Article
Chemistry, Inorganic & Nuclear
Konstantin V. Deriabin, Ekaterina A. Golovenko, Nikita S. Antonov, Sergey V. Baykov, Vadim P. Boyarskiy, Regina M. Islamova
Summary: A platinum polymer catalyst (Pt-PDMS) was synthesized by immobilizing a platinum catalytic complex in a polysiloxane chain using an azide-alkyne CuAAC cycloaddition. Insoluble Pt-PDMS can be used as an effective heterogeneous macrocatalyst for Si-O dehydrocoupling. Pt-PDMS is easy to recover, purify, and reuse again for heterogeneous catalysis.
DALTON TRANSACTIONS
(2023)
Correction
Chemistry, Organic
Adimulam Harinath, Himadri Karmakar, Devadkar Ajitaro Kisan, Hari Pada Nayek, Tarun K. Panda
Summary: This study reports a correction for the NHC-Zn alkyl catalyzed cross-dehydrocoupling of amines and silanes, and provides insights into the reaction mechanism.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
A. Babkin, A. A. Kissel, A. M. Ob'edkov, A. A. Trifonov
Summary: The Scandium tris(o-aminobenzyl) complex and its cationic derivative have been found to be effective catalysts for the dehydrocoupling of alkoxyarenes with aromatic hydrosilanes. The cationic derivative exhibits higher catalytic activity and substrate conversion compared to the neutral complex.
RUSSIAN CHEMICAL BULLETIN
(2022)
Review
Chemistry, Multidisciplinary
Brock E. Leland, Joydeb Mondal, Ryan J. Trovitch
Summary: This article explores the historical and recent efforts in catalyzing the dehydrocoupling of amines and silanes, a direct method for Si-N bond formation with hydrogen as a byproduct. The advantages of this transformation have driven the development of catalysts across the periodic table, leading to advances in efficiency and selectivity. The article highlights the formation of monomeric, oligomeric, and polymeric aminosilanes separately, and features a recent study on the manganese-catalyzed synthesis of perhydropolysilazane and commercial chemical vapor deposition precursors.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Matthew B. Reuter, Claire E. Bushey, Diego R. Javier-Jimenez, Rory Waterman
Summary: A family of commercially available organolithium compounds were found to catalyze the heterodehydrocoupling of silanes and amines under ambient conditions. The reaction exhibited high conversions and short reaction times, producing aminosilanes by coupling primary, secondary, and tertiary arylsilanes with electron-donating amines. The preliminary mechanistic analysis suggests a nucleophilic-type system involving the formation of a hypervalent silicon intermediate. Organolithium reagents are highlighted as straightforward and cost-effective precatalysts for this transformation.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Kosuke Iizuka, Yumiko Nakajima, Kazuhiko Sato
Summary: Heterolytic cleavage of a Si-H bond mediated by metal-ligand cooperation has been achieved. The reaction has been applied to the catalytic hydrosilylation of benzaldehyde and its derivatives, yielding the corresponding hydrosilylated products in moderate to good yields.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Matthew B. Reuter, Diego R. Javier-Jimenez, Claire E. Bushey, Rory Waterman
Summary: Group I alkoxides can serve as highly active catalysts for the heterodehydrocoupling of silanes and amines to produce aminosilane products. Commercially available KOtAmyl is commonly used as the benchmark precatalyst. Even challenging substrates such as anilines and alkyl triphenylsilanes can undergo high conversion coupling reactions with primary, secondary, and tertiary alkylsilanes under mild conditions.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Applied
Xin-Hua Peng, Rui Bai, Shanshan Liu, Zhuo Li, Lin-Yu Jiao
Summary: A novel and efficient protocol for the rare-earth metal salt-catalyzed substitution of phosphoryl azides with amines was disclosed. The methodology generated a series of phosphoryl amides, but secondary analogues or anilines were reluctant to undergo desired transformations.
APPLIED ORGANOMETALLIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Shanxuan Wu, Zijun Huang, Xiaolin Jiang, Fachao Yan, Yuehui Li, Chen-Xia Du
Summary: An efficient method using oxofluorovanadates as catalysts has been developed for the reductive amination of CO2, resulting in the transformation of various amines into N-formylated products in moderate to excellent yields at room temperature in the presence of phenylsilane. Mechanistic studies indicate a reaction pathway initiated through F-Si interactions, with activated phenylsilane allowing for CO2 insertion and subsequent formation of the target product through amine attack.
