Article
Multidisciplinary Sciences
Maximilian Raisch, Wafa Maftuhin, Michael Walter, Michael Sommer
Summary: By designing a mechanochromic donor-acceptor torsional spring, force-dependent red-shifted absorption and emission spectra can be achieved, allowing for sensing and measuring forces, as well as visualizing force distributions in materials.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Raphael Hertel, Wafa Maftuhin, Michael Walter, Michael Sommer
Summary: In this study, we used a series of thiophene-flanked quinoxalines as molecular torsional springs for force sensing in bulk polymers at room temperature. Through detailed spectroscopy and calculations, we identified the thiophene ring flip as the major part of the overall mechanochromic response. The thiophene ring flip requires much smaller forces than planarization of the DAD spring, allowing for sensing of tiny forces and expanding the sensitivity and force range of conformational mechanochromophores.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Kai Sun, Anzai Shi, Yan Liu, Xiaolan Chen, Panjie Xiang, Xiaotong Wang, Lingbo Qu, Bing Yu
Summary: A new method of photoactivation of electron donor-acceptor complexes between arylsulfonium salts and 1,4-diazabicyclo[2.2.2]octane with visible light or natural sunlight was discovered, enabling the generation of aryl radicals under mild conditions, offering a novel opportunity for two-step para-selective C-H functionalization of complex arenes.
Article
Chemistry, Multidisciplinary
Anna C. Overholts, Wendy Granados Razo, Maxwell J. Robb
Summary: Mechanophores are stress-sensitive molecules that undergo productive chemical transformations under mechanical force. A new platform has been introduced to achieve mechanically gated multicolour chromogenic reactivity. This platform is based on an activated furan precursor, which, when mechanochemically activated, generates a diverse range of color variations. This system has been applied to create a complex multicolour composite image through localized compression and reaction with different secondary amines.
Article
Chemistry, Applied
Kevin Masson, Maxime Dousset, Bohdan Biletskyi, Sara Chentouf, Jean-Valere Naubron, Jean-Luc Parrain, Laurent Commeiras, Paola Nava, Gaelle Chouraqui
Summary: An access to functionalised eight-membered carbocyclic ring compounds was developed by stirring an unusual vinylogous Donor-Acceptor Cyclopropane (DAC) in boiling o-xylene. Experimental and computational studies were conducted to explain the observed diastereoselectivity/regioselectivity transfer and provide mechanistic insights.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Energy & Fuels
Bin-Wen Chen, Piao-Yang Xu, Si-Hao Chen, Ke Luan, Zhen-Lin Qiu, Lu Wang, Le-Shan Dai, Yun-Fei Li, Da-Qin Yun, Lin-Long Deng, Su-Yuan Xie, Lan-Sun Zheng
Summary: Three novel donor-acceptor-acceptor small molecules with benzotriazole as the central building block are synthesized and investigated for their molecular structure, electrochemical behavior, and optical properties. Vacuum-deposited small-molecule organic solar cells (SMOSCs) fabricated with these molecules and C-70 as the acceptor exhibit power conversion efficiencies (PCEs) in the range of 6.42-7.43%. One of the molecules shows a promising PCE of 14.84% under indoor illumination, demonstrating its potential in indoor photovoltaic applications.
Article
Chemistry, Multidisciplinary
Yaser Balmohammadi, Simon Grabowsky
Summary: Arsenic and its compounds pollute fresh water and are a major cause of human health problems in some countries due to their toxicity. Intermolecular-interaction-based filters, such as metal-organic frameworks, are an important approach to remove arsenic from fresh water. Therefore, gaining deeper insight and understanding of arsenic-involving intermolecular interactions is crucial.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Chenyu Han, Jianxiao Wang, Liangliang Chen, Jingfei Chen, Long Zhou, Pengchao Wang, Wenfei Shen, Nan Zheng, Shuguang Wen, Yonghai Li, Xichang Bao
Summary: This study investigates the impact of A/A and D/A interactions on the performance of organic solar cells by designing small molecular acceptors with different end caps. It reveals the synergistic or balancing effect of D/A and A/A interactions on the efficiency of bulk-heterojunction interfaces in organic solar cells.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Thomas Choisnet, David Canevet, Marc Salle, Cedric Lorthioir, Laurent Bouteiller, Patrice Woisel, Frederick Niepceron, Erwan Nicol, Olivier Colombani
Summary: Janus nanocylinders were prepared by supramolecular coassembly in water of two different polymers functionalized with complementary assembling units, utilizing a method that combines charge transfer complexation and hydrogen bonding to achieve one-dimensional structures and Janus nanoparticles.
