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  • 1.
    Huang, Shiliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Open-Framework Germanates and Nickel Germanates: Synthesis and Characterization2012Doktoravhandling, med artikler (Annet vitenskapelig)
    Abstract [en]

    Microporous materials have a wide range of important applications in separation, gas adsorption, ion-exchange and catalysis. Open-framework germanates are a family of microporous compounds and are of particular interest. This thesis focuses on the synthesis and characterization of new open-framework germanates as well as introducing the transition-metal nickel into germanate structures.

    One new microporous germanosilicate, SU-78 and four new open-framework germanates, SU-74, SU-75, SU-69 and SU-76 have been obtained by using organic molecules as structure directing agents (SDAs). The incorporation of nickel and organic SDAs in the synthesis resulted in five novel nickel germanates, SUT-1, SUT-2, SUT-3, SUT-4 and SUT-5, in which nickel complexes act either as framework-forming components or as structure directing agents.

    The general synthesis route is described and the variables that affect the synthesis products are summarized. Different techniques applied on the characterization of chemical and physical properties of the products are also introduced.

  • 2.
    Huang, Shiliang
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Christensen, Kirsten
    Peskov, Maxim V.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Yang, Sihai
    Li, Kuo
    Zou, Xiaodong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Two Open-Framework Germanates with Nickel Complexes Incorporated into the Framework2011Inngår i: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 50, nr 20, s. 9921-9923Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Two open-framework germanates, SUT-1 and SUT-2, have been synthesized under hydrothermal conditions using ethylenecliamine (en, H(2)NCH(2)CH(2)NH(2)) as templates and Ni(NO(3))(2)center dot 6H(2)O as the transition-metal source. Their frameworks are built with Gel() clusters and [Ni(en)(2)](2+) complexes. In both structures, Gel clusters form square nets in the a-c plane, while the [Ni(en)2]2+ complexes bridge the square nets via Ni-O-Ge bonds to form 3D networks. They present the first examples to incorporate Ni(2+) complexes into the germanate frameworks. In SUT-2, additional linkages by Ge(2)O(7) clusters between the square nets generate a new type of topology.

  • 3.
    Huang, Shiliang
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Inge, A. Ken
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Yang, Sihai
    Christensen, Kirsten E.
    Zou, Xiaodong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    SU-75: a disordered Ge-10 germanate with pcu topology2012Inngår i: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 41, nr 40, s. 12358-12364Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    A disordered open-framework germanate, denoted as SU-75, was synthesized under hydrothermal conditions using diethylenetriamine (dien) or alternatively 1,4-diaminobutane (dab) as the structure directing agent (SDA). SU-75 crystallizes in a tetragonal space group I-42d(No. 122) with a= 18.145(3) Å and c= 41.701(9) Å. The three-dimensional (3D) framework is built from Ge10(O,OH)28(Ge10) clusters that are connected following the pcu ( primitive cubic) net topology. SU-75 has 10-, 11- and 12-ring channels along the a- and b-axes and channels with alternating 8-, 10-, 12-, 10-ring openings along the c-axis. The framework exhibits a serious disorder, resulted from two possible connectivities between the units of four Ge 10clusters (4Ge10 unit). The chemical formula of SU-75 is |(H2SDA)2(H2O)n|[Ge10O21(OH)2] (SDA = dien or dab,n= 5–6), determined by combining single crystalsynchrotron X-ray diffraction, thermogravimetric analysis (TGA) and CHN elemental analysis. A superoctahedron is introduced to simplify the description of the connectivity of the Ge10 clusters and to illustrate the disorder. This is also used to compare the structure of SU-75 with those of related Ge10 germanates.