Article
Chemistry, Applied
Lara H. Polak, John B. Soltys, Kai C. Hultzsch
Summary: The intermolecular anti-Markovnikov hydroamination of vinylsilanes was successfully achieved using five silyl-substituted ortho-terphenoxide yttrium complexes, resulting in excellent activity and complete anti-Markonikov selectivity.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Mirela A. Farcas-Johnson, Sara H. Kyne, Ruth L. Webster
Summary: We describe the iron-catalyzed polymerizations of diol and silane monomers to obtain various poly(silylether) products. The reactions are simple and applicable to different types of silane and diol substrates. The obtained materials exhibit low T-g values and high thermal stability, with the use of 2 degrees silane leading to higher thermal stability compared to 1 degree silane.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Organic
Daniel Raydan, Sofia Friaes, Nuno Viduedo, A. Sofia Santos, Clara S. B. Gomes, Beatriz Royo, M. Manuel B. Marques
Summary: In this study, a wide variety of imines were synthesized through the oxidative coupling of alcohols and aromatic amines using Mn complexes as catalysts. The prepared imines exhibited excellent yields (up to 99%). The Mn-based catalysts proved to be highly efficient and versatile, enabling the synthesis of imines containing N-based heterocycles for the first time.
Article
Chemistry, Physical
Ziyin Kong, Weipeng Hu, James P. P. Morken
Summary: A Pt-catalyzed hydrosilylation reaction of (Z)-1,2-diborylethylene leads to the formation of a 1,2-diboryl-1-silylalkane, which can be used in catalytic cross-coupling reactions. Depending on the catalyst and the reaction conditions, the coupling can occur at either the α or β position relative to the silane center.
Article
Chemistry, Multidisciplinary
Liping Zhang, Teng Li, Xingchao Dai, Jian Zhao, Ce Liu, Dongcheng He, Kang Zhao, Peiqing Zhao, Xinjiang Cui
Summary: In this study, a Cu-Co double-atom catalyst was developed to significantly reduce the energy barrier of water activation and promote silane oxidation. The catalyst showed superior catalytic performance compared to single-atom catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Naroa Almenara, Maria A. Garralda, Xabier Lopez, Jon M. Matxain, Zoraida Freixa, Miguel A. Huertos
Summary: An unprecedented quantum tunneling effect has been observed in catalytic Si-H bond activations at room temperature. Both experimental and computational studies showed that quantum tunneling plays a crucial role in the catalytic process, affecting the activation energy and reaction rate significantly.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Thangavel Vijayakanth, David J. Liptrot, Ehud Gazit, Ramamoorthy Boomishankar, Chris R. Bowen
Summary: This article comprehensively reviews the application of piezo- and ferro-electric materials based on organic molecules and organic-inorganic hybrids in mechanical energy harvesting. The article describes the characterization of the piezo- and ferroelectric properties of these materials and highlights the advantages they have over traditional materials. It also discusses the potential of peptide-based and other biomolecular materials as alternative options. The article concludes with an analysis of the current limitations and future prospects in this field of research.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
Laura E. English, Matthew D. Jones, David J. Liptrot
Summary: An N-heterocyclic phosphine (NHP) has been investigated as a catalyst for transesterification reactions of commercial polymer samples, displaying high degradation activity towards poly(lactic acid) with methanol. However, attempts to depolymerise other polymers were unsuccessful, and NHP was found to form a new active catalyst under transesterification conditions.
