Article
Biochemical Research Methods
Jaekyun Jeon, C. Blake Wilson, Wai-Ming Yau, Kent R. Thurber, Robert Tycko
Summary: This article reviews recent developments in the experimental approach to characterizing transient intermediate states in biomolecular processes. This approach relies on solid state nuclear magnetic resonance (ssNMR) measurements at very low temperatures, enhanced by dynamic nuclear polarization (DNP). It also involves novel technologies for initiating and freezing the process of interest quickly. Recent applications include studying the formation of a complex between calmodulin and its target protein, as well as the conversion of the bee venom peptide melittin from an unstructured monomeric state to a helical, tetrameric state. Future applications of millisecond time-resolved ssNMR are also briefly discussed.
JOURNAL OF MAGNETIC RESONANCE
(2022)
Article
Biochemistry & Molecular Biology
Anna Helena Mazurek, Lukasz Szeleszczuk, Kostas Bethanis, Elias Christoforides, Marta Katarzyna Dudek, Monika Zielinska-Pisklak, Dariusz Maciej Pisklak
Summary: In this study, the host-guest inclusion complex between ss-CD and EST was prepared using four different methods, and the obtained samples were deeply characterized. The crystal structure of the complex was determined using SCXRD, which is the first solved crystal structure of an estrogen/CD complex to our knowledge. Periodic DFT calculations using GIPAW were found to be particularly helpful in analyzing disorder in the solid state and interpreting experimental NMR results. This study highlights the importance of a combined ssNMR/SCXRD approach to studying the structure of inclusion complexes formed by cyclodextrins.
Article
Chemistry, Multidisciplinary
Mattia Negroni, Dennis Kurzbach
Summary: A method for real-time NMR of 'hyperpolarized' proteins at residue resolution is proposed using dissolution dynamic nuclear polarization. This approach enables selective detection of hyperpolarized residues, addressing limitations in sensitivity and monitoring speed in protein NMR spectroscopy. Hyperpolarization of solvent and subsequent transfer to target molecules significantly enhances signal in protein NMR, allowing for residue-resolved spectra recording at a high sampling rate.
COMMUNICATIONS CHEMISTRY
(2021)
Article
Chemistry, Physical
Chuanyu Yan, Enzo Moretto, Oussema Kachouri, Jean-Luc Biagi, Jean-Sebastien Thomann, Francois Kayser, Reiner Dieden
Summary: This study demonstrates the use of solid-state nuclear magnetic resonance spectroscopy for studying dehydration and deuterium exchange at the liquid-solid interface. The results provide evidence of complete removal of physically adsorbed water molecules on the silica surface in the presence of DMSO, and satisfactory deuteration of silanol groups in the presence of a DMSO-D2O mixture. Additionally, the study develops a liquid-state NMR-based technique for quantifying moisture and hydroxyls on solids.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2022)
Article
Chemistry, Physical
Stephan N. Steinmann, Carine Michel
Summary: Reactions at the water/solid interface are crucial for sustainable processes. In the past decade, modeling approaches, such as polarisable continuum models and microsolvation, have improved our understanding of these reactions. Efforts are being made to achieve a full atomistic description of the water/liquid interface.
Article
Chemistry, Physical
Ren-Hao Cheng, Honghao Cai, Yu-Ren Huang, Xiaohong Cui, Zhong Chen, Hsuan-Ying Chen, Shangwu Ding
Summary: Understanding the water state in Nafion is crucial for fuel cell operation and proton transport mechanism elucidation. By designing different types of Nafion samples with substituted cations, preparing samples carefully, and conducting solid state NMR experiments, clear and straightforward information can be obtained to reduce ambiguity in interpreting data. The results show that the type of substituting cation affects the unfrozen water in Nafion, and there is a broad distribution of water state and dynamics as the temperature decreases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2021)
Article
Chemistry, Multidisciplinary
Gordon Agbenyegah, Joshua P. Clark, John Hanna, Margaret Hyland, James B. Metson, Grant McIntosh, Ronny Etzion, Graham A. Bowmaker, Zoran Zujovic
Summary: The fluorination mechanism of low-level fluorinated materials obtained by calcination of Bayer gibbsite at different temperatures was studied using 27Al and 19F solid-state NMR spectroscopy and X-ray diffraction. Different types of Al-F species on the surface of fluorinated gibbsite were proposed based on 19F magic angle spinning (MAS) NMR spectra, showing distinct peaks at various ppm values. The fluorination process in aluminas involves elementary exchange reactions where F- replaces surface -OH groups, confirmed by 27Al MAS NMR and 19F-27Al cross-polarization-MAS experiments.
JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
(2022)
Article
Chemistry, Applied
Mustapha El Hariri El Nokab, Alessia Lasorsa, Khaled O. Sebakhy, Francesco Picchioni, Patrick C. A. van der Wel
Summary: Alginate hydrogels are versatile materials with diverse applications in biomedicine and food industry. The formation of hydrogel involves cross-linking with calcium ions and hydration of alginate groups. Solid-state NMR spectroscopy is used to detect and study water molecules in re-hydrated alginate hydrogels, revealing the different water phases and the effects of calcium cross-linking on water-filled macropores.
FOOD HYDROCOLLOIDS
(2022)
Article
Chemistry, Analytical
Olivier Devos, Mahdiyeh Ghaffari, Raffaele Vitale, Anna de Juan, Michel Sliwa, Cyril Ruckebusch
Summary: The study introduces a multivariate curve resolution method based on data slicing, allowing tailored and fit-free analysis of multiexponential fluorescence decay curves. This approach enables the recovery of individual components with decay profiles that are only partially describable by monoexponential functions, and can extract fluorescence lifetime information accurately.
ANALYTICAL CHEMISTRY
(2021)
Article
Engineering, Biomedical
Yannick Coppel, Yann Prigent, Genevieve Gregoire
Summary: This study introduces a set of solid state NMR experiments for characterizing the main components of human dentin, focusing on the H-1 signals of water molecules, HPO42-, and OH- groups. By utilizing sample modifications, hydrogen signals of these species can be distinguished, providing valuable structural and dynamic information for biomaterials.
ACTA BIOMATERIALIA
(2021)
Article
Chemistry, Multidisciplinary
Alexander V. Yakimov, Manoj Ravi, Rene Verel, Vitaly L. Sushkevich, Jeroen A. van Bokhoven, Christophe Coperet
Summary: This study investigates the structures of Brosted acid sites and Lewis acid sites in Zeolite and their interactions with pyridine using NMR spectroscopy and DFT modeling. The study reveals the temperature-dependent variations of the structures and emphasizes the importance of considering temperature effects in obtaining accurate structural assessments.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Thomas Pigeon, Gabriel Stoltz, Manuel Corral-Valero, Ani Anciaux-Sedrakian, Maxime Moreaud, Tony Lelievre, Pascal Raybaud
Summary: In this study, a method for computing accurate rate constants for catalytic events at surface was proposed. The method combined adaptive multilevel splitting (AMS) rare event sampling technique and ab initio molecular dynamics. Various approaches were used to build reaction coordinates, and a case study on the conformation change and dissociation of water molecule on γ-alumina (100) surface was conducted to evaluate the proposed method. The calculated rate constants and transition mechanisms were compared with the results obtained from a conventional static approach. It was found that the AMS method can provide rate constants smaller by up to 2 orders of magnitude due to entropic effects.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Fumitoshi Kumaki, Masanari Nagasaka, Ryo Fukaya, Yasuaki Okano, Shohei Yamashita, Shunsuke Nozawa, Shin-ichi Adachi, Jun-ichi Adachi
Summary: Operando time-resolved soft x-ray absorption spectroscopy (TR-SXAS) is used to study photochemical processes of metal complexes in solutions. In this study, a TR-SXAS measurement system is developed using laser pump pulses and soft x-ray probe pulses. The system is evaluated by measuring iron phenanthroline solutions during a photoinduced spin transition process.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Jacopo De Bellis, Cristina Ochoa-Hernandez, Christophe Fares, Hilke Petersen, Jan Ternieden, Claudia Weidenthaler, Amol P. Amrute, Ferdi Schueth
Summary: A straightforward methodology to synthesize tohdite nanopowders was developed, and comprehensive characterization of the material was conducted using various techniques, providing further insights into its properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
Michael J. Jaroszewicz, Mengxiao Liu, Jihyun Kim, Guannan Zhang, Yaewon Kim, Christian Hilty, Lucio Frydman
Summary: Nuclear magnetic resonance (NMR) spectroscopy provides detailed information about dynamic processes through line-shape changes under equilibrium conditions. However, studying chemical reactions under off-equilibrium conditions and monitoring the reactants and products in real time can provide additional valuable information. In this study, the authors propose and demonstrate a time-resolved kinetic NMR experiment that combines rapid mixing techniques, continuous flow, and single-scan spectroscopic imaging methods, leading to a 2D spectrotemporal NMR correlation that provides high-quality kinetic information of off-equilibrium chemical reactions.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Rick W. Dorn, Lesli O. Mark, Ivan Hung, Melissa C. Cendejas, Yijue Xu, Peter L. Gor'kov, Wenping Mao, Faysal Ibrahim, Zhehong Gan, Ive Hermans, Aaron J. Rossini
Summary: In this study, the atomistic structure of boron oxide/hydroxide catalyst supported on oxidized activated carbon (B/OAC) was determined using the 35.2 T B-11 and O-17 solid-state NMR experiments. The catalyst shows comparable activity and selectivity to boron nitride in the oxidative dehydrogenation (ODH) of propane. The approach used in this study can be generally applied to determine the atomistic structures of heterogeneous catalysts containing quadrupolar nuclei.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Ieva Goldberga, Nicholai D. Jensen, Christele Combes, Frederic Mentink-Vigier, Xiaoling Wang, Ivan Hung, Zhehong Gan, Julien Trebosc, Thomas-Xavier Metro, Christian Bonhomme, Christel Gervais, Danielle Laurencin
Summary: This study investigates the possibility of enriching O-17 isotopes in water molecules within hydrated biominerals using liquid assisted grinding. The results show that the labelled water molecules are mainly located at the core of the crystal structures and can enter the lattice through dissolution/recrystallization or diffusion. This work highlights the importance of high-resolution O-17 NMR in understanding the roles of water as a grinding agent and as a reagent for isotopic enrichment.
