Article
Chemistry, Physical
Benedikt Soeldner, Kristof Grohe, Peter Neidig, Jelena Auch, Sebastian Blach, Alexander Klein, Suresh K. Vasa, Lars V. Schaefer, Rasmus Linser
Summary: Understanding macromolecular function, interactions, and stability requires detailed assessment of conformational ensembles. Limited by the qualitative or low abundance of solid-state nuclear magnetic resonance internuclear distance information, accurately elucidating the spatial dynamics of solid proteins at physiological temperatures is challenging. However, this study demonstrates unprecedented access to abundant proton-proton internuclear distances, enabling accurate molecular dynamics simulations and providing atomic-level spatial details of conformational dynamics in various biomolecular systems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Feng Shi, Lili Hu, Yun Cui, Jinjun Ren
Summary: Glasses in the xLa(2)O(3)-yAl(2)O(3)-(100 - x - y)NaPO3 system were synthesized and characterized using advanced multinuclei solid-state nuclear magnetic resonance spectroscopy and X-ray photoelectron spectroscopy. The study revealed that the depolymerization of the glass Q(2) structure by La2O3 and Al2O3 resulted in the formation of multiple phosphorus species. La coordination number was predominantly nine, with some La atoms transitioning to lower coordination with the addition of Al2O3, and the connection methods between Al/P and La/P were found to be different.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Polymer Science
Stepan A. Ostanin, Maxim Mokeev, Dmitry Pikhurov, Aleksandr S. Sakhatskii, Vjacheslav V. Zuev
Summary: Aromatic-oxyaliphatic polyurethanes were synthesized with varying mass fractions of components, including fluorinated fragments, and their rigid domains were found to be formed by units containing urethane bonds as well as oxyethylene fragments. The urethane bonds and oxyethylene fragments were incorporated into both rigid and soft phases, showing good agreement with the Cooper and Tobolsky model under specific solubility parameters for different segments.
Article
Energy & Fuels
Francesco Panattoni, Jonathan Mitchell, Edmund J. Fordham, Ravinath Kausik, Clare P. Grey, Pieter C. M. M. Magusin
Summary: The study utilized high-field, solid-state NMR methods to analyze kerogen isolates of different maturity levels, finding that the aromatic/aliphatic ratio of kerogen increases with maturity. This increase in ratio is reflected in the H-1 MAS NMR spectra by the intensity ratio of aliphatic-to-aromatic signals, suggesting a decrease in kerogen proton density during maturation.
Review
Biochemistry & Molecular Biology
Vitaly Volkov, Alexander Chernyak, Nikita A. Slesarenko, Irina A. Avilova
Summary: This review focuses on the progress of solvation and mobility studies in solid electrolyte, particularly ion-exchange membranes and composite materials, using NMR techniques. The applications of various NMR techniques are discussed, and comparisons are made between diffusion coefficients and ionic conductivity data. The microscopic mechanism of ionic transfer is also explored.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2022)
Article
Materials Science, Paper & Wood
Darren H. Brouwer, Janelle G. Mikolajewski
Summary: Solid-state 13C nuclear magnetic resonance (NMR) spectroscopy is an important tool for identifying different forms of cellulose. In this paper, the authors show that the secondary crystalline form in bacterial cellulose differs from the I beta allomorph found in tunicate cellulose, based on their analysis of 1D and 2D NMR spectra.
Review
Chemistry, Multidisciplinary
Sahil Ahlawat, Kaustubh R. Mote, Nils-Alexander Lakomek, Vipin Agarwal
Summary: In the past two decades, solid-state nuclear magnetic resonance (ssNMR) spectroscopy has evolved from investigating small molecules and industrial polymers to decrypting complex biological systems. This transformation is due to improvements in hardware design, sample preparation, and sensitivity. This review discusses state-of-the-art ssNMR methods and recent developments in signal filtering, proton methodologies, and data acquisition speed in fast magic-angle spinning (MAS) systems.
