| 1. |
- Chen, Hong, et al.
(author)
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PKU-3 : An HCI-Inclusive Aluminoborate for Strecker Reaction Solved by Combining RED and PXRD
- 2015
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 137:22, s. 7047-7050
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Journal article (peer-reviewed)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. |
- Christensen, Kirsten E., et al.
(author)
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An open-framework silicogermanate with 26-ring channels built from seven-coordinated (Ge,Si)10(O, OH)28 clusters
- 2008
-
In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 130:12, s. 3758-3759
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Journal article (peer-reviewed)abstract
- We report a new open-framework silicogermanate SU-61 containing 26-ring channels with a low framework density. It can be seen as a crystalline analogue to the mesoporous silica MCM-41. The structure is built from the assembly of (Ge,Si)10(O,OH)28 clusters. It is the first time that silicon has been successfully introduced in the Ge10 cluster in significant amounts (21% of the tetrahedral sites). Five- and six-coordinated Ge10 clusters have previously been observed in other germanate compounds leading to either dense or open structures. In SU-61, the seven-coordinated clusters fall onto yet another underlying net, the osf net. SU-61, along with other Ge10 based frameworks, shows the versatility of the germanate system to adopt defined topologies playing on the connectivity of the clusters following the principles of net decoration and scale chemistry.
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| 3. |
- Gao, Chao, et al.
(author)
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Twist Building Blocks from Planar to Tetrahedral for the Synthesis of Covalent Organic Frameworks
- 2020
-
In: Journal of the American Chemical Society. - 0002-7863 .- 1520-5126. ; 142:8, s. 3718-3723
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Journal article (peer-reviewed)abstract
- Rational construction of covalent organic frameworks (COFs) with novel structures still remains a challenge. Herein, we report the designed synthesis of two COFs, 2D-BPTA-COF and 3D-BMTA-COF, starting from biphenyl-based precursors but with different groups at the ortho positions. Both COFs exhibited high crystallinity and large surface area, and interestingly, 2D-BPTA-COF crystallizes into 2D sheets with AB stacking mode while 3D-BMTA-COF adopts a 7-fold interpenetrated structure with pts topology. This structural difference could be ascribed to the introduction of methyl groups in the building blocks, as the dihedral angle of biphenyl rings in 2D-BPTA-COF is similar to 0 degrees while in 3D-BMTA-COF it is similar to 60 degrees. Therefore, it is possible to synthesize COFs with different structures by twisting building blocks from planar to tetrahedral with steric hindrance. We believe this result represents a general and straightforward way to expand the diversity of tetrahedral nodes for constructing 3D COFs in the future, and moreover, a new tetrahedral node for constructing 3D COFs is now available.
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| 4. |
- Li, Jian, et al.
(author)
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Discovery of Complex Metal Oxide Materials by Rapid Phase Identification and Structure Determination
- 2019
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 141:12, s. 4990-4996
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Journal article (peer-reviewed)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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| 5. |
- Liu, Xiaoling, et al.
(author)
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A Crystalline Three-Dimensional Covalent Organic Framework with Flexible Building Blocks
- 2021
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 143:4, s. 2123-2129
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Journal article (peer-reviewed)abstract
- The construction of three-dimensional covalent organic frameworks (3D COFs) has proven to be very challenging, as their synthetic driving force mainly comes from the formation of covalent bonds. To facilitate the synthesis, rigid building blocks are always the first choice for designing 3D COFs. In principle, it should be very appealing to construct 3D COFs from flexible building blocks, but there are some obstacles blocking the development of such systems, especially for the designed synthesis and structure determination. Herein, we reported a novel highly crystalline 3D COF (FCOF-5) with flexible C–O single bonds in the building block backbone. By merging 17 continuous rotation electron diffraction data sets, we successfully determined the crystal structure of FCOF-5 to be a 6-fold interpenetrated pts topology. Interestingly, FCOF-5 is flexible and can undergo reversible expansion/contraction upon vapor adsorption/desorption, indicating a breathing motion. Moreover, a smart soft polymer composite film with FCOF-5 was fabricated, which can show a reversible vapor-triggered shape transformation. Therefore, 3D COFs constructed from flexible building blocks can exhibit interesting breathing behavior, and finally, a totally new type of soft porous crystals made of pure organic framework was announced.
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| 6. |
- Ma, Tianqiong, et al.
