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  • 1
    Online Resource
    Online Resource
    Switching between Local and Global Aromaticity in a Conjugated Macrocycle for High‐Performance Organic Sodium‐Ion Battery Anodes
    Wiley ; 2020
    In:  Angewandte Chemie International Edition Vol. 59, No. 31 ( 2020-07-27), p. 12958-12964
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 59, No. 31 ( 2020-07-27), p. 12958-12964
    Abstract: Aromatic organic compounds can be used as electrode materials in rechargeable batteries and are expected to advance the development of both anode and cathode materials for sodium‐ion batteries (SIBs). However, most aromatic organic compounds assessed as anode materials in SIBs to date exhibit significant degradation issues under fast‐charge/discharge conditions and unsatisfying long‐term cycling performance. Now, a molecular design concept is presented for improving the stability of organic compounds for battery electrodes. The molecular design of the investigated compound, [2.2.2.2]paracyclophane‐1,9,17,25‐tetraene (PCT), can stabilize the neutral state by local aromaticity and the doubly reduced state by global aromaticity, resulting in an anode material with extraordinarily stable cycling performance and outstanding performance under fast‐charge/discharge conditions, demonstrating an exciting new path for the development of electrode materials for SIBs and other types of batteries.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v59.31
    DOI: 10.1002/anie.202003386
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2020
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 2
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    Mixed-valent 1:1 oxidotellurates(IV/VI) of Na, K and Rb: superstructure and three-dimensional disorder
    Walter de Gruyter GmbH ; 2023
    In:  Zeitschrift für Kristallographie - Crystalline Materials Vol. 238, No. 1-2 ( 2023-01-27), p. 7-15
    Details
    In: Zeitschrift für Kristallographie - Crystalline Materials, Walter de Gruyter GmbH, Vol. 238, No. 1-2 ( 2023-01-27), p. 7-15
    Abstract: Single crystals of three mixed-valent oxidotellurates(IV/VI) with general formula M 2 Te IV Te VI O 6 (H 2 O) x ( M  = Na, K, Rb) were grown under hydrothermal conditions at 210 °C from M 2 CO 3 , TeO 2 and Te(OH) 6 in a 4:1:1 molar ratio. Na 2 Te 2 O 6 ·11/8H 2 O (where Te IV Te VI is abbreviated as Te 2 ) crystallizes as a monoclinic eightfold superstructure with occupational modulation of the water molecules. The structure is built of diperiodic corrugated [Te 2 O 6 ] 2− networks interleaved by the Na atoms and H 2 O molecules. The hexagonal crystal structures of M 2 Te 2 O 4 (OH) 4 ( M  = K, Rb; x  = 2) with P 6 3 / mmc symmetry are made up of [Te 2 O 4 (OH) 4 ] 2− rods extending in the [001] direction. The rods are connected by the M atoms. The [Te IV O 2 (OH) 2 ] units are disordered about the threefold axis, resulting in pronounced three-dimensional diffuse scattering.