Article
Chemistry, Physical
Clayton J. Dahlman, Rhys M. Kennard, Piotr Paluch, Naveen R. Venkatesan, Michael L. Chabinyc, G. N. Manjunatha Reddy
Summary: Layered hybrid organic-inorganic perovskites, such as the lead halide Ruddlesden-Popper (RP) series, exhibit tunable optoelectronic properties due to dynamic interactions between the ionic perovskite substructure and organic spacer cations. Solid-state NMR spectroscopy was used to characterize the static and dynamic structures of linear alkylammonium and aromatic spacers in lead iodide RP phases, revealing different site-specific rigidity trends for short and long spacers. The study highlights the interplay between spacer interactions with lead iodide octahedra and van der Waals forces in contributing to a variety of site-specific dynamics and structural distortions at intermediate time scales.
CHEMISTRY OF MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Binayak Roy, Urbi Pal, Ankita Bishnoi, Luke A. O'Dell, Pratibha Sharma
Summary: Solid-state H-1-N-14(OT) HMQC, B-11 MQMAS and H-1-B-11 HETCOR NMR experiments were used to investigate the role of homopolar B-B interaction in the thermal dehydrogenation of pure and supported ammonia borane. The study also addressed the subtlety of homopolar interactions in amine borane compounds and their differences from heteropolar interactions.
CHEMICAL COMMUNICATIONS
(2021)
Article
Materials Science, Multidisciplinary
M. Arbel-Haddad, Y. Harnik, Y. Schlosser, A. Goldbourt
Summary: Geopolymers are a promising option for immobilizing nuclear waste, particularly radioactive cesium. The study found that cesium ions preferentially bind to zeolite F, and zeolite F is more efficient in immobilizing cesium compared to other crystalline or amorphous phases.
JOURNAL OF NUCLEAR MATERIALS
(2022)
Article
Chemistry, Physical
Gabrielle E. Harmon-Welch, John C. Hoefler, Martha R. Trujillo, Nattamai Bhuvanesh, Vladimir I. Bakhmutov, Janet Blumel
Summary: Ferrocene and nickelocene do not react with each other in solution, but the paramagnetic component affects the 1H NMR signal of ferrocene. It has been found that co-crystallization of ferrocene and nickelocene can occur without a solvent, and the two substances crystallize in the same space group. Furthermore, when exposed to polycrystalline nickelocene, ferrocene single crystal forms a mixed crystal with nickelocene migrating into its lattice. The migration of one organometallic component into the crystal lattice of another has not been described previously.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Claire Welton, Parth Raval, Julien Trebosc, G. N. Manjunatha Reddy
Summary: Chemically assisted swapping of labile protons by deuterons is demonstrated for amino acids, polysaccharides, pharmaceutical compounds, and their solid formulations. Solid-state packing interactions in these compounds are investigated using H-1-H-2 isotope correlation NMR spectroscopy (iCOSY). A minute concentration of dopamine, 5 wt% or approximately 100 μg, in a solid formulation can be detected by H-2 NMR at 28.2 T (H-1, 1200 MHz) in under a minute.
CHEMICAL COMMUNICATIONS
(2022)
Article
Pharmacology & Pharmacy
Peter I. I. I. J. G. Remoto, Karlis Berzins, Sara J. Fraser-Miller, Timothy M. Korter, Thomas Rades, Jukka Rantanen, Keith C. Gordon
Summary: The solid-state landscape of carbamazepine during dehydration was investigated using both low- (-300 to -15, 15 to 300 cm(-1)) and mid- (300 to 1800 cm(-1)) frequency Raman spectroscopy. Density functional theory with periodic boundary conditions was employed to characterize the carbamazepine dihydrate and different forms, which showed good agreement with experimental Raman spectra. The dehydration process of carbamazepine dihydrate at various temperatures (40, 45, 50, 55, and 60 ?) was explored using principal component analysis and multivariate curve resolution, revealing different transformation pathways of solid-state forms. Low-frequency Raman spectroscopy was found to effectively detect the rapid growth and subsequent decline of carbamazepine form IV, which was not as well observed by mid-frequency Raman spectroscopy. These findings highlight the potential benefits of low-frequency Raman spectroscopy in pharmaceutical process monitoring and control.