Article
Chemistry, Physical
Xiufang Hou, Weiyi Zhang, Quan-Song Li
Summary: Surface passivation by organic dyes is an effective strategy to improve the efficiency and stability of perovskite solar cells. The challenge lies in understanding how subtle structural changes in dyes lead to different passivation effects. In this study, three donor-pi-acceptor dyes (SP1, SP2, and SP3) with distinct electron donors were used to passivate the perovskite surface, resulting in varying efficiency and stability of the solar cells.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Anna Pomogaeva, Alexey Y. Timoshkin
Summary: The electronic structures and thermodynamic characteristics of hydroxy-substituted chain inorganic group 13-15 oligomers were investigated, showing that donor-acceptor interaction can effectively stabilize chain isomers and alter their electronic structure.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Editorial Material
Chemistry, Multidisciplinary
M. Rica Garcia, Inigo Iribarren, Isabel Rozas, Cristina Trujillo
Summary: This computational work investigates different binding modes of hydrogen bonds (HBs) between neighboring HB donors and acceptors in structures important in catalysis and biology. Substituted and unsubstituted HB donors were studied to analyze the electronic effect on the sigma-hole. Three binding modes were observed upon complexation: bifurcated, parallel, and zigzag. The strength of HBs follows the order of parallel > bifurcated > zigzag, which is consistent with experimental structures found in a search within the CSD.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Marianne Rica Garcia, Inigo Iribarren, Isabel Rozas, Cristina Trujillo
Summary: This computational work examines different hydrogen bond binding modes between neighboring donors and acceptors in structures relevant to catalysis and biology. Three binding modes were observed: bifurcated, parallel, and zigzag. It was found that the parallel pattern exhibits the strongest hydrogen bonds, followed by bifurcated and zigzag modes, leading to competition between the latter two. Experimental structures in the CSD showed similar patterns and trends. In conclusion, while acceptors determine the pattern and strength of hydrogen bond interactions, donors choose the type of binding within a particular dimer when multiple binding modes are possible.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Brigitte A. G. Lamers, Martin H. C. van Son, Freek de Graaf, Bart W. L. van den Bersselaar, Bas F. M. de Waal, Kazuki Komatsu, Hiroshi Sato, Takuzo Aida, Jose Augusto Berrocal, Anja R. A. Palmans, Ghislaine Vantomme, Stefan C. J. Meskers, E. W. Meijer
Summary: The assembly of highly ordered nanomaterials through charge transfer interactions is achieved in this study, where pyrene and naphthalenediimide functionalized oligodimethylsiloxanes are synthesized and co-assembled in bulk. By tuning the donor-acceptor interactions through connecting pyrene and NDI to the same oligomer or to two separate oligomers, different types of donor-acceptor molecules are obtained. The discreet length of the oligodimethylsiloxane units plays a crucial role in the formation of liquid crystalline materials and CT dimers.
MATERIALS HORIZONS
(2022)
Article
Chemistry, Multidisciplinary
Lakhya J. Mazumder, Amlan J. Kalita, Shahnaz S. Rohman, Chayanika Kashyap, Sabnam S. Ullah, Indrani Baruah, Ashapurna Boro, Ankur K. Guha, Pankaz K. Sharma
Summary: The study investigates unsupported donor-acceptor complexes of noble gases with group 13 elements using density functional theory. It finds that heavier noble gases can form thermodynamically stable compounds. The research suggests that prepyramidalization at the Lewis acid center may be an interesting alternative to stabilize these complexes, instead of requiring a rigid framework.