FARADAY DISCUSSIONS
(2023)
Article
Engineering, Chemical
Changshun Deng, Kai Wang, Xiaofeng Qian, Jun Yao, Nianhua Xue, Luming Peng, Xuefeng Guo, Yan Zhu, Weiping Ding
Summary: We report a green oxidation method for the conversion of toluene to benzaldehyde using air under mild conditions with over 99% selectivity at 35% conversion and 180 degrees C. Previous studies have made little progress in this important reaction, with low selectivity or conversion. In this work, a modified catalytic system using 1 MPa of air as an oxidant and optimized catalytic center is developed, which shows realistic feasibility for high-performance and atom economy benzaldehyde production.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Analytical
Jinhua Zhou, Kaishuai Yang, Qi Kang, Cong Liu, Xiaoge Li, Ningna Chen, Chunliang Lu, Xizhang Wang, Luming Peng, Xuefeng Guo, Weiping Ding, Wenhua Hou
Summary: Li-ion capacitors (LICs) combine the high energy density of batteries, high power density of capacitors, and long cycle life. In this study, a TiO2/Ti3C2Tx heterostructure was fabricated, resulting in enhanced specific capacity, outstanding rate capability, and excellent cyclic stability. The TiO2/Ti3C2Tx//CPC LIC demonstrated a wide operating voltage window, high energy density, high power density, and good cycling stability.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Yuuki Wittmer, Khaled M. Jami, Rachelle K. Stowell, Truc Le, Ivan Hung, Dylan T. Murray
Summary: Protein domains biased toward a few amino acid types play a crucial role in the formation of biomolecular condensates. These compartments are formed by molecules with various movements and structural order. Missense mutations can increase the persistence lifetimes or structural order of condensates, which are associated with pathological protein aggregation. In the study of stress granules related to neurodegenerative diseases, the liquid droplets of protein are transformed into beta-strand rich fibrils. The research focuses on the molecular mechanism of the rigidification of liquid droplets and the influence of disease mutations.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Racha Bayzou, Julien Trebosc, Ivan Hung, Zhehong Gan, Andrew Rankin, Olivier Lafon, Jean-Paul Amoureux
Summary: The indirect NMR detection of quadrupolar nuclei in solids can be achieved through the T-HMQC sequence incorporating the TRAPDOR dipolar recoupling. Numerical simulations of spin dynamics show that the fastest coherence transfer in the T-HMQC scheme is achieved when using the highest compatible rf field. Furthermore, the indirect detection of triple-quantum coherences improves the spectral resolution for spin-3/2 quadrupolar nuclei.
