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3D Open-Framework Vanadoborate as a Highly Effective Heterogeneous Pre-catalyst for the Oxidation of Alkylbenzenes
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK), Avdelningen för oorganisk kemi och strukturkemi.
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för organisk kemi.
Stockholms universitet, Naturvetenskapliga fakulteten, Institutionen för material- och miljökemi (MMK).
Visa övriga samt affilieringar
2013 (Engelska)Ingår i: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 25, nr 24, s. 5031-5036Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Three three-dimensional (3D) open-framework vanadoborates, denoted as SUT-6-Zn, SUT-6-Mn, and SUT-6-Ni, were synthesized using diethylenetriamine as a template. SUT-6-Zn, SUT-6-Mn, and SUT-6-Ni are isostructural and built from (VO)(12)O-6 B18O36(OH)(6) clusters bridged by ZnO5, MnO6, and NiO6 polyhedra, respectively, to form the 3D frameworks. SUT-6 is the first vanadoborate with a 3D framework. The framework follows a semiregular hxg net topology with a 2-fold interpenetrated diamond-like channel system. The amount of template used in the synthesis played an important role in the dimensionality of the resulting vanadoborate structures. A small amount of diethylenetriamine led to the formation of this first 3D vanadoborate framework, while an increased amount of diethylenetriamine resulted in vanadoborates with zero-dimensional (0D) and one-dimensional (1D) structures. SUT-6-Zn was proved to be an efficient heterogeneous precatalyst for the oxidation of alkylbenzenes.

Ort, förlag, år, upplaga, sidor
2013. Vol. 25, nr 24, s. 5031-5036
Nyckelord [en]
vanadoborates, open-framework materials, hxg topology, heterogeneous catalysis, oxidation
Nationell ämneskategori
Fysikalisk kemi Materialkemi
Identifikatorer
URN: urn:nbn:se:su:diva-100387DOI: 10.1021/cm401400mISI: 000329137800024OAI: oai:DiVA.org:su-100387DiVA, id: diva2:693404
Forskningsfinansiär
VetenskapsrådetVinnova
Anmärkning

AuthorCount:8;

Funding agencies:

Swedish Research Council (VR)   Swedish Governmental Agency for Innovation Systems (VINNOVA) through Berzelii EXSELENT;   National Basic Research Program of China  2013CB933402; Diamond Light Source I19.

Tillgänglig från: 2014-02-04 Skapad: 2014-02-03 Senast uppdaterad: 2017-12-06Bibliografiskt granskad
Ingår i avhandling
1. Open-framework Structures Built by Inorganic Clusters: Synthesis and Characterization
Öppna denna publikation i ny flik eller fönster >>Open-framework Structures Built by Inorganic Clusters: Synthesis and Characterization
2014 (Engelska)Doktorsavhandling, sammanläggning (Övrigt vetenskapligt)
Abstract [en]

Novel open-framework germanates and vanadoborates, which are constructed from typical types of clusters, have been synthesized based on different strategies. The crystal structures are solved by using single crystal X-ray diffraction (SXRD) technique or by combined techniques. Additionally, the structures of two open-framework materials, PKU-3 and PKU-16, are determined from nano-sized crystals by rotation electron diffraction (RED) combined with powder X-ray diffraction (PXRD).

This thesis serves as an introduction to synthesis of open-framework germanates and vanadoborates based on different design strategies. Two germanates are obtained; SU-74 is achieved by employing a novel structure directing agent (SDA), SUT-8 is achieved by assembling the novel structure building units (SBUs) of Co@Ge14 with the introduction of cobalt ions in the synthesis. Four strategies are successfully used in construction of open-framework vanadoborates: using metal-oxo polyhedra as the linkages in SUT-6; applying the scale chemistry approach in SUT-7; employing metal-organic complexes as the linkages in SUT-12, SUT-13, SUT-14; and introducing covalent bond organic linkages into SUT-10 and SUT-11. Single crystal X-ray diffraction is used to conduct the structure determination in combination with other techniques.

Furthermore, the structures of two open-framework materials, an aluminoborate PKU-3 and a germanosilicate PKU-16, are solved from nano-sized crystals using RED data. The structures are further confirmed by Rietveld refinement against PXRD data. The advantages of the RED techniques are demonstrated in two aspects. In PKU-3, the presence of seriously preferred orientation and light elements in the structure makes it difficult for structure determination by PXRD, but it is easier by RED. In PKU-16, the RED technique is used to determine its structure from the as-synthesized multi-phasic sample containing nano-sized crystals. After the structure of PKU-16 has been solved, the synthesis of this interesting phase can be optimized and pure PKU-16 can be obtained.

Keywords: Open-framework, germanates, vanadoborates, aluminoborates, germanosilicates, crystal structure, hydrothermal synthesis, single crystal X-ray diffraction, rotation electron diffraction, powder X-ray diffraction

Ort, förlag, år, upplaga, sidor
Stockholm: Department of Materials and Environmental Chemistry (MMK), Stockholm Univeristy, 2014. s. 87
Nyckelord
Open-framework, germanates, vanadoborates, aluminoborates, germanosilicates, crystal structure, hydrothermal synthesis, crystal X-ray diffraction, rotation electron diffraction, powder X-ray diffraction
Nationell ämneskategori
Oorganisk kemi
Forskningsämne
oorganisk kemi
Identifikatorer
urn:nbn:se:su:diva-106853 (URN)978-91-7447-962-1 (ISBN)
Disputation
2014-09-29, Magnélisalen, Kemiska övningslaboratoriet, Svante Arrhenius väg 16 B, Stockholm, 10:00 (Engelska)
Opponent
Handledare
Tillgänglig från: 2014-09-07 Skapad: 2014-08-25 Senast uppdaterad: 2014-09-15Bibliografiskt granskad

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Av författaren/redaktören
Chen, HongYao, QingxiaZou, XiaodongBäckvall, Jan-E.Sun, Junliang
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Avdelningen för oorganisk kemi och strukturkemiInstitutionen för organisk kemiInstitutionen för material- och miljökemi (MMK)
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Chemistry of Materials
Fysikalisk kemiMaterialkemi

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