Article
Chemistry, Multidisciplinary
Paresh Kumar Majhi, Volker Huch, David Scheschkewitz
Summary: The synthesis and isolation of a stable potassium silagermenide compound with a Si=Ge bond as a suitable synthon for functional silagermenes has been reported. X-ray crystallographic analysis, UV/Vis spectroscopy, and DFT calculations confirmed a significant degree of pi-conjugation between N=C and Si=Ge double bonds in the compound.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Rosalyn L. Falconer, Gary S. Nichol, Ivan Smolyar, Scott L. Cockroft, Michael J. Cowley
Summary: This study presents a new class of organometallic compounds, dihydrodialanes supported by amidophosphine ligands. The ligand acts as a stereochemical reporter for reversible reductive elimination/oxidative addition chemistry involving Al-I and Al-III intermediates.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Applied
Alessandro Bismuto, Michael J. Cowley, Stephen P. Thomas
Summary: The hydroboration of alkynes and styrene using (B(C6F5)(3) has been developed, with the alkynes being activated by Lewis acid to form a reactive zwitterionic species. This species reacts with HBpin to give the desired alkenyl boronic ester. Additionally, the zwitterionic intermediate can act as a competent catalyst for the hydroboration of styrene.
ADVANCED SYNTHESIS & CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Paresh Kumar Majhi, Michael Zimmer, Bernd Morgenstern, David Scheschkewitz
Summary: A novel sesquimetallic complex containing a Si2Ge cyclopropene has been synthesized, showing a unique coordination mode where the sigma-component of the Ge = Si double bond acts as both a donor and acceptor, allowing for the formation of a nearly unsupported Si-Ge pi-bond. This complex can be easily modified and substituted with different functional groups, providing access to a variety of nickel complexes with high yields.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Inorganic & Nuclear
Andreas T. Kell, Naim M. Obeid, Prasenjit Bag, Michael Zimmer, Volker Huch, David Scheschkewitz
Summary: The regiodivergent reaction of phenylacetylene with various disilenes and bridged tetrasiladienes was studied, revealing that the regioselectivity of the [2+2] cycloaddition strongly depends on the nature of the substituent R. The presence of catalytic quantities of base suppresses cycloaddition in favor of the formal CH addition of phenylacetylene. Intermediacy of an alkynyl-substituted disilanyl lithium suggests a carbolithiation pathway for the net CH addition.
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
(2021)
Article
Chemistry, Inorganic & Nuclear
Thomas Buettner, Konstantin Weisshaar, Philipp Willmes, Volker Huch, Bernd Morgenstern, Rolf Hempelmann, David Scheschkewitz
Summary: The synthesis of p-methylthio-functionalized disilenes with (oligo)phenylene-linkers of different sizes was reported, with Si-29 NMR and UV/vis data suggesting that the linker-size only moderately affects the Si=Si moiety. Cyclic voltammetry showed an increasing number of reduction events with the number of phenylene rings, clearly associated with the oligo(phenylene) linking unit. Significant differences in the exchange current density of oxidation and reduction reactions were observed between the prepared disilenes using linear sweep voltammetry with a rotating disc electrode.
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
(2021)
Article
Chemistry, Inorganic & Nuclear
Marcel Lambert, Nadine E. Poitiers, Volker Huch, Andrea Goforth, David Scheschkewitz
Summary: The first silicon-carbon hybrid ladderanes with highly distorted ring systems and long silicon-carbon bridgehead bonds were obtained.
