| 1. |
- Chen, Hong, et al.
(författare)
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PKU-3 : An HCI-Inclusive Aluminoborate for Strecker Reaction Solved by Combining RED and PXRD
- 2015
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 137:22, s. 7047-7050
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Tidskriftsartikel (refereegranskat)abstract
- A novel microporous aluminoborate, denoted as PKU-3, was prepared by the boric acid flux method. The structure of PKU-3 was determined by combining the rotation electron diffraction and synchrotron powder X-ray diffraction data with well resolved ordered Cl- ions in the channel. Composition and crystal structure analysis showed that there are both proton and chlorine ions in the channels. Part of these protons and chlorine ions can be washed away by basic solutions to activate the open pores. The washed PKU-3 can be used as an efficient catalyst in the Strecker reaction with yields higher than 90%.
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| 2. |
- Chen, Yanping, et al.
(författare)
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PKU-20 : A new silicogermanate constructed from sti and asv layers
- 2016
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Ingår i: Microporous and Mesoporous Materials. - : Elsevier BV. - 1387-1811 .- 1873-3093. ; 224, s. 384-391
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Tidskriftsartikel (refereegranskat)abstract
- A new silicogermanate (PKU-20) was hydrothermally synthesized using triethylisopropylammonium cation as the structure directing agent in the presence of fluoride. Its structure was determined from a combination of synchrotron single crystal X-ray diffraction and powder X-ray diffraction data. PKU-20 crystallizes in the monoclinic space group C2/m, with the lattice parameters of a = 18.5901(6) angstrom, b = 13.9118 (4) angstrom, c = 22.2614(7) angstrom and beta = 100.1514 (12)degrees. The framework of PKU-20 is constructed from an alternate stacking of sti and asv layers. The sti layer is exactly the same as that in the STI framework, while the asv layer is a new layer sliced off from the ASV framework parallel to the (112) plane. The takeout scheme of the layer is discussed on the basis of a composite building unit D4R-/au-D4R. PKU-20 possesses a two-dimensional channel system, where the 10-ring channels parallel to the [010] direction are intercrossed by 12-ring pockets along the [101] direction.
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| 3. |
- Li, Jian, et al.
(författare)
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Discovery of Complex Metal Oxide Materials by Rapid Phase Identification and Structure Determination
- 2019
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Ingår i: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 141:12, s. 4990-4996
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Tidskriftsartikel (refereegranskat)abstract
- The discovery of new inorganic functional materials is of fundamental importance in synthetic and materials science. In the past, the discovering new materials relied on a slow and serendipitous trial-and-error process, especially in the well-studied oxide systems. Here, we presented a strategy to shorten the period of discovery of new complex metal oxide materials by rapid phase identification and structure determination with 3D electron diffraction (ED) techniques, which do not require pure samples or single crystal growth. With such strategy, three new complex metal oxide materials (BiTi0.855Fe1.145O4.93, BiTi4FeO11 and BiTi2FeO7) were discovered in the simple ternary Bi2O3-Fe2O3-TiO2 system. To our best knowledge, it is the first time to discover three new complex metal oxide materials with new structure types in a single study of ternary metal oxide system. The structures of new materials were refined by combining powder X-ray diffraction (PXRD) with powder neutron diffraction (PND). The most striking feature in this system is that BiTi0.855Fe1.145O4.93 presents edge-shared five-coordinated iron/titanium polyhedra. In addition, another new phase BiTi4GaO11, which is isostructural with BiTi4FeO11, can be obtained when replacing Fe in BiTi4FeO11 with Ga. The band structure investigation of BiTi0.855Fe1.145O4.93, BiTi4FeO11, BiTi2FeO7 and BiTi4GaO11 shown that they were semiconductors with band gaps of 1.65, 2.0, 1.9, and 2.8 eV, respectively. Although this study focused on rapid developing of new inorganic functional materials, this method for developing new materials is available to all fields in chemistry and material chemistry where the limiting factors are impurity, submicrometersized crystals, etc.
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| 4. |
- Lin, Junzhong, et al.