SOLID STATE NUCLEAR MAGNETIC RESONANCE
(2022)
Article
Chemistry, Multidisciplinary
Wanlin Fu, Wanlin Xu, Kuibo Yin, Xiangyu Meng, Yujie Wen, Luming Peng, Mingyu Tang, Litao Sun, Yueming Sun, Yunqian Dai
Summary: In this study, TiO2 nanofibers were reinforced by introducing Al3+-species during electrospinning, leading to improved mechanical performance. The toughening mechanism was revealed by TEM observation and solid-state O-17-NMR spectra. The modified TiO2 nanofibers exhibited excellent sinter-resistance and were successfully folded into 3D sponge filters with high filtration efficiency.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Physical
Vinicius Martins, Bryan E. G. Lucier, Kuizhi Chen, Ivan Hung, Zhehong Gan, Christel Gervais, Christian Bonhomme, Heng-Yong Nie, Wanli Zhang, Yining Huang
Summary: Porous metal-organic frameworks (MOFs) have diverse applications in various fields, and post synthetic modification (PSM) approaches can enhance their properties. In this study, high-field solid-state NMR techniques were used to gain molecular-level insights into a prototypical aluminum MOF and its interactions with metal guests. The results provide detailed information about the oxygen environment, intermolecular interactions, and host-guest connectivity in the MOF.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Junchao Chen, Fang Wang, Yujie Wen, Weiping Tang, Luming Peng
Summary: Recent advances in applying O-17 solid-state NMR spectroscopy have provided valuable information on the surface structure, active sites, and reaction mechanisms of catalytic oxides. This article provides a brief introduction to O-17 solid-state NMR spectroscopy and discusses recent methodological developments related to its applications. Furthermore, it reviews the applications of O-17 NMR in elucidating the structure of oxide catalysts and related mechanisms, with a specific focus on recent research on oxide nanomaterials and zeolites. Finally, it offers opinions on remaining challenges and future directions in this emerging field.
Article
Chemistry, Multidisciplinary
Changju Yang, Xiang Ning, Shanyong Chen, Xiaoxia Hou, Xiaoli Xia, Zhiyang Zhang, Weiping Ding, Luming Peng
Summary: In this study, the synthesis conditions for preparing CeO2 nanorods with exposed (111) facets were investigated. Optimal synthesis conditions were found and CeO2 nanorods with very narrow O-17 NMR peaks were obtained, providing a foundation for future research on mechanisms involving ceria materials using O-17 solid-state NMR spectroscopy.
Article
Chemistry, Inorganic & Nuclear
Molly Wagner, Roberta Pigliapochi, Valeria Di Tullio, Jaclyn Catalano, Nicholas Zumbulyadis, Silvia A. Centeno, Xiaoling Wang, Kuizhi Chen, Ivan Hung, Zhehong Gan, Michael R. Dworzak, Glenn P. A. Yap, Cecil Dybowski
Summary: A series of medium- and long-chain zinc carboxylates were analyzed using ultra-high-field Zn-67 NMR, C-13 NMR, and FTIR spectroscopy. The single-crystal X-ray diffraction structures of zinc nonanoate, zinc decanoate, and zinc oleate were also reported for the first time. The NMR and X-ray diffraction data suggest the existence of three distinct geometric groups for the carboxylates. This study provides a future direction for the use of dynamic nuclear polarization (DNP)-NMR-based minimally invasive methods to test artwork for the presence of zinc carboxylates.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Wanli Zhang, Alia Hassan, Jochem Struppe, Martine Monette, Ivan Hung, Zhehong Gan, Vinicius Martins, Victor Terskikh, Yining Huang
Summary: By combining new cryogenic MAS probe technology and conducting NMR experiments at a high magnetic field, the challenges of low sensitivity in Zn-67 solid-state NMR have been overcome, leading to remarkable signal enhancement and providing enhanced information for MOF characterization.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ivan Hung, Wenping Mao, Eric G. Keeler, Robert G. Griffin, Peter L. Gor'kov, Zhehong Gan
Summary: High sensitivity and resolution solid-state NMR methods are developed for selecting hydrogen-bonded N-15-O-17 pairs in peptides, aiding protein secondary and tertiary structure determination. Enhanced sensitivity is achieved through indirect H-1 detection under fast MAS and stronger relayed dipole couplings.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Yijue Xu, Miriam Calabrese, Nicola Demitri, Andrea Pizzi, Tamali Nag, Ivan Hung, Zhehong Gan, Giuseppe Resnati, David L. Bryce
Summary: The bonding between rhenium and organic perrhenates is investigated using Re-185/187 solid-state NMR and Re-185/187 NQR techniques. The quadrupolar couplings of Re-185/187 can distinguish MaB samples from control samples, and their precise values are affected by the shear strain of ReO4- anions.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Yijue Xu, Miriam Calabrese, Nicola Demitri, Andrea Pizzi, Tamali Nag, Ivan Hung, Zhehong Gan, Giuseppe Resnati, David L. Bryce
Summary: In this study, the bonding between rhenium and the matrix in a set of organic perrhenates was investigated using Re-185/187 solid-state NMR and Re-185/187 NQR techniques. The quadrupolar couplings of Re-185/187 were able to distinguish between MaB samples and control samples, and their precise values were determined by the shear strain of the ReO4- anions.
CHEMICAL COMMUNICATIONS
(2023)
