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  • 1
    Online Resource
    Online Resource
    Microporous Cyclic Titanium‐Oxo Clusters with Labile Surface Ligands
    Wiley ; 2017
    In:  Angewandte Chemie Vol. 129, No. 51 ( 2017-12-18), p. 16470-16474
    Details
    In: Angewandte Chemie, Wiley, Vol. 129, No. 51 ( 2017-12-18), p. 16470-16474
    Abstract: By using ethylene glycol and monocarboxylic acid as surface ligands, a series of cyclic Ti‐oxo clusters (CTOC) with permanent microporosity are successfully synthesized. With a cyclic {Ti 32 O 16 } backbone made of eight connected Ti 4 tetrahedral cages that are arranged in a zigzag fashion, the clusters have a “donut” shape with an inner diameter of 8.3 Å, outer diameter of 26.9 Å and height of 10.4 Å. While both inner and outer walls of the “donut” clusters are modified by double‐deprotonated ethylene glycolates, their upper and lower surfaces are bound by carboxylates and mono‐deprotonated ethylene glycolates. The clusters are readily packed into one‐dimensional tubes which are further arranged in two different modes into crystalline microporous solids with surface areas over 660 m 2  g −1 , depending on the surface carboxylates. The solid with olefin‐bearing carboxylates exhibits a superior CO 2 adsorption capacity of 40 cm 3  g −1 at 273 K under 1 atm. Moreover, the mono‐deprotonated ethylene glycolates on the clusters are demonstrated to be highly exchangeable by other alcohols, providing a nice platform for creating microporous solids or films with a wide variety of surface functionalities.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v129.51
    DOI: 10.1002/ange.201709096
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2017
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  • 2
    Online Resource
    Online Resource
    Thiol-stabilized atomically precise, superatomic silver nanoparticles for catalysing cycloisomerization of alkynyl amines
    Oxford University Press (OUP) ; 2018
    In:  National Science Review Vol. 5, No. 5 ( 2018-09-01), p. 694-702
    Details
    In: National Science Review, Oxford University Press (OUP), Vol. 5, No. 5 ( 2018-09-01), p. 694-702
    Abstract: Both the electronic and surface structures of metal nanomaterials play critical roles in determining their chemical properties. However, the non-molecular nature of conventional nanoparticles makes it extremely challenging to understand the molecular mechanism behind many of their unique electronic and surface properties. In this work, we report the synthesis, molecular and electronic structures of an atomically precise nanoparticle, [Ag206L72]q (L = thiolate, halide; q = charge). With a four-shell Ag7@Ag32@Ag77@Ag90 Ino-decahedral structure having a nearly perfect D5h symmetry, the metal core of the nanoparticle is co-stabilized by 68 thiolate and 4 halide ligands. Both electrochemistry and plasmonic absorption reveal the metallic nature of the nanoparticles, which is explained by density functional theory calculations. Electronically, the nanoparticle can be considered as a superatom, just short of a major electron shell closing of 138 electrons (q = –4). More importantly, many of ligands capping on the nanoparticle are labile due to their low-coordination modes, leading to high surface reactivity for catalysing the synthesis of indoles from 2-ethynylaniline derivatives. The results exemplify the power of the atomic-precision nanocluster approach to catalysis in probing reaction mechanisms and in revealing the interplay of heterogeneous reactivities, electronic and surface structural dynamics, thereby providing ways for optimization.
    Type of Medium: Online Resource
    ISSN: 2095-5138 , 2053-714X
    URL: Article
    DOI: 10.1093/nsr/nwy034
    Language: English
    Publisher: Oxford University Press (OUP)
    Publication Date: 2018
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  • 3
    Online Resource
    Online Resource
    Microporous Cyclic Titanium‐Oxo Clusters with Labile Surface Ligands
    Wiley ; 2017
    In:  Angewandte Chemie International Edition Vol. 56, No. 51 ( 2017-12-18), p. 16252-16256
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 56, No. 51 ( 2017-12-18), p. 16252-16256
    Abstract: By using ethylene glycol and monocarboxylic acid as surface ligands, a series of cyclic Ti‐oxo clusters (CTOC) with permanent microporosity are successfully synthesized. With a cyclic {Ti 32 O 16 } backbone made of eight connected Ti 4 tetrahedral cages that are arranged in a zigzag fashion, the clusters have a “donut” shape with an inner diameter of 8.3 Å, outer diameter of 26.9 Å and height of 10.4 Å. While both inner and outer walls of the “donut” clusters are modified by double‐deprotonated ethylene glycolates, their upper and lower surfaces are bound by carboxylates and mono‐deprotonated ethylene glycolates. The clusters are readily packed into one‐dimensional tubes which are further arranged in two different modes into crystalline microporous solids with surface areas over 660 m 2  g −1 , depending on the surface carboxylates. The solid with olefin‐bearing carboxylates exhibits a superior CO 2 adsorption capacity of 40 cm 3  g −1 at 273 K under 1 atm. Moreover, the mono‐deprotonated ethylene glycolates on the clusters are demonstrated to be highly exchangeable by other alcohols, providing a nice platform for creating microporous solids or films with a wide variety of surface functionalities.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v56.51
    DOI: 10.1002/anie.201709096
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2017
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