    Type of Medium: Online Resource
    ISSN: 2194-4946 , 2196-7105
    URL: Article
    DOI: 10.1515/zkri-2022-0036
    RVK:
    VA 8180
    Language: English
    Publisher: Walter de Gruyter GmbH
    Publication Date: 2023
    SSG: 13
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  • 3
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    Online Resource
    Synthese N ‐heterocyclischer Carbene und ihrer Komplexe durch Chloroniumionabstraktion von 2‐Chlorazoliumsalzen mit elektronenreichen Phosphanen
    Wiley ; 2022
    In:  Angewandte Chemie Vol. 134, No. 28 ( 2022-07-11)
    Details
    In: Angewandte Chemie, Wiley, Vol. 134, No. 28 ( 2022-07-11)
    Abstract: NHCs werden konventionell durch Deprotonierung von Azoliumsalzen mit starken anionischen Basen synthetisiert. Diese Reaktion ist oft unselektiv und kann zu Alkalimetall‐Komplexen der NHCs oder zu dimerisierten NHCs führen. Alternativ können NHCs durch Dechlorierung von 2‐Chlorazoliumsalzen mit elektronenreichen Phosphanen erhalten werden. PPh 3 , PCy 3 und PtBu 3 sind ungeeignet für die Cl + ‐Abstraktion, während das sterisch anspruchsvolle Tris(1,3‐ tert ‐butylimidazolidin‐2‐ylidenamino)phosphan 1 selektiv Cl + von 2‐Chlorazoliumsalzen entfernt. Da das sterisch anspruchsvolle 1 nicht an Metallkomplexe bindet, wurde es für die Synthese von NHC‐Komplexen durch in‐situ‐Chloroniumabstraktion von 2‐Chlorazoliumsalzen eingesetzt. Die Dechlorierung wurde auch für die regioselektive Monometallierung einer Bis‐NHC‐Ligandenvorstufe bestehend aus einer 2‐Chlorbenzimidazolium‐ und einer 2‐Chlorbenzimidazolgruppe mit Ir I , Ir III , Rh I , Rh III und Ru II eingesetzt, gefolgt von der Synthese des heterobimetallischen Ir III /Pd II ‐Komplexes [ 18 ](BF 4 ) 2 in einer Dechlorierung/Oxidative‐Addition‐Reaktionssequenz.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v134.28
    DOI: 10.1002/ange.202202190
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2022
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    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
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  • 4
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    Synthesis of N ‐Heterocyclic Carbenes and Their Complexes by Chloronium Ion Abstraction from 2‐Chloroazolium Salts Using Electron‐Rich Phosphines
    Wiley ; 2022
    In:  Angewandte Chemie International Edition Vol. 61, No. 28 ( 2022-07-11)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 61, No. 28 ( 2022-07-11)
    Abstract: N ‐Heterocyclic carbenes (NHCs) are commonly prepared by deprotonation of azolium salts using strong anionic bases. This reaction is often unselective, yielding alkali metal NHC complexes or dimerized NHCs. Alternatively, free NHCs are obtained by the dechlorination of 2‐chloroazolium salts using electron‐rich phosphines. PPh 3 , PCy 3 , and P t Bu 3 are unsuitable for Cl + abstraction, while the sterically encumbered tris(1,3‐ tert ‐butylimidazolidin‐2‐ylidenamino)phosphine 1 selectively removes Cl + from 2‐chloroazolium salts. Since bulky 1 does not bind to metal complexes, it was used for the preparation of NHC complexes via in situ Cl + abstraction from 2‐chloroazolium salts. The dechlorination was employed for the site‐selective monometallation with Ir I , Ir III , Rh I , Rh III , and Ru II of a bis‐NHC precursor composed of a 2‐chlorobenzimidazolium and a 2‐chlorobenzimidazole group, followed by the preparation of the heterobimetallic Ir III /Pd II complex [ 18 ](BF 4 ) 2 by a dechlorination/oxidative addition reaction sequence.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v61.28
    DOI: 10.1002/anie.202202190
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 5