Article
Chemistry, Multidisciplinary
Han-Ying Liu, Samuel E. Neale, Michael S. Hill, Mary F. Mahon, Claire L. McMullin, Emma Richards
Summary: Ionic compounds containing sodium cations are known for their stability and resistance to redox reactivity. However, when treated with non-reducible organic bases, a low oxidation state {Mg2Na2} species undergoes selective extrusion of sodium metal and oxidation of the Mg-I centers. Quantum chemical studies indicate that intramolecular electron transfer is facilitated by the molecular orbitals of the {Mg2Na2} ensemble.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Laura E. English, Thomas M. Horsley Downie, Catherine L. Lyall, Mary F. Mahon, Claire L. McMullin, Samuel E. Neale, Carla M. Saunders, David J. Liptrot
Summary: The (IPr)CuOtBu catalysed reduction of 11 aryl and alkyl isocyanates with pinacolborane resulted in the formation of boraformamides, pinBN(R)C(O)H, in most cases. Overreduction was observed only for electron poor aryl isocyanates (4-NC-C6H4NCO, 4-F3C-C6H4NCO, 3-O2N-C6H4NCO). Computational analysis revealed that the stability of [(IPr)CuH](2), proposed as the catalyst resting state, influences selectivity and offers a potential solution to prevent overreduction in future work. In the case of iPrNCO, the formation of [(IPr)CuH](2) prevents overreduction kinetically. However, for 4-NC-C6H4NCO, the barrier height for the first step of overreduction is much lower, resulting in unselective reduction.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Kyle G. G. Pearce, Michael S. S. Hill, Mary F. F. Mahon
Summary: Reaction of BeCl2 with dilithium diamide yields the dimeric chloroberyllate, leading to the formation of a 2-coordinate beryllium amide. Reduction of the beryllium amide using lithium or sodium in benzene produces relevant organoberyllate products, likely through transient Be(i) radicals.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Henry T. W. Shere, Michael S. Hill, Samuel E. Neale, Mary F. Mahon, Claire L. McMullin, Andrew S. S. Wilson
Summary: This article investigates the contrasting reactivities of molecular beta-diketiminato (BDI) calcium hydride and n-hexyl derivatives towards bis(pinacolato)diboron (B(2)pin(2)). The study finds that the dimeric calcium hydride forms an unusual diborane(6) dianion, while the initially dimeric organocalcium reagent converts to a calcium diboranate monomer. Attempts to induce heterolysis of the B-B bond in the calcium diboranate monomer were unsuccessful, resulting in either dismutation or the generation of N-donor adduct derivatives. These different reactivities can be explained by density functional theory (DFT) calculations, which attribute them to the larger radius and lower steric congestion of the third-row group 2 cation.
ZEITSCHRIFT FUR ANORGANISCHE UND ALLGEMEINE CHEMIE
(2023)
Article
Chemistry, Inorganic & Nuclear
Dawid J. J. Babula, Rex S. C. Charman, Thomas H. H. Jerome, Thomas M. Horsley M. Downie, Mary F. F. Mahon, David J. J. Liptrot
Summary: Sigma-bond metathesis reactions between [(6-Dipp)CuOtBu] and three diboranes resulted in the synthesis of three new copper(I) boryl complexes [(6-Dipp)CuBcat], [(6-Dipp)CuBneop], and [(6-Dipp)CuBhex]. While [(6-Dipp)CuBcat] and [(6-Dipp)CuBneop] formed rapidly, heating was required to obtain [(6-Dipp)CuBhex]. Crystallographic analysis revealed that all three complexes were monomers with distorted-linear structures at the copper atom. [(6-Dipp)CuBneop] exhibited comparable stability to [(IPr*)Cu-Bneop], remaining stable in solution for days without decomposition. [(6-Dipp)CuBhex] represents a rare example of a crystallographically characterized complex containing a boryl anion supported by a hexylene glycolato ligand.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Rex S. C. Charman, Josie A. Hobson, Ross A. Jackson, Mary F. Mahon, Samuel E. Neale, David J. Liptrot
Summary: In this study, two acyclic boryl complexes, (6-Dipp)CuB(OMe)2 and (6-Dipp)CuB(OMe)NMe2, were synthesized and their similar reactivities were demonstrated.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Inorganic & Nuclear
Han-Ying Liu, Mary F. Mahon, Michael S. Hill
Summary: The potassium diamidoalumanyl reacts with pinacolato boron esters and B(OMe) to produce potassium (alkoxy)borylaluminate derivatives. The reactivity of these derivatives with heteroallene molecules highlights the kinetic inaccessibility of their Al-B bonds.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Kyle G. Pearce, Chiara Dinoi, Ryan J. Schwamm, Laurent Maron, Mary F. Mahon, Michael S. Hill
Summary: This study investigates the formation of a series of calcium complexes, in which the orientation and hapticity of the aryl units are influenced by the position of the methyl substituent and steric hindrance. Additionally, an unusual reaction mechanism involving the generation of an intermediate dicalcium species and the polyhapto engagement of the aryl substituents with calcium is observed.
