Article
Thermodynamics
Rajaa Bouamoud, Raphael Mulongo-Masamba, Adnane El Hamidi, Mohammed Halim, Said Arsalane
Summary: The study characterized kerogen-rich oil shale from Central Kongo (CK) in the Democratic Republic of the Congo using various methods, indicating low maturity type I kerogen predominated by aliphatic carbons with marine origin.
JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
(2022)
Article
Agriculture, Multidisciplinary
Elif Gokcen Ates, Maria J. Beira, Mecit H. Oztop, Pedro J. Sebastiao
Summary: This study investigated the effects of different sugar components on pectin gels using a combination of H-1 nuclear magnetic resonance (NMR) relaxometry at the molecular level and assessment of viscoelastic properties at the macroscopic level. The results showed that changes in hardness and viscosity were influenced by moisture content, while local diffusion processes probed by NMR relaxometry remained unaffected. This highlights the importance of combining micro- and macroscopic information for analyzing food product properties.
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
(2021)
Article
Energy & Fuels
Deping Zhang, Huairen Cao, Yan Lei, Hao Wu, Xiaoyu Wang, Xuelian Guo, Jianping Yan, Shuhua Wang, Tianchi Shi, Haolin Li, Yan-rong Zou, Ping'an Peng
Summary: This study simulated the maturation process of lacustrine type II kerogen and investigated the molecular structure evolution. It was found that the aliphatic fractions decreased and aromatic fractions increased with increasing maturity. Before the main oil window, nonhydrocarbon heteroatomic functional groups were the main products. The oil peak occurred when hydrocarbon C14+ production reached its maximum. After the oil peak, aromatic groups became dominant. In the gas window, the large quantity of C1-5 was mainly due to the secondary cracking of hydrocarbons. The number of aromatic structures caused by alkyl bond breaking and condensation was estimated.
Review
Biochemistry & Molecular Biology
Philipp Innig Aguion, Alexander Marchanka
Summary: MAS ssNMR is an established tool for studying non-soluble or non-crystalline biomolecules, with significant progress in protein studies but challenges in RNA research. Resonance assignment is a critical step in NMR studies, determining the feasibility of structure determination. Recent research focuses on RNA resonance assignment methods and ssNMR secondary structure determination.
FRONTIERS IN MOLECULAR BIOSCIENCES
(2021)
Article
Energy & Fuels
Xiaoye Wang, Xiangxin Han, Yulong You, Xiumin Jiang
Summary: Solid-state nuclear magnetic resonance (SSNMR) techniques were used to characterize Dachengzi oil shale kerogen, revealing that protonated aromatic signals account for 24% of total aromatic signals and oxygen atoms play a crucial role in connectivities between different groups. Additionally, the presence of long methylene chain structures was indicated in the study.
Article
Multidisciplinary Sciences
Alexander Klein, Petra Rovo, Varun V. Sakhrani, Yangyang Wang, Jacob B. Holmes, Viktoriia Liu, Patricia Skowronek, Laura Kukuk, Suresh K. Vasa, Peter Guentert, Leonard J. Mueller, Rasmus Linser
Summary: NMR chemical shifts provide detailed information on the chemical properties of molecules. This study demonstrates the use of higher-dimensional, proton-detected, solid-state NMR to assign a large protein, tryptophan synthase, and characterize its chemical properties and relaxation. The results suggest a connection between active-site chemistry, electrostatic environment, and catalytically important dynamics.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Yu Rao, Amrit Venkatesh, Pinelopi Moutzouri, Lyndon Emsley
Summary: Dynamic nuclear polarization (DNP) is a method to enhance the sensitivity of nuclear magnetic resonance. In this study, we demonstrate the generation of significant H-1 hyperpolarization in solution by implementing steady-state C-13 Overhauser DNP and transferring the polarization to H-1.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Analytical
Huan Du, Xiu Gu, Jialuo Chen, Caihong Bai, Xiaohui Duan, Kaifeng Hu
Summary: The 2D 1H-13C HSQC method is widely used in metabolomics studies, but its preprocessing methods are lagging behind those of the 1D 1H NMR method. Therefore, we propose a new algorithm called Global Intensity-Guided Peak Matching and Alignment (GIPMA) for peak matching and alignment in 2D 1H-13C HSQC-based metabolomics. This algorithm dynamically searches for and intelligently selects the optimal chemical shift tolerance to improve the accuracy of the results.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Francesca Brero, Paolo Arosio, Martin Albino, Davide Cicolari, Margherita Porru, Martina Basini, Manuel Mariani, Claudia Innocenti, Claudio Sangregorio, Francesco Orsini, Alessandro Lascialfari
Summary: We investigated the effect of different organic coatings on the H-1-NMR relaxation properties of ultra-small iron-oxide-based magnetic nanoparticles. Magnetization measurements revealed similar behavior as a function of temperature and field for nanoparticles with different coatings but the same core diameter. However, the H-1-NMR longitudinal relaxivity showed different intensity and frequency behavior for the smallest particles depending on the kind of coating, indicating different electronic spin dynamics. On the other hand, no differences were found in the relaxivity of the biggest particles when the coating was changed.