  • 4.
    Huang, Shiliang
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Su, Jie
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Christensen, Kirsten
    Liang, Jie
    Zou, Xiaodong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Synthesis and characterization of two new nickel germanates: SUT-3 and SUT-4Manuskript (preprint) (Annet vitenskapelig)
  • 5.
    Inge, Andrew Kentaro
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Huang, Shiliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Chen, Hong
    Moraga, Francisca
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Zou, Xiaodong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    The Structure of a Complex Open-framework Germanate Obtained by Combining Powder Charge-Flipping and Simulated Annealing2012Inngår i: Crystal Growth & Design, ISSN 1528-7483, E-ISSN 1528-7505, Vol. 12, nr 10, s. 4853-4860Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    A novel open-framework germanate SU-74 containing intersecting 10- and 12-ring channels was prepared by hydrothermal synthesis using 2-methylpentamethylenediamine (MPMD) or 1-(2-aminoethyl)piperazine (AEP) as the organic structure directing agent (SDA). The framework structure of SU-74-MPMD was solved from X-ray powder diffraction (XRPD) data using powder charge-flipping (pCF). The guest species H2MPMD2+, NH4+ cations and water molecules were located in the voids using real-space simulated annealing. SU-74-MPMD contains 51 non-hydrogen atoms in its asymmetric unit and is one of the most complex framework structures solved by XRPD. The structure of SU-74-AEP was solved by single crystal synchrotron X-ray diffraction. SU-74-MPMD and SU-74-AEP have the same framework structure. The location of the NH4+ cations in both structures is similar, while the positions of the SDAs in the pores are different. SU-74 follows the fcu-11-P21/c net. The underlying topology of SU-74 is compared to those of other Ge10 structures containing additional GeO4 tetrahedra. The presence of additional tetrahedra can significantly affect the framework topology through the addition of edges between the Ge10 nodes.

  • 6. Yang, Tao
    et al.
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Yeon, Jeongho
    Halasyamani, Shiv
    Huang, Shiliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Hemberger, Joachim
    Greenblatt, Martha
    Cd1−xBix(Cd1+xIn1−x)VO6 (0 ≤ x ≤ 0.14): A New Polar Oxide with Second-Harmonic Generation2010Inngår i: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 22, nr 16, s. 4814-4820Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    The structure of the new polar oxide, Cd2InVO6, was determined by powder X-ray diffraction. Cd2InVO6 crystallizes in space group P31 with the unit cell parameters: a = 12.21896(4), c = 9.25675(4) Å. The Cd2+ and In3+ ions are statistically disordered in nine independent positions (M1−M9) with a certain level of site preference. M1−M3 form highly asymmetric oxygen-coordination polyhedra, which are similar to those formed by alkali or alkali-earth cations. M4−M9 are in distorted octahedral cavities. It is shown that M1−M3 are likely occupied mostly by Cd2+ while M4−M9 are extensively mixed by Cd2+ and In3+. The structure is best described as a framework of interconnected M4−M9 distorted octahedra with the M1−M3 polyhedra off-framework and the three independent VO4 tetrahedra filling the channels of the framework structure by corner-sharing with the MO6 octahedra. The polar framework is composed of M4O6M9O6 octahedra in a five-connected net with the topology nomination (33, 63, 94). The Bi3+-substituted compounds were also investigated with the rationale that the lone pair electrons of Bi3+ might enhance ferroelectricity. Single phase Cd1−xBix(Cd1+xIn1−x)VO6 forms limited solid solutions (0.02 ≤ x ≤ 0.14). Ferroelectricity was observed for neither the parent nor the Bi3+-substituted compounds, which suggest that the dipole moments are not switchable or too insignificant in magnitude. The powder second-harmonic generation measurements with 1064 nm radiation established that Cd1−xBix(Cd1+xIn1−x)VO6 are type-1 phase-matchable materials for x = 0, 0.14 with 70 and 90 times the efficiency of α-SiO2, respectively.

  • 7.
    Yu, Zheng-Bao
    et al.
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Han, Yu
    Zhao, Lan
    Huang, Shiliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Zheng, Qi-Yu
    Lin, Shuangzheng
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Córdova, Armando
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
    Zou, Xiaodong
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Sun, Junliang
    Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
    Intergrown New Zeolite Beta Polymorphs with Interconnected 12-Ring Channels Solved by Combining Electron Crystallography and Single-Crystal X-ray Diffraction2012Inngår i: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 24, nr 19, s. 3701-3706Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Two new polymorphs of zeolite beta, denoted as SU-78A and SU-78B, were synthesized by employing dicyclohexylammonium hydroxides as organic structuredirecting agents. The structure was solved by combining transmission electron microscopy and single-crystal X-ray diffraction. SU-78 is an intergrowth of SU-78A and SU-78B and contains interconnected 12-ring channels in three directions. The two polymorphs are built from the same building layer, similar to that for the zeolite beta family. The layer stacking in SU-78, however, is different from those in zeolite beta polymorph A, B, and C, showing new zeolite framework topologies. SU-78 is thermally stable up to 600°C.

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