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
(2022)
Article
Chemistry, Multidisciplinary
Nadine E. Poitiers, Volker Huch, Bernd Morgenstern, Michael Zimmer, David Scheschkewitz
Summary: This study reports the growth of stable siliconoid clusters through a series of substitution, rearrangement, and reduction reactions with a single germanium atom. The findings are significant for understanding nucleation processes in gaseous and condensed phases.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Hanna Huebner, Bart-Jan Niebuur, Thomas Buettner, Marcus Koch, Bernd Stuehn, Tobias Kraus, David Scheschkewitz, Markus Gallei
Summary: This study characterizes the self-assembled structures of PDMSB-b-P2VP block copolymer in different solvents and evaluates its response to different solvents and temperatures. The influence of additional solvents, temperature, and ultrasonication on colloidal dispersion is investigated. Additionally, the introduction of surfactants in the solvent evaporation method leads to a plethora of additional colloidal structures.
Article
Chemistry, Inorganic & Nuclear
Marc Hunsicker, Nadine E. Poitiers, Volker Huch, Bernd Morgenstern, Michael Zimmer, David Scheschkewitz
Summary: A new potential model system for silicon monoxide has been synthesized by connecting an unsaturated silicon cluster with a polyhedral silsequioxane cage. The stoichiometry between silicon and oxygen in this model system is 14:12.
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
(2022)
Article
Chemistry, Multidisciplinary
Philipp Dabringhaus, Silja Zedlitz, Luisa Giarrana, David Scheschkewitz, Ingo Krossing
Summary: Schnockel's [(AlCp*)(4)] and Jutzi's [SiCp*][B(C6F5)(4)] are important in modern main-group chemistry with various applications in synthesis and catalysis. However, the reactivity between AlCp* and [SiCp*](+) has not been explored. In this study, their reaction was investigated and complex salts [Cp*Si(AlCp*)(3)][WCA] were obtained. The tetrahedral [SiAl3](+) core not only represents a rare example of a low-valent silicon-doped aluminium-cluster, but also provides a convenient preparative entry towards low-valent Si-Al clusters.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Taiki Imagawa, Luisa Giarrana, Diego M. Andrada, Bernd Morgenstern, Masaaki Nakamoto, David Scheschkewitz
Summary: By a series of addition and reduction reactions, the synthesis of a structurally rare silapyramidane compound was achieved from an amidinate-supported silylene and tetrakis(trimethylsilyl)cyclobutadiene as starting materials. The silapyramidane compound exhibited an unusually shielded 29Si NMR resonance at -448.3 ppm for the apex silicon atom. Treatment of the silapyramidane with Fe2(CO)9 resulted in the formation of the corresponding silapyramidane-iron complex. Moreover, the silapyramidane also underwent a reaction with the cyclobutadiene starting material to afford a fluorescent spirobis(silole) compound.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Philipp Grewelinger, Tim Wiesmeier, Carsten Praesang, Bernd Morgenstern, David Scheschkewitz
Summary: A straightforward synthesis of the first peraryl diboriranide was reported, demonstrating its preference for s-type coordination modes towards main group and transition metal centers. The synthesis involved the preparation of the non-classical diborirane from a readily available 1,2-dichlorodiborane(4) and subsequent conversion to the peraryl diboriranide lithium salt in three steps. Representative complexes with tin, copper, gold, and zinc were prepared and characterized to illustrate the reactivity and complexation behavior of the diboriranide.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Inorganic & Nuclear
Thomas Buettner, Oliver Janka, Volker Huch, Debabrata Dhara, Anukul Jana, David Scheschkewitz
Summary: In this study, a new single source chemical vapor deposition (CVD) method was developed for the synthesis of binary iron-germanium thin films. The technique allows for the preparation of uniform and dense Fe(x)G(e)y films under standard CVD conditions, without the need for harsh conditions.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Debabrata Dhara, David Scheschkewitz, Vadapalli Chandrasekhar, Cem B. Yildiz, Anukul Jana
Summary: The reactivity of isolable Au(i)-hydride stabilized by an NHC-coordinated diphosphene towards substrates containing C-C and N-N multiple bonds was reported. Different products were obtained in reactions with dimethyl acetylenedicarboxylate, azobenzene, ethyl diazoacetate, and phenyl acetylene, showing higher reactivity compared to a related NHC-stabilized Au(i)-hydride without the mediating diphosphene moiety.
CHEMICAL COMMUNICATIONS
(2021)