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    The alkali metal copper(II) oxidotellurates(IV) Li 2 Cu 2 Te 3 O 9 , Li 2 Cu 3 Te 4 O 12 , Rb 2 Cu 3 Te 6 O 16 and Cs 2 Cu 3 Te 6 O 16 – four new structure types
    Wiley ; 2022
    In:  Zeitschrift für anorganische und allgemeine Chemie Vol. 648, No. 23 ( 2022-12-13)
    Details
    In: Zeitschrift für anorganische und allgemeine Chemie, Wiley, Vol. 648, No. 23 ( 2022-12-13)
    Abstract: Four new M I /Cu II /Te IV /O phases were obtained under hydrothermal conditions or with water as a mineralizer, and their crystal structures determined by single‐crystal X‐ray diffraction. Li 2 Cu 2 Te 3 O 9 comprises trigonal‐pyramidal [TeO 3 ], distorted tetrahedral [LiO 4 ] and distorted square‐pyramidal [CuO 5 ] units, forming a framework penetrated by channels into which the electron lone pairs of the Te IV atoms are directed. Li 2 Cu 3 Te 4 O 12 contains isolated trigonal‐pyramidal [TeO 3 ] units, tetrahedral [LiO 4 ] groups forming [Li 2 O 6 ] dimers by sharing an edge, as well as square‐planar [CuO 4 ] and square‐pyramidal [CuO 5 ] units, forming [Cu 3 O 10 ] chains oriented parallel to [100] . These units also form a framework structure with channels where the electron lone pairs reside. Rb 2 Cu 3 Te 6 O 16 and Cs 2 Cu 3 Te 6 O 16 have isopointal crystal structures containing isolated [TeO 3 ] groups and [Te 4 O 10 ] chains oriented parallel to [010] . While in Rb 2 Cu 3 Te 6 O 16 both Cu sites are 4‐coordinate in form of nearly square‐planar [CuO 4 ] units, in Cs 2 Cu 3 Te 6 O 16 one Cu site has a fifth oxygen contact resulting in a distorted square‐pyramidal [CuO 5 ] polyhedron. Both crystal structures are made up from two alternating layer types stacked along [100] . The differences between Rb 2 Cu 3 Te 6 O 16 and Cs 2 Cu 3 Te 6 O 16 originate almost exclusively from the layer type consisting of the 5‐coordinate Cu site in Cs 2 Cu 3 Te 6 O 16 , while the other layer type shows almost no difference. A quantitative comparison between the two crystal structures is given.
    Type of Medium: Online Resource
    ISSN: 0044-2313 , 1521-3749
    URL: Issue
    URL: Article
    DOI: 10.1002/zaac.v648.23
    DOI: 10.1002/zaac.202200089
    RVK:
    VA 8102
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 201094-X
    detail.hit.zdb_id: 1481139-X
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  • 6
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    Online Resource
    Cr(II) and Cr(III) NCN pincer complexes: synthesis, structure, and catalytic reactivity
    Springer Science and Business Media LLC ; 2023
    In:  Monatshefte für Chemie - Chemical Monthly
    Details
    In: Monatshefte für Chemie - Chemical Monthly, Springer Science and Business Media LLC
    Abstract: The synthesis, characterization, and reactivity of several new Cr(II) and Cr(III) complexes featuring an NCN pincer ligand with an arene backbone connected to amine donors NEt 2 and N i Pr 2 via CH 2 -linkers is described. Reacting the in situ lithiated ligand precursor N(C–Br)N CH2 -Et with [CrCl 3 (THF) 3 ] resulted in the formation of the Cr(III) complex trans -[Cr(κ 3 NCN -NCN CH2 -Et)(Cl) 2 (THF)]. Upon reaction of lithiated N(C–Br)N CH2 - i Pr with a suspension of anhydrous CrCl 2 , the Cr(II) complex [Cr(κ 2 NC -NCN CH2 - i Pr) 2 ] is formed featuring two NCN ligands bound in κ 2 NC -fashion. In contrast, when lithiated N(C–Br)N CH2 - i Pr is reacted with a homogeneous solution of anhydrous Cr X 2 ( X  = Cl, Br), complexes [Cr(κ 3 NCN- NCN CH2 - i Pr)X] are obtained. Treatment of [Cr(κ 3 NCN- NCN CH2 - i Pr)Cl] with 1 equiv of PhCH 2 MgCl and LiCH 2 SiMe 3 afforded the alkyl complexes [Cr(κ 3 NCN -NCN CH2 - i