Article
Chemistry, Multidisciplinary
Sylwia Ostrowska, Pierre Arnaut, David J. Liptrot, Catherine S. J. Cazin, Steven P. Nolan
Summary: The synthesis, isolation, and full characterization of a new copper complex [Cu(IPr)(OC(H)(CF3)(2))] (IPr = 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidene) are reported. This copper(I) complex is a versatile synthon capable of activating various X-H bonds including C-H, N-H, and S-H bonds. [Cu(IPr)(OC(H)(CF3)(2))] was investigated as a pre-catalyst in several catalytic reactions.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ross A. A. Jackson, Aidan J. R. Matthews, Petra Vasko, Mary F. F. Mahon, Jamie Hicks, David J. J. Liptrot
Summary: The potassium aluminyl complex K-2[Al{N(Dipp)SiMe3}(2)](2) was synthesized, representing the first example of an aluminyl anion supported by an acyclic ligand framework. Attempts to form the same structure with a larger ligand framework resulted in C-H cleavage. K-2[Al{N(Dipp)SiMe3}(2)](2) behaved as a nucleophilic source of aluminum, forming a monomeric, acyclic magnesium aluminyl complex when reacted with an electrophilic b-diketiminate supported magnesium(II) iodide.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Han-Ying Liu, Samuel E. Neale, Michael S. Hill, Mary F. Mahon, Claire L. McMullin, Benjamin L. Morrison
Summary: [{SiNDipp}MgNa](2) reacts directly with H-2 to form a heterobimetallic hydride. Computational density functional theory (DFT) studies suggest that this reactivity is initiated by orbitally-constrained sigma(Mg-Mg)-> sigma*(H-H) and sigma(H-H) -> n*(Na(3s)) interactions between the frontier MOs of both H-2 and the tetrametallic core of [{SiNDipp}MgNa](2).
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Han-Ying Liu, Samuel E. Neale, Michael S. Hill, Mary F. Mahon, Claire L. McMullin
Summary: The copper(i) alumanyl derivative reacts with up to three equivalents of various terminal alkynes, resulting in the sequential formation of cuprous (hydrido)(alkynyl)aluminate, (alkenyl)(alkynyl)aluminate, and bis(alkynyl)aluminate derivatives. The alkene liberation process in the latter step is a unique case of alkyne transfer semi-hydrogenation.
Article
Chemistry, Inorganic & Nuclear
Rex S. C. Charman, Thomas M. Horsley Downie, Thomas H. Jerome, Mary F. Mahon, David J. Liptrot
Summary: Frustrated Lewis pairs (FLPs) are widely applied catalysts that can react with various substrates, including water, hydrogen, and phenylacetylene. The reactivity of a specific FLP, (6-Dipp)CuC(=(NBu)-Bu-t)Bpin, was explored through synthetic studies and characterization techniques.
Article
Chemistry, Multidisciplinary
Alexander M. Prophet, Kritanjan Polley, Gary J. Van Berkel, David T. Limmer, Kevin R. Wilson
Summary: The oxidation kinetics of iodide by ozone at the air-water interface is studied in single microdroplets. Molecular simulations and kinetic modeling are used to understand the underlying multiphase mechanism.
Article
Chemistry, Multidisciplinary
Rong Zhang, Jiajing Lan, Fei Wang, Shumei Chen, Jian Zhang
Summary: By utilizing 1,1'-ferrocene dicarboxylic acid as a chelating and surface protection ligand, we have synthesized multi-nuclear indium oxide clusters with varying nuclear sizes, including heptanuclear and thirteen-nuclear clusters. These clusters possess labile coordination sites, allowing for structural modification and self-assembly, resulting in the formation of various cluster structures.
Article
Chemistry, Multidisciplinary
Hui Wang, Hui Liu, Mingsen Wang, Jiaheng Hou, Yongjun Li, Yuancheng Wang, Yingjie Zhao
Summary: Two supramolecular complexes were prepared using CBs and M1, and their single-crystal structures were analyzed by SCXRD. The unexpected 1:2 self-assembly structure between M1 and CB[8] was discovered for the first time. These complexes exhibit unique photophysical properties and provide valuable information about the structure and photophysical properties of supramolecular complexes.
Article
Chemistry, Multidisciplinary
Chang-Hee Lee, Sookil Park, Sanggil Kim, Ji Young Hyun, Hyun Soo Lee, Injae Shin
Summary: The epidermal growth factor receptor (EGFR) is a cell-surface glycoprotein involved in cell proliferation and tumor development. This study used a fluorescently labeled EGFR to investigate its time-dependent endocytosis in live cells and found that appended glycans affect EGFR internalization. Additionally, the study detected sialic acid residues attached to EGFR on the live cell surface using FRET-based imaging. This research provides valuable insights into the cellular functions of EGFR.
Article
Chemistry, Multidisciplinary
Subhankar Sahu, Lokesh Kumar, Sumita Das, Dipti Gupta, Ruchi Anand
Summary: This study proposes a strategy that combines organic electronics with biosensor scaffolds to create a compact device for monitoring environmental aromatic pollution. By coupling biosensing protein MopR with an organic electrochemical transistor (OECT), a sensor module capable of efficient detection of phenol was designed. Exclusive phenol detection with minimal loss of sensitivity could be achieved in complex pollutant mixtures and real environmental samples.