(författare)
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Hierarchical MFI zeolite synthesized via regulating the kinetic of dissolution-recrystallization and their catalytic properties
- 2018
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Ingår i: Catalysis communications. - : Elsevier BV. - 1566-7367 .- 1873-3905. ; 115, s. 82-86
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Tidskriftsartikel (refereegranskat)abstract
- Hierarchical MFI zeolites with open pores were synthesized by a temperature programmed dissolution-recrystallization post-treatment. By controlling the temperature of post-treatment using TPAOH, open macropores and mesopores were created by simply regulating the kinetics of dissolution and recrystallization. Benzyl alcohol self-etherification reaction, which only occurs in micropores, was tested on ZSM-5 to understand the effect of hierarchical pore system. The catalytic activity of hierarchical TS-1 was tested with cyclohexanone ammoximation. Hierarchical ZSM-5 and TS-1 zeolites with open pores showed higher catalytic activity compared with both hollow and conventional ones. The increased catalytic activities can be ascribed to the enhanced diffusion.
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| 5. |
- Lin, Jia, et al.
(författare)
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Pressure-induced semiconductor-to-metal phase transition of a charge-ordered indium halide perovskite
- 2019
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Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : Proceedings of the National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 116:47, s. 23404-23409
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Tidskriftsartikel (refereegranskat)abstract
- Phase transitions in halide perovskites triggered by external stimuli generate significantly different material properties, providing a great opportunity for broad applications. Here, we demonstrate an In-based, charge-ordered (In+/In3+) inorganic halide perovskite with the composition of Cs2In(I)In(III)Cl-6 in which a pressure-driven semiconductor-to-metal phase transition exists. The single crystals, synthesized via a solid-state reaction method, crystallize in a distorted perovskite structure with space group I4/m with a = 17.2604(12) angstrom, c = 11.0113(16) angstrom if both the strong reflections and superstructures are considered. The supercell was further confirmed by rotation electron diffraction measurement. The pressure-induced semiconductor-to-metal phase transition was demonstrated by high-pressure Raman and absorbance spectroscopies and was consistent with theoretical modeling. This type of charge-ordered inorganic halide perovskite with a pressure-induced semiconductor-to-metal phase transition may inspire a range of potential applications.
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| 6. |
- Meng, Qingpeng, et al.
(författare)
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Zeolite A synthesized from alkaline assisted pre-activated halloysite for efficient heavy metal removal in polluted river water and industrial wastewater
- 2017
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Ingår i: Journal of Environmental Sciences(China). - : Elsevier BV. - 1001-0742 .- 1878-7320. ; 56, s. 254-262
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Tidskriftsartikel (refereegranskat)abstract
- High quality zeolite A was synthesized through a hydrothermal process using alkaline-assisted pre-activated halloysite mineral as the alumina and silica source. The synthesis conditions employed in this study were finely tuned by varying the activating temperature, sodium hydroxide content, water content and Si/Al ratio. The obtained zeolite A showed excellent adsorption properties for both single metal cation solutions and mixed cation solutions when the concentrations of the mixed cations were comparable with those in polluted natural river water and industrial wastewater. High adsorptive capacities for Ag+ (123.05 mg/g) and Pb2+ (227.70 mg/g) were achieved using the synthesized zeolite A. This observation indicates that the zeolite A synthesized from alkaline-assisted pre-activated halloysite can be used as a low-cost and relatively effective adsorbent to purify heavy metal cation polluted natural river water and industrial wastewater.
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| 7. |
- Xu, Le, et al.
(författare)
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Crystallization of a Novel Germanosilicate ECNU-16 Provides Insights into the Space-Filling Effect on Zeolite Crystal Symmetry
- 2018
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Ingår i: Chemistry - A European Journal. - : Wiley. - 0947-6539 .- 1521-3765. ; 24:37, s. 9247-9253
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Tidskriftsartikel (refereegranskat)abstract
- Synthesis of new zeolites involving organic molecules relies heavily on the trial-and-error approach, because it is difficult to interpret the determining effects of organics on zeolite crystal symmetry. Here, the intrinsic relationships among the space-filling of organics, included volume of channels, and zeolite crystal symmetry, are systematically demonstrated by experimental and computational means. Under controlled conditions, the dimer and monomer organics of 1-ethyl-3-methylimidazolium selectively direct different, but related, germanosilicates, the ECNU-16 with a new topology and the existing IM-16 with the UOS topology, respectively. The comprehensive computational study reveals that the zeolite phase selectivity is determined by the unique space-filling behavior of the dimer and monomer organics, which is closely correlated to their rotation freedom, as well as the included volume of host zeolite channels. The elucidation of this crucial space-filling effect from the fundamental viewpoint will provide new guidelines for the rational design and synthesis of new zeolites in future.