Pr)(CH 2 Ph)] and [Cr(κ 3 NCN -NCN CH2 - i Pr)(CH 2 SiMe 3 )]. All Cr(II) complexes exhibit effective magnetic moments in the range of 4.7–4.9  µ B which is indicative for d 4 high spin systems. If a solution of lithiated N(C–Br)N CH2 - i Pr is treated with CrCl 2 , followed by addition of an excess of Na[HB(Et) 3 ], the dimeric complex [Cr(κ 2 NC -NCN CH2 - i Pr)(μ 2 -H)] 2 is obtained bearing two bridging hydride ligands. [Cr(κ 3 NCN -NCN CH2 - i Pr)(CH 2 SiMe 3 )] turned out to be catalytically active for the hydrosilylation of ketones at room temperature with a catalyst loading of 1 mol%. X-ray structures of all complexes are presented. Graphical abstract
    Type of Medium: Online Resource
    ISSN: 0026-9247 , 1434-4475
    URL: Article
    DOI: 10.1007/s00706-023-03128-6
    RVK:
    VA 6100
    Language: English
    Publisher: Springer Science and Business Media LLC
    Publication Date: 2023
    detail.hit.zdb_id: 1462037-6
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  • 7
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    Online Resource
    Tuning Heterocalixarenes to Improve Their Anion Recognition: A Computational Approach
    American Chemical Society (ACS) ; 2018
    In:  The Journal of Physical Chemistry A Vol. 122, No. 12 ( 2018-03-29), p. 3328-3336
    Details
    In: The Journal of Physical Chemistry A, American Chemical Society (ACS), Vol. 122, No. 12 ( 2018-03-29), p. 3328-3336
    Type of Medium: Online Resource
    ISSN: 1089-5639 , 1520-5215
    URL: Article
    URL: Article
    DOI: 10.1021/acs.jpca.8b01866
    DOI: 10.1021/acs.jpca.8b01866.s001
    RVK:
    VA 5430.A
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2018
    detail.hit.zdb_id: 2006031-2
    detail.hit.zdb_id: 1357795-5
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  • 8
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    Phase formation studies and crystal structure refinements in the Mn II /Te IV /O/(H) system
    Wiley ; 2022
    In:  Zeitschrift für anorganische und allgemeine Chemie Vol. 648, No. 24 ( 2022-12-27)
    Details
    In: Zeitschrift für anorganische und allgemeine Chemie, Wiley, Vol. 648, No. 24 ( 2022-12-27)
    Abstract: Systematic phase formation studies in the system Mn II /Te IV /O/‐(H) using either solid‐state reactions between stoichiometric MnO:TeO 2 mixtures or hydrothermal reactions under basic conditions led to crystal growth of two polymorphs ( α ‐, γ ‐) of MnTeO 3 , Mn 6 Te 5 O 16 , Mn 15 (TeO 3 ) 14 (OH) 2 and Mn 3 (TeO 3 ) 2 (OH) 2 . Although α‐ MnTeO 3 and Mn 6 Te 5 O 16 have been reported previously, crystal structure refinements were missing so far. Whereas α ‐MnTeO 3 crystallizes in a unique structure (space group Pbca , Z =16), Mn 6 Te 5 O 16 ( Pnma , Z =4) is isotypic with its Co‐homologue. The previously unknown phases γ ‐MnTeO 3 ( Pbca , Z =8), Mn 15 (TeO 3 ) 14 (OH) 2 ( , Z =3) and Mn 3 (TeO 3 ) 2 (OH) 2 ( P 6 3 mc , Z =4) all have isotypic relationships, namely with ZnTeO 3 , Co 15 (TeO 3 ) 14 F 2 and M 3 (TeO 3 ) 2 (OH) 2 ( M =Ni, Co), respectively. Common to all crystal structures of the five manganese(II) oxidotellurate(IV) phases is the presence of [MnO 5 ] or [MnO 6 ] polyhedra and isolated trigonal‐pyramidal [TeO 3 ] groups (except for one of the Te IV atoms in Mn 6 Te 5 O 16 [TeO 4 ] bisphenoids) as principal building units, which share corners and edges with the [MnO 5/6 ] groups. The resulting three‐dimensional frameworks are dominated by the influence of the stereochemically active 5  s 2 electron lone pair situated at the Te IV atom, leading to the formation of channels or interstices. Quantitative comparisons between the corresponding isotypic crystal structures are given.
