TY  - JOUR
A1  - Yang, Jin
A1  - Ghosh, Samrat
A1  - Roeser, Jérôme
A1  - Acharjya, Amitava
A1  - Penschke, Christopher
A1  - Tsutsui, Yusuke
A1  - Rabeah, Jabor
A1  - Wang, Tianyi
A1  - Tameu, Simon Yves Djoko
A1  - Ye, Meng-Yang
A1  - Grüneberg, Julia
A1  - Li, Shuang
A1  - Li, Changxia
A1  - Schomaecker, Reinhard
A1  - Van de Krol, Roel
A1  - Seki, Shu
A1  - Saalfrank, Peter
A1  - Thomas, Arne
T1  - Constitutional isomerism of the linkages in donor–acceptor covalent organic frameworks and its impact on photocatalysis
JF  - Nature Communications
N2  - When new covalent organic frameworks (COFs) are designed, the main efforts are typically focused on selecting specific building blocks with certain geometries and properties to control the structure and function of the final COFs. The nature of the linkage (imine, boroxine, vinyl, etc.) between these building blocks naturally also defines their properties. However, besides the linkage type, the orientation, i.e., the constitutional isomerism of these linkages, has rarely been considered so far as an essential aspect. In this work, three pairs of constitutionally isomeric imine-linked donor-acceptor (D-A) COFs are synthesized, which are different in the orientation of the imine bonds (D-C=N-A (DCNA) and D-N=C-A (DNCA)). The constitutional isomers show substantial differences in their photophysical properties and consequently in their photocatalytic performance. Indeed, all DCNA COFs show enhanced photocatalytic H2 evolution performance than the corresponding DNCA COFs. Besides the imine COFs shown here, it can be concluded that the proposed concept of constitutional isomerism of linkages in COFs is quite universal and should be considered when designing and tuning the properties of COFs.
Y1  - 2022
U6  - https://doi.org/10.1038/s41467-022-33875-9
SN  - 2041-1723
VL  - 13
IS  - 1
PB  - Nature Publishing Group UK
CY  - [London]
ER  - 
TY  - JOUR
A1  - Mondal, Suvendu Sekhar
A1  - Thomas, Arne
A1  - Holdt, Hans-Jürgen
T1  - In situ synthesis of amide-imidate-imidazolate ligand and formation of metal-organic frameworks: Application for gas storage
JF  - Microporous and mesoporous materials : zeolites, clays, carbons and related materials
N2  - In this review article, we highlight the synthesis, structures and gas-sorption properties of a series of nine isostructural IFPs (IFP = Imidazolate Framework Potsdam) and two H-bonded networks. IFPs were synthesized by in situ partial hydrolysis of a 4,5-dicyanoimidazole under solvothermal conditions and hence an imidazolate-4-amide-5-imidate linker (C5H3N4O2) was generated, forming the metal -amide-imidate-imidazolateframeworks [M(C5H3N4O2)-R]. Varying R in the 2-substitued linker (R = Me, Cl, Br, Et, OMe and OEt) and metal centre (M2+ = zinc and cobalt) allowed the variation in channel diameter (4.2-03 angstrom) and a fine-tuning of the polarity and functionality of the channel walls of IFPs. Furthermore, we show that using ethyl or alkoxy substituted IFPs the flexible groups act as molecular gates for guest molecules. This allows highly selective CO2 sorption over Ny and CH4 gases. Moreover, during the synthesis of methoxy substituted IFPs (IFP-7 and -8), an imidazolate-4,5-diamide-2-olate linker (C5H4N4O3) formed in situ leads to the formation of a molecular building block (MBB) with a M-6 octahedron inscribed in a M-8 cube (M Zn2+ and Co2+). The MBBs connect by amide amide hydrogen bonds to a 3D robust supramolecular networks [Zn-14(C5H4N4O3)(12)(O) (OH)(2) (DMF)(4) denoted as 1 and 2, respectively, DMF = N,N'-dimethylformamide], which can be activated for N-2, CO2, CH4, and H-2 gas-sorption. (C) 2015 Elsevier Inc. All rights reserved.