Article
Chemistry, Multidisciplinary
Linda Cerofolini, Kristian Vasa, Elisa Bianconi, Maria Salobehaj, Giulia Cappelli, Alice Bonciani, Giulia Licciardi, Anna Perez-Rafols, Luis Padilla-Cortes, Sabrina Antonacci, Domenico Rizzo, Enrico Ravera, Caterina Viglianisi, Vito Calderone, Giacomo Parigi, Claudio Luchinat, Antonio Macchiarulo, Stefano Menichetti, Marco Fragai
Summary: Several protein-drug conjugates are currently used in cancer therapy, relying on covalently attached cytotoxic organic compounds or non-covalent interactions. Human transthyretin (TTR) has been identified as a potential carrier protein for cytotoxic drug delivery. This study demonstrates the importance of integrating multiple biophysical and structural techniques, such as microscale thermophoresis, X-ray crystallography, and NMR. Solid-state NMR is particularly valuable in revealing ligand binding effects and their impact on macromolecular complex stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
ShengQi Xiang, Cecilia Pinto, Marc Baldus
Summary: Membrane proteins play important biological roles by forming complexes in cell membranes. This study focuses on understanding the role of the lipoprotein BamC in the assembly of the beta-barrel assembly machinery (BAM) complex in lipid bilayers. By developing a selective preparation scheme and using proton-detected solid-state NMR methods, the researchers were able to investigate the structure and dynamics of BamC embedded in the entire BAM complex in lipid bilayers. This approach provides insights into the formation and functioning of membrane protein complexes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Sami El Sayed, Alexis Bordet, Claudia Weidenthaler, Walid Hetaba, Kylie L. Luska, Walter Leitner
Review
Chemistry, Applied
Claudia Weidenthaler
JOURNAL OF ENERGY CHEMISTRY
(2020)
Editorial Material
Multidisciplinary Sciences
Amol P. Amrute, Zbigniew Lodziana, Hannah Schreyer, Claudia Weidenthaler, Ferdi Schueth
Article
Chemistry, Physical
Michael Hirscher, Volodymyr A. Yartys, Marcello Baricco, Jose Bellosta von Colbe, Didier Blanchard, Robert C. Bowman, Darren P. Broom, Craig E. Buckley, Fei Chang, Ping Chen, Young Whan Cho, Jean-Claude Crivello, Fermin Cuevas, William I. F. David, Petra E. de Jongh, Roman Denys, Martin Dornheim, Michael Felderhoff, Yaroslav Filinchuk, George E. Froudakis, David M. Grant, Evan MacA Gray, Bjorn C. Hauback, Teng He, Terry D. Humphries, Torben R. Jensen, Sangryun Kim, Yoshitsugu Kojima, Michel Latroche, Hai-Wen Li, Mykhaylo Lototskyy, Joshua W. Makepeace, Kasper T. Moller, Lubna Naheed, Peter Ngene, Dag Noreus, Magnus Moe Nygard, Shin-ichi Orimo, Mark Paskevicius, Luca Pasquini, Dorthe B. Ravnsbaek, M. Veronica Sofianos, Terrence J. Udovic, Tejs Vegge, Gavin S. Walker, Colin J. Webb, Claudia Weidenthaler, Claudia Zlotea
JOURNAL OF ALLOYS AND COMPOUNDS
(2020)
Article
Chemistry, Physical
Tatiana Priamushko, Remy Guillet-Nicolas, Mingquan Yu, Matthew Doyle, Claudia Weidenthaler, Harun Tueysuez, Freddy Kleitz
ACS APPLIED ENERGY MATERIALS
(2020)
Article
Electrochemistry
Daniel Jalalpoor, Daniel Goehl, Paul Paciok, Marc Heggen, Johannes Knossalla, Ivan Radev, Volker Peinecke, Claudia Weidenthaler, Karl J. J. Mayrhofer, Marc Ledendecker, Ferdi Schueth
Summary: The study shows that the interaction between platinum nanoparticles supported on antimony-doped tin oxide affects the catalytic performance of platinum, reducing the accessible surface area of platinum.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Applied
Hrishikesh Joshi, Cristina Ochoa-Hernandez, Edward Nuerenberg, Liqun Kang, Feng Ryan Wang, Claudia Weidenthaler, Wolfgang Schmidt, Ferdi Schueth
MICROPOROUS AND MESOPOROUS MATERIALS
(2020)
Article
Chemistry, Physical
Moritz O. Haus, Alexander Meledin, Sebastian Leiting, Yannik Louven, Nico C. Roubicek, Sven Moos, Claudia Weidenthaler, Thomas E. Weirich, Regina Palkovits
Summary: This study extensively compares the synthesis protocols and materials of Pt-Re bimetallic catalysts, revealing common features like Pt-0 nanoparticles and partially reduced Re species. Differences in active site numbers and Re reduction extent affect catalytic performance, with the optimal catalyst outperforming a previous benchmark in the reduction of N-(2-hydroxyethyl)succinimide.