Review
Chemistry, Multidisciplinary
Changseok Lee, Hyung-Joon Kang, Sungwoo Hong
Summary: The formation of C-N bonds through hydroamination reactions catalyzed by nickel hydrides has been a topic of recent interest. This approach offers a way to efficiently transform a variety of alkene and alkyne substrates into compounds enriched with C-N bonds. The review provides a concise overview of the underlying reaction mechanisms and aims to stimulate further progress in NiH-catalytic techniques and catalyst design.
Article
Chemistry, Multidisciplinary
Yueci Wu, Lu-Lu Sun, Hai-Hao Han, Xiao-Peng He, Weiguo Cao, Tony D. James
Summary: Drug-induced liver injury (DILI) is a common cause of acute liver failure in the USA and Europe, but most cases can be recovered or prevented by discontinuing the offending drug. Recent research has found that peroxynitrite (ONOO-) can be used as a potential indicator for early diagnosis of DILI, and there is an urgent need to establish a method to detect and track peroxynitrite in DILI cases. In this study, a FRET-based nano fluorescent probe CD-N-I was developed, which showed high selectivity and sensitivity in detecting peroxynitrite. The probe successfully detected exogenous peroxynitrite in live cells and endogenous peroxynitrite in APAP-induced liver injury of HepG2 cells.
Article
Chemistry, Multidisciplinary
Dmitry L. Lipilin, Mikhail O. Zubkov, Mikhail D. Kosobokov, Alexander D. Dilman
Summary: This article describes a direct photocatalytic method for the thiolation of unprotected acids, which was previously challenging. By using a thionocarbonate reagent with an N-O bond, the efficient conversion of carboxylic acids to thiols is achieved.
Article
Chemistry, Multidisciplinary
Jason Malenfant, Lucille Kuster, Yohann Gagne, Kouassi Signo, Maxime Denis, Sylvain Canesi, Mathieu Frenette
Summary: Raman microscopy can reveal compound-specific vibrational fingerprints without sample preparation. The combination of efficient theoretical calculations and a user-friendly software can accurately predict peak positions and provide match scores to assist with structure determination.
Article
Chemistry, Multidisciplinary
Jayoh A. Hernandez, Paul S. Micus, Sean Alec Lois Sunga, Luca Mazzei, Stefano Ciurli, Gabriele Meloni
Summary: Essential trace metals play crucial roles in the survival and virulence of bacterial pathogens. Helicobacter pylori requires nickel for colonization and persistence in the stomach, and NixA is an essential nickel transporter in this process. This study characterizes the selectivity and electrogenic nature of NixA-mediated nickel transport.
Article
Chemistry, Multidisciplinary
Tarali Devi, Kuheli Dutta, Jennifer Deutscher, Stefan Mebs, Uwe Kuhlmann, Michael Haumann, Beatrice Cula, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: This study emphasizes the importance of subtle electronic changes and secondary interactions in the stability of biologically relevant metal-dioxygen intermediates. It also shows that the role of the chloride ligand in stabilizing the Fe-III-(OOBu)-Bu-t moiety can extend to other anions, including the thiolate ligand.
Article
Chemistry, Multidisciplinary
Jacqueline R. Santhouse, Jeremy M. G. Leung, Lillian T. Chong, W. Seth Horne
Summary: By studying the folding kinetics and mechanism of the BdpA sequence, researchers found that altering the backbone connectivity can affect protein folding. This suggests that protein mimetic chains have a significant degree of plasticity in transitioning between unfolded and folded states.
Article
Chemistry, Multidisciplinary
Divanshu Gupta, Ralf Einholz, Holger F. Bettinger
Summary: This study presents the first direct spectroscopic evidence of a cyclic seven-membered iminoborane. Compared to linear amino-iminoboranes, this cyclic iminoborane exhibits weakened bond strength and lower Lewis acidity value. The study suggests that the reduced ring strain of cyclic iminoborane prevents nitrogen fixation but allows facile (2 + 2) cycloaddition reaction with C2H4.
Article
Chemistry, Multidisciplinary
Renny Mathew, Aniruddha Mazumder, Praveen Kumar, Julie Matula, Sharmarke Mohamed, Petr Brazda, Mahesh Hariharan, Brijith Thomas
Summary: This study reveals the packing arrangement of partially disordered nitro-perylenediimide (NO2-PDI) using a synergistic approach that combines 3D ED, ssNMR, and DFT techniques. By overcoming these challenges, this methodology opens up new avenues for material characterization, driving exciting advancements in the field.