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| 8. |
- Cao, Lingyun, et al.
(författare)
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Self-Supporting Metal–Organic Layers as Single-Site Solid Catalysts
- 2016
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Ingår i: Angewandte Chemie International Edition. - : Wiley. - 1433-7851 .- 1521-3773. ; 55:16, s. 4962-4966
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Tidskriftsartikel (refereegranskat)abstract
- Metal–organic layers (MOLs) represent an emerging class of tunable and functionalizable two-dimensional materials. In this work, the scalable solvothermal synthesis of self-supporting MOLs composed of [Hf6O4(OH)4(HCO2)6] secondary building units (SBUs) and benzene-1,3,5-tribenzoate (BTB) bridging ligands is reported. The MOL structures were directly imaged by TEM and AFM, and doped with 4′-(4-benzoate)-(2,2′,2′′-terpyridine)-5,5′′-dicarboxylate (TPY) before being coordinated with iron centers to afford highly active and reusable single-site solid catalysts for the hydrosilylation of terminal olefins. MOL-based heterogeneous catalysts are free from the diffusional constraints placed on all known porous solid catalysts, including metal–organic frameworks. This work uncovers an entirely new strategy for designing single-site solid catalysts and opens the door to a new class of two-dimensional coordination materials with molecular functionalities.
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| 9. |
- Dai, Ruihan, et al.
(författare)
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Electron crystallography reveals atomic structure of metal-organic nanoplate with Hf12(µ3-O)8(µ3-OH)8(µ2-OH)6 secondary building unit
- 2017
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Ingår i: Inorganic Chemistry. - : American Chemical Society (ACS). - 0020-1669 .- 1520-510X. ; 56:14, s. 8128-8134
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Tidskriftsartikel (refereegranskat)abstract
- Nanoscale metal–organic frameworks (nMOFs) have shown tremendous potential in cancer therapy and biomedical imaging. However, their small dimensions present a significant challenge in structure determination by single-crystal X-ray crystallography. We report here the structural determination of nMOFs by rotation electron diffraction (RED). Two isostructural Zr- and Hf-based nMOFs with linear biphenyldicarboxylate (BPDC) or bipyridinedicarboxylate (BPYDC) linkers are stable under intense electron beams to allow the collection of high-quality RED data, which reveal a MOF structure with M12(μ3-O)8(μ3-OH)8(μ2-OH)6 (M = Zr, Hf) secondary building units (SBUs). The nMOF structures differ significantly from their UiO bulk counterparts with M6(μ3-O)4(μ3-OH)4 SBUs and provide the foundation for clarifying the structures of a series of previously reported nMOFs with significant potential in cancer therapy and biological imaging. Our work clearly demonstrates the power of RED in determining nMOF structures and elucidating the formation mechanism of distinct nMOF morphologies.
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| 10. |
- Ding, Huimin, et al.
(författare)
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An AIEgen-based 3D covalent organic framework for white light-emitting diodes
- 2018
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 9
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Tidskriftsartikel (refereegranskat)abstract
- The design and synthesis of three-dimensional covalent organic frameworks (3D COFs) have still been considered as a big challenge. Here we report the design and synthesis of an AIEgen-based 3D COF (3D-TPE-COF), with a high surface area (1084 m(2)g(-1)). According to powder X-ray diffraction and continuous rotation electron diffraction analyses, 3D-TPE-COF is identified to adopt a seven-fold interpenetrated pts topology. Interestingly, 3D-TPE-COF emits yellow fluorescence upon excitation, with a photoluminescence quantum yield of 20%. Moreover, by simply coating 3D-TPE-COF onto a commercial blue light-emitting diode (LED), a prototype white LED (WLED) under continuously driving without degradation for 1200 h was demonstrated. The present work suggests the possibility of using COF materials for stable WLEDs, which will greatly inspire us to design and synthesize fluorescent 3D COFs and facilitate the development of COF-based WLEDs in future.
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