial nanowire (NW) arrays were prepared on sapphire substrates by metal-organic chemical vapor deposition combined with a sputtering system. We present a comparative investigation of the morphological and optical properties of the produced heterostructures with different MgO layer thicknesses. Photoluminescence measurements showed that the optical performances of ZnO/MgO coaxial NWs were strongly dependent on the MgO layer thickness. The intensity of deep-level emission (DLE) decreased monotonously with the increase of MgO thickness, while the enhancement of ultraviolet (UV) emission showed a critical thickness of 15 nm, achieving a maximum intensity ratio (∼226) of IUV/IDLE at the same time. The significantly improved exciton emission efficiency of the coaxial NW structures allows us to study the surface passivation effect, photogenerated carrier confinement and transfer in terms of energy band theory. More importantly, we achieved an ultralow threshold (4.5 mA, 0.58 A cm(-2)) electrically driven UV lasing action based on the ZnO/MgO NW structures by constructing an Au/MgO/ZnO metal/insulator/semiconductor diode, and the continuous-current-driven diode shows a good temperature tolerance. The results obtained on the unique optical properties of ZnO/MgO coaxial NWs shed light on the design and development of ZnO-based UV laser diodes assembled with nanoscale building blocks.

5.
Guang Pu Xue Yu Guang Pu Fen Xi ; 28(8): 1745-8, 2008 Aug.
Artigo em Zh | MEDLINE | ID: mdl-18975794

RESUMO

In the present paper, the authors study the photolumimescence spectra of the novel 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine casting film and vacuum-deposited film. Photolumimescence spectras of casting film on the quartz substrate were measured at 10, 77, 177 and 300 K, and the photolumimescence spectra of vacuum-deposited film with a thickness of about 200 nm on the silicon substrate was studied at room temperature (300 K). For 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine, the casting films all show fluorescence peaks at 942, 937, 942 and 942 nm and phosphorescence peaks at 1114, 1057, 1114 and 1114 nm in the photolumimescence spectra at 10, 77, 177 and 300 K, respectively. In the cases of 2,3-tetra-(2-isopropyl-5-methyl -benzoyl) hydrogen phthalocyanine, the peaks of excimers, which are related with the resistance ability of molecular aggregation, were found around 1673 nm as observed from photolumimescence spectra of the novel phthalocyanine casting films at 177 and 300 K. And the peak of excimers at 300 K is stronger than at 177 K also as can be seen from photolumimescence spectra of its casting films. With the increase in the temperature, the fluorescence peak was weakened and the peaks of excimers became stronger from the photoluminescence spectra of 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine casting films at 10, 77, 177 and 300 K. At the same time, the authors discussed the reason for coming into being 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine excimers as can be concluded from the structure of 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine molecules through the parameters of Chem 3D Ultra 9.0 MM2 calculation and simulated diagram of C4h isomer of 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine. The peaks of casting film and vacuum-deposited film of 2,3-tetra-(2-isopropyl-5-methyl -benzoyl) hydrogen phthalocyanine presented different maximum emission wavelength and full width at half maximum. The peak of 2,3-tetra-(2-isopropyl-5-methyl-benzoyl) hydrogen phthalocyanine vacuum-deposited films displays the maximum emission wavelengths around 1140 nm, while the maximum emission wavelengths of casting films show obvious differences compared with the vacuum-deposited films. The usual full width at half maximum is approximately 300 nm for casting film, which is in contrasts with that the full width at half maximum is about 100 nm for the vacuum-deposited film as can be seen from photolumimescence spectra of 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine casting film and photolumimescence spectra of 2,3-tetra-(2-isopropyl-5-methylbenzoyl) hydrogen phthalocyanine vacuum-deposited film.