Article
Chemistry, Multidisciplinary
Alexander Bodach, Thomas Bernert, Michael Fischer, Morten Brix Ley, Claudia Weidenthaler
Summary: Dehydrocoupling of the dimethylamine and borane adduct, NH(CH3)(2)-BH3, leads to dimethylaminoborane with a composition of NH(CH3)(2)-BH3. The structure of the product depends on synthesis conditions, crystallizing either as a trimer with a six-membered ring or as a dimer with a four-membered ring. The triclinic structure is stable at low temperatures, but heating can cause a phase transition to a monoclinic polymorph, with crystal structure determined in this study.
ACTA CRYSTALLOGRAPHICA SECTION B-STRUCTURAL SCIENCE CRYSTAL ENGINEERING AND MATERIALS
(2021)
Article
Chemistry, Physical
Oliver Wetzel, Shabnam Hosseini, Kateryna Loza, Marc Heggen, Oleg Prymak, Peter Bayer, Christine Beuck, Torsten Schaller, Felix Niemeyer, Claudia Weidenthaler, Matthias Epple
Summary: Ultrasmall silver nanoparticles were prepared through reduction and surface modification, with NMR analysis indicating a small hydrodynamic diameter and XPS showing binding of silver to GSH. XRD confirmed a twinned fcc structure. The nanoparticles exhibited strong cytotoxicity in cell culture and a stoichiometry of Ag(about 250)GSH(about 155).
JOURNAL OF PHYSICAL CHEMISTRY B
(2021)
Article
Chemistry, Inorganic & Nuclear
Hilke Petersen, Niklas Stegmann, Michael Fischer, Bodo Zibrowius, Ivan Radev, Wladimir Philippi, Wolfgang Schmidt, Claudia Weidenthaler
Summary: Transition-metal phosphates have a wide range of applications and can be used as catalysts, battery materials, and fuel cell membranes. This study successfully determined the structures of two novel titanium pyrophosphates using experimental data, and found that these compounds exhibit good conductivity and potential for electrochemical device applications.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Bodo Zibrowius, Michael Fischer
Summary: The quadrupole coupling constants and asymmetry parameters of two complex aluminium hydrides were determined using Al-27 NMR spectra recorded for stationary samples with the Solomon echo sequence. The results for KAlH4 and NaAlH4 agreed well with previous MAS NMR spectra data. The accuracy of static spectra determination was found to be comparable to the MAS approach. Comparisons were made with DFT-GIPAW calculations, showing excellent agreement except for one parameter being overestimated in the calculations.
Article
Chemistry, Multidisciplinary
Ezgi Onur Sahin, Harun Tueysuez, Candace K. Chan, Gun-hee Moon, Yitao Dai, Wolfgang Schmidt, Joohyun Lim, Christina Scheu, Claudia Weidenthaler
Summary: The structural evolution of tantalum-based oxides was studied from the formation of hydrolysed clusters to temperature-induced crystallisation processes, providing insight on the connectivity, arrangement, and size of clusters as well as the transformation into crystalline orthorhombic L-Ta2O5 without intermediate structures.
Article
Chemistry, Physical
Bodo Zibrowius, Michael Felderhoff
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2019)
Article
Chemistry, Inorganic & Nuclear
Yunxiang Qiao, Nils Theyssen, Bernd Spliethoff, Jan Folke, Claudia Weidenthaler, Wolfgang Schmidt, Gonzalo Prieto, Cristina Ochoa-Hernandez, Eckhard Bill, Shengfa Ye, Holger Ruland, Ferdi Schueth, Walter Leitner
Summary: Sheet silicates, such as talc and pyrophyllite, contain parallel sheets of tetrahedral silicate, with the ferric analogue being rarely found in nature and synthetic protocols for purely iron-based pyrophyllite yet to be published. This study reports the first artificial synthesis of ferripyrophyllite under exceptional mild conditions, showing high thermostability and catalytic activity in ammonia synthesis.
DALTON TRANSACTIONS
(2021)