(author)
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Observation of Interpenetration Isomerism in Covalent Organic Frameworks
- 2018
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 140:22, s. 6763-6766
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Journal article (peer-reviewed)abstract
- We report herein the first example of interpenetration isomerism in covalent organic frameworks (COFs). As a well-known three-dimensional (3D) COF, COF-300 was synthesized and characterized by the Yaghi group in 2009 as a 5-fold interpenetrated diamond structure (dia-cS topology). We found that adding an aging process prior to the reported synthetic procedure afforded the formation of an interpenetration isomer, dia-c7 COF-300. The 7-fold interpenetrated diamond structure of this new isomer was identified by powder Xray diffraction and rotation electron diffraction analyses. Furthermore, we proposed a universal formula to accurately determine the number of interpenetration degrees of dia-based COFs from only the unit cell parameters and the length of the organic linker. This work not only provides a novel example to the category of interpenetration isomerism but also provides new insights for the further development of 3D COFs.
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| 7. |
- Willhammar, Tom, et al.
(author)
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EMM-23 : A Stable High-Silica Multidimensional Zeolite with Extra-Large Trilobe-Shaped Channels.
- 2014
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In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 136:39, s. 13570-3
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Journal article (peer-reviewed)abstract
- Stable, multidimensional, and extra-large pore zeolites are desirable by industry for catalysis and separation of bulky molecules. Here we report EMM-23, the first stable, three-dimensional extra-large pore aluminosilicate zeolite. The structure of EMM-23 was determined from submicron-sized crystals by combining electron crystallography, solid-state nuclear magnetic resonance (NMR), and powder X-ray diffraction. The framework contains highly unusual trilobe-shaped pores that are bound by 21-24 tetrahedral atoms. These extra-large pores are intersected perpendicularly by a two-dimensional 10-ring channel system. Unlike most ideal zeolite frameworks that have tetrahedral sites with four next-nearest tetrahedral neighbors (Q(4) species), this unusual zeolite possesses a high density of Q(2) and Q(3) silicon species. It is the first zeolite prepared directly with Q(2) species that are intrinsic to the framework. EMM-23 is stable after calcination at 540 °C. The formation of this highly interrupted structure is facilitated by the high density of extra framework positive charge introduced by the dicationic structure directing agent.
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| 8. |
- Xie, Yang, et al.
(author)
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Tuning the Topology of Three-Dimensional Covalent Organic Frameworks via Steric Control : From pts to Unprecedented Ijh
- 2021
-
In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 143:19, s. 7279-7284
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Journal article (peer-reviewed)abstract
- Whether or not the topology of three-dimensional covalent organic frameworks (3D COFs) can be tuned via steric control remains a big question and has never been reported. Herein, we describe the designed synthesis of two highly crystalline 3D COFs (3D-TPB-COF-OMe and 3D-TPB-COF-Ph), through the polycondensation of tetra(p-aminophenyl)methane and methoxy-or phenyl- substituted 1,2,4,5-tetralcis(4-formylphenyobenzene on the 3- and 6-positions. Amazingly, by using the continuous rotation electron diffraction technique, 3D-TPB-COF-OMe is determined to have a 5-fold interpenetrated structure with a reported pts net, while 3D-TPB-COF-Ph adopts an unprecedented self-penetrated Ijh topology (Ijh = Luojia Hill) that does not exist in the database of ToposPro. Therefore, by altering the substituents from methoxy to phenyl groups, the topology of designed 3D COFs changes accordingly, and a rare net is now available. This result clearly demonstrates that such COF structures need to be carefully determined due to its complexity, and moreover, it is promising to design 3D COFs with new topology for interesting application by increasing the steric hindrance of molecular building blocks.
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| 9. |
- Yang, Sihai, et al.
(author)
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Irreversible Network Transformation in a Dynamic Porous Host Catalyzed by Sulfur Dioxide
- 2013
-
In: Journal of the American Chemical Society. - : American Chemical Society (ACS). - 0002-7863 .- 1520-5126. ; 135:13, s. 4954-4957
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Journal article (peer-reviewed)abstract
- Porous NOTT-202a shows exceptionally high uptake of SO2, 13.6 mmol g(-1) (87.0 wt %) at 268 K and 1.0 bar, representing the highest value reported to date for a framework material. NOTT-202a undergoes a distinct irreversible framework phase transition upon SO2 uptake at 268-283 K to give NOTT-202b which has enhanced stability due to the formation of strong pi...pi interactions between interpenetrated networks.
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