KW  - Flexible linker
KW  - Gas sorption
KW  - Gate-effects
KW  - Hydrogen-bonding
KW  - Solvothermal synthesis
Y1  - 2015
U6  - https://doi.org/10.1016/j.micromeso.2015.01.049
SN  - 1387-1811
SN  - 1873-3093
VL  - 216
SP  - 2
EP  - 12
PB  - Elsevier
CY  - Amsterdam
ER  - 
TY  - JOUR
A1  - Debatin, Franziska
A1  - Möllmer, Jens
A1  - Mondal, Suvendu Sekhar
A1  - Behrens, Karsten
A1  - Möller, Andreas
A1  - Staudt, Reiner
A1  - Thomas, Arne
A1  - Holdt, Hans-Jürgen
T1  - Mixed gas adsorption of carbon dioxide and methane on a series of isoreticular microporous metal-organic frameworks based on 2-substituted imidazolate-4-amide-5-imidates
JF  - Journal of materials chemistry
N2  - In this work the adsorption of CO2 and CH4 on a series of isoreticular microporous metal-organic frameworks based on 2-substituted imidazolate-4-amide-5-imidates, IFP-1-IFP-6 (IFP Imidazolate Framework Potsdam), is studied firstly by pure gas adsorption at 273 K. All experimental isotherms can be nicely described by using the Toth isotherm model and show the preferred adsorption of CO2 over CH4. At low pressures the Toth isotherm equation exhibits a Henry region, wherefore Henry's law constants for CO2 and CH4 uptake could be determined and ideal selectivity (alpha CO2/CH4) has been calculated. Secondly, selectivities were calculated from mixture data by using nearly equimolar binary mixtures of both gases by a volumetric-chromatographic method to examine the IFPs. Results showed the reliability of the selectivity calculation. Values of (alpha CO2/CH4) around 7.5 for IFP-5 indicate that this material shows much better selectivities than IFP-1, IFP-2, IFP-3, IFP-4 and IFP-6 with slightly lower selectivity (alpha CO2/CH4) = 4-6. The preferred adsorption of CO2 over CH4 especially of IFP-5 and IFP-4 makes these materials suitable for gas separation application.
Y1  - 2012
U6  - https://doi.org/10.1039/c2jm15811f
SN  - 0959-9428
VL  - 22
IS  - 20
SP  - 10221
EP  - 10227
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Thiel, Kerstin
A1  - Zehbe, Rolf
A1  - Röser, Jerome
A1  - Strauch, Peter
A1  - Enthaler, Stephan
A1  - Thomas, Arne
T1  - A polymer analogous reaction for the formation of imidazolium and NHC based porous polymer networks
JF  - Polymer Chemistry
N2  - A polymer analogous reaction was carried out to generate a porous polymeric network with N-heterocyclic carbenes (NHC) in the polymer backbone. Using a stepwise approach, first a polyimine network is formed by polymerization of the tetrafunctional amine tetrakis(4-aminophenyl)methane. This polyimine network is converted in the second step into polyimidazolium chloride and finally to a polyNHC network. Furthermore a porous Cu(II)-coordinated polyNHC network can be generated. Supercritical drying generates polymer networks with high permanent surface areas and porosities which can be applied for different catalytic reactions. The catalytic properties were demonstrated for example in the activation of CO2 or in the deoxygenation of sulfoxides to the corresponding sulfides.