    Type of Medium: Online Resource
    ISSN: 0044-2313 , 1521-3749
    URL: Issue
    URL: Article
    DOI: 10.1002/zaac.v648.24
    DOI: 10.1002/zaac.202200205
    RVK:
    VA 8102
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 201094-X
    detail.hit.zdb_id: 1481139-X
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  • 9
    Online Resource
    Online Resource
    Switching between Local and Global Aromaticity in a Conjugated Macrocycle for High‐Performance Organic Sodium‐Ion Battery Anodes
    Wiley ; 2020
    In:  Angewandte Chemie Vol. 132, No. 31 ( 2020-07-27), p. 13058-13064
    Details
    In: Angewandte Chemie, Wiley, Vol. 132, No. 31 ( 2020-07-27), p. 13058-13064
    Abstract: Aromatic organic compounds can be used as electrode materials in rechargeable batteries and are expected to advance the development of both anode and cathode materials for sodium‐ion batteries (SIBs). However, most aromatic organic compounds assessed as anode materials in SIBs to date exhibit significant degradation issues under fast‐charge/discharge conditions and unsatisfying long‐term cycling performance. Now, a molecular design concept is presented for improving the stability of organic compounds for battery electrodes. The molecular design of the investigated compound, [2.2.2.2]paracyclophane‐1,9,17,25‐tetraene (PCT), can stabilize the neutral state by local aromaticity and the doubly reduced state by global aromaticity, resulting in an anode material with extraordinarily stable cycling performance and outstanding performance under fast‐charge/discharge conditions, demonstrating an exciting new path for the development of electrode materials for SIBs and other types of batteries.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v132.31
    DOI: 10.1002/ange.202003386
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2020
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
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  • 10
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    Online Resource
    Order-disorder (OD) structures of Rb 2 Zn(TeO 3 )(CO 3 )·H 2 O and Na 2 Zn 2 Te 4 O 11
    Walter de Gruyter GmbH ; 2022
    In:  Zeitschrift für Kristallographie - Crystalline Materials Vol. 237, No. 8-9 ( 2022-09-27), p. 329-341
    Details
    In: Zeitschrift für Kristallographie - Crystalline Materials, Walter de Gruyter GmbH, Vol. 237, No. 8-9 ( 2022-09-27), p. 329-341
    Abstract: Single crystals of the two alkali metal zinc oxidotellurates(IV), Rb 2 Zn(TeO 3 )(CO 3 )·H 2 O and Na 2 Zn 2 Te 4 O 11 , were obtained by reactions of mixtures of ZnO, TeO 2 , Rb 2 CO 3 (molar ratios 2:3:6) and ZnO, TeO 2 , Na 2 CO 3 (molar ratios 2:3:10), respectively, with small amounts of water as a mineralizer. Both compounds crystallize as order-disorder (OD) structures of layers and feature a high stacking fault probability. The crystal structure of Rb 2 Zn(TeO 3 )(CO 3 )·H 2 O is composed of layers extending parallel to (100). The structure is composed of two kinds of non-polar OD layers consisting of trigonal-pyramidal [TeO 3 ] 2− , tetrahedral [ZnO 4 ] 6− , Rb1 + , and CO 3 2− , H 2 O, Rb2 + , respectively. Different centrings of the layer groups lead to an ambiguity in the stacking arrangement. The crystal structure of Na 2 Zn 2 Te 4 O 11 is built from layers extending parallel to (001). Trigonal-pyramidal [TeO 3 ] 2− and bisphenoidal [TeO 4 ] 4− polyhedra form [Te 4 O 11 ] 6− groups, which are connected by longer Te–O-contacts to form 1 ∞ [Te 8 O 22 ] 12− double chains oriented along either [100] or [010] . These chains form non-polar layers, which appear alternatingly in two orientations related by a fourfold rotoinversion. The Zn 2+ and Na + cations are located at the layer interface. The stacking ambiguity is due to different lattices of adjacent layers.
    Type of Medium: Online Resource
    ISSN: 2194-4946 , 2196-7105
    URL: Article
    DOI: 10.1515/zkri-2022-0030
    RVK:
    VA 8180
    Language: English
    Publisher: Walter de Gruyter GmbH
    Publication Date: 2022
    SSG: 13
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