6.
Nanoscale ; 10(43): 20131-20139, 2018 Nov 08.
Artigo em Inglês | MEDLINE | ID: mdl-30376029

RESUMO

Recently, inorganic halide perovskite (CsPbX3, X = Cl, Br, I) quantum dots (QDs) have attracted tremendous research interests because of their great potential for application in the fields of low-cost light sources and displays. However, the unsatisfactory structural and chemical stabilities of such materials are the main obstacles hindering reliable device operation significantly. In this study, we successfully prepared CsPbBr3/silica QD composites through a simple sol-gel reaction by using tetramethoxysilane as a single molecule precursor. The as-prepared CsPbBr3/silica QD composites demonstrated substantially improved stability against heat, light, and environmental oxygen/moisture. Besides, a relatively narrower photoluminescence linewidth and higher quantum yield were achieved compared with that of fresh CsPbBr3 QDs. Furthermore, the CsPbBr3 QDs/silica composites were applied as color-converting layer curing on blue light-emitting diodes (LEDs) for white LED applications. Finally, a high power efficiency of 63.5 lm W-1 was obtained and the light emission could be efficiently sustained over 13 h without any decay in the continuous current mode, demonstrating remarkable operation stability than that reported previously. It can be anticipated that the excellent properties and facile processing technique used here will make perovskite QDs/silica composites attractive for applications in optoelectronics and industrial fields.

7.
Nanoscale ; 8(19): 9997-10003, 2016 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-27142941

RESUMO

Semi-transparent all-oxide light-emitting diodes based on ZnO/NiO-core/shell nanowire structures were prepared on double-polished c-Al2O3 substrates. The entire heterojunction diode showed an average transparency of ∼65% in the ultraviolet and visible regions. Under forward bias, the diode displayed an intense ultraviolet emission at ∼382 nm, and its electroluminescence performance was remarkable in terms of a low emission onset, acceptable operating stability, and the ability to optically excite emissive semiconductor nanoparticle chromophores.

8.
Nanoscale ; 8(19): 10035-42, 2016 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-27140056

RESUMO

Recently, perovskite-based light-emitting diodes based on organometal halide emitters have attracted much attention because of their excellent properties of high color purity, tunable emission wavelength and a low-temperature processing technique. As is well-known, organic light-emitting diodes have shown powerful capabilities in this field; however, the fabrication of these devices typically relies on high-temperature and high-vacuum processes, which increases the final cost of the product and renders them uneconomical for use in large-area displays. Organic/inorganic hybrid halide perovskites match with these material requirements, as it is possible to prepare such materials with high crystallinity through solution processing at low temperature. Herein, we demonstrated a high-brightness green light-emitting diode based on PEDOT: PSS/CH3NH3PbBr3/ZnO sandwich structures by a spin-coating method combined with a sputtering system. Under forward bias, a dominant emission peak at ∼530 nm with a low full width of half-maximum (FWHM) of 30 nm can be achieved at room temperature. Owing to the high surface coverage of the CH3NH3PbBr3 layer and a device design based on carrier injection and a confinement configuration, the proposed diode exhibits good electroluminescence performance, with an external quantum efficiency of 0.0645%. More importantly, we investigated the working stability of the studied diode under continuous operation to verify the sensitivity of the electroluminescence performance to ambient atmosphere and to assess the suitability of the diode for practical applications. Moreover, the underlying reasons for the undesirable emission decay are tentatively discussed. This demonstration of an effective green electroluminescence based on CH3NH3PbBr3 provides valuable information for the design and development of perovskites as efficient emitters, thus facilitating their use in existing applications and suggesting new potential applications.

9.
Nanoscale ; 5(11): 5080-5, 2013 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-23640662

RESUMO

Electrically pumped lasing action has been realized in ZnO from an n-MgZnO/i-ZnO/SiO2/p-Si asymmetric double heterostructure, an ultralow threshold of 3.9 mA was obtained. The mechanism of the laser is associated with the in-plane random resonator cavities formed in the ZnO films and the elaborate hollow-shaped SiO2 cladding pattern, which prevent the lateral diffusion of injection current and ultimately lower the threshold current of the laser diode. In addition, a waveguide mechanism due to different refractive indices of three epilayers enhances the guided optical field on the ZnO side, resulting in an improved light extraction efficiency.

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