Y1  - 2013
U6  - https://doi.org/10.1039/c2py20947k
SN  - 1759-9954
VL  - 4
IS  - 6
SP  - 1848
EP  - 1856
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Fischer, Sabrina
A1  - Schmidt, Johannes
A1  - Strauch, Peter
A1  - Thomas, Arne
T1  - An anionic microporous polymer network prepared by the polymerization of weakly coordinating anions
JF  - Angewandte Chemie : a journal of the Gesellschaft Deutscher Chemiker ; International edition
KW  - borates
KW  - conjugated microporous polymers
KW  - covalent organic frameworks
KW  - ion exchange
KW  - weakly coordinating ions
Y1  - 2013
U6  - https://doi.org/10.1002/anie.201303045
SN  - 1433-7851
SN  - 1521-3773
VL  - 52
IS  - 46
SP  - 12174
EP  - 12178
PB  - Wiley-VCH
CY  - Weinheim
ER  - 
TY  - JOUR
A1  - Thiel, Kerstin
A1  - Zehbe, Rolf
A1  - Roesner, Jerômé
A1  - Strauch, Peter
A1  - Enthaler, Stephan
A1  - Thomas, Arne
T1  - A polymer analogous reaction for the formation of imidazolium and NHC based porous polymer networks
N2  - A polymer analogous reaction was carried out to generate a porous polymeric network with N-heterocyclic carbenes (NHC) in the polymer backbone. Using a stepwise approach, first a polyimine network is formed by polymerization of the tetrafunctional amine tetrakis(4-aminophenyl)methane. This polyimine network is converted in the second step into polyimidazolium chloride and finally to a polyNHC network. Furthermore a porous Cu(II)-coordinated polyNHC network can be generated. Supercritical drying generates polymer networks with high permanent surface areas and porosities which can be applied for different catalytic reactions. The catalytic properties were demonstrated for example in the activation of CO2 or in the deoxygenation of sulfoxides to the corresponding sulfides.
Y1  - 2013
UR  - http://pubs.rsc.org/en/content/articlepdf/2013/py/c2py20947k
U6  - https://doi.org/10.1039/C2PY20947K
ER  - 
TY  - JOUR
A1  - Debatin, Franziska
A1  - Thomas, Arne
A1  - Kelling, Alexandra
A1  - Hedin, Niklas
A1  - Bacsik, Zoltan
A1  - Senkovska, Irena
A1  - Kaskel, Stefan
A1  - Junginger, Matthias
A1  - Müller, Holger
A1  - Schilde, Uwe
A1  - Jäger, Christian
A1  - Friedrich, Alwin
A1  - Holdt, Hans-Jürgen
T1  - In situ synthesis of an imidazolate-4-amide-5-imidate ligand and formation of a microporous zinc-organic framework with H2-and CO2-storage ability
N2  - Narrow channels with polar walls are the structural and functional features responsible for the high capacity of a zinc-organic framework based on an imidazolate-amide-imidate ligand for the uptake of H2 and CO2 (see structure: orange Zn, blue N, red O, dark gray C, light gray H). The rigid and stable chelating ligand was synthesized in situ by partial hydrolysis of a dicyanoimidazole compound.
Y1  - 2010
UR  - http://www3.interscience.wiley.com/cgi-bin/jhome/26737/
U6  - https://doi.org/10.1002/anie.200906188
SN  - 1433-7851
ER  - 
TY  - GEN
A1  - Thiel, Kerstin
A1  - Zehbe, Rolf
A1  - Roeser, Jerômé
A1  - Strauch, Peter
A1  - Enthaler, Stephan
A1  - Thomas, Arne
T1  - A polymer analogous reaction for the formation of imidazolium and NHC based porous polymer networks
N2  - A polymer analogous reaction was carried out to generate a porous polymeric network with N-heterocyclic carbenes (NHC) in the polymer backbone. Using a stepwise approach, first a polyimine network is formed by polymerization of the tetrafunctional amine tetrakis(4-aminophenyl)methane. This polyimine network is converted in the second step into polyimidazolium chloride and finally to a polyNHC network. Furthermore a porous Cu(II)-coordinated polyNHC network can be generated. Supercritical drying generates polymer networks with high permanent surface areas and porosities which can be applied for different catalytic reactions. The catalytic properties were demonstrated for example in the activation of CO2 or in the deoxygenation of sulfoxides to the corresponding sulfides.
T3  - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 243 
KW  - covalent organic framework
KW  - n-heterocyclic carbenes
KW  - carbon-dioxide
KW  - intrinsic microporosity
KW  - heterogeneous catalysis
KW  - sulfoxides
KW  - reduction
KW  - complex
KW  - system
KW  - transformation
Y1  - 2013
U6  - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-95118
SP  - 1848
EP  - 1856
ER  -