Article
Food Science & Technology
Sinem Akkaya, Baris Ozel, Mecit Halil Oztop, Derya Kocak Yanik, Fahrettin Gogus
Summary: This study investigated the application of pectin-wax-based emulsion systems in preparing edible films and coatings. The addition of suitable concentrations of pectin and sunflower oil wax improved the physical characteristics of the emulsions. Furthermore, NMR relaxometry parameters were found to be effective in monitoring the formation and stability of the emulsions.
JOURNAL OF FOOD SCIENCE
(2021)
Article
Construction & Building Technology
Jing Li, Sarah Mailhiot, Harisankar Sreenivasan, Anu M. Kantola, Mirja Illikainen, Elijah Adesanya, Lubica Kriskova, Ville-Veikko Telkki, Paivo Kinnunen
Summary: Geopolymers based on metakaolin with a water-to-solid ratio of 0.59-0.66 were studied during the curing process. Monitoring of the curing process and pore structures was done using NMR relaxometry and cryoporometry, showing changes in relaxation times and pore sizes as the geopolymers matured during curing.
CEMENT AND CONCRETE RESEARCH
(2021)
Article
Construction & Building Technology
Tingjie Huang, Qiang Yuan, Shenghao Zuo, Baiyun Li, Qihong Wu, Youjun Xie
Summary: AC impedance spectroscopy (ACIS) is a promising technique for monitoring the microstructure evolution of fresh cement paste in real-time. This paper compared the change of bulk electric resistivity (rho(bulk)) obtained from ACIS with the developments of storage modulus (G') and the mean transverse relaxation times (T-2) of fresh Portland cement pastes within 5 h, showing that different microstructural phases can be accurately distinguished. The use of rho(bulk) fails to characterize the microstructural changes in Phase I due to sensitivity to the electrical conductivity of the interstitial solution, but is successful in reflecting the developing features of microstructure in Phases II and III.
CEMENT AND CONCRETE RESEARCH
(2021)
Article
Biochemical Research Methods
Harri Heikkinen, Ilkka Kilpelainen, Sami Heikkinen
Summary: In this study, 3D iDOSY-HMBC pulse sequences were modified to incorporate convection compensation element, which improved its usability. Convection compensation was achieved using the pulsed field gradient double echo method, avoiding intensity loss issues. This provides a new solution for the resolution decrease and signal intensity decrease problems at elevated temperatures.
JOURNAL OF MAGNETIC RESONANCE
(2023)
Article
Chemistry, Analytical
Runlian Qu, Lu Shan, Qun Sun, Yao Wei, Pengchi Deng, Xiandeng Hou
Summary: A simple, fast, and green method has been established to quantitatively detect isotope labelled compounds in biology and pharmacy using a novel H-1 Nuclear Magnetic Resonance (H-1-NMR) technique. This method removes the coupling between nearby H-1 and C-13, N-15, simplifying the spectrum and enhancing the signal intensity, allowing for the quantitative detection of real polypeptide samples.
Article
Thermodynamics
He Yang, Yankun Xiong, Zhouwei Xie, Lijun Jin, Yang Li, Juan Yang, Haoquan Hu
Summary: This paper proposes a method for quantitatively characterizing the carbon skeletal structure of coal using high-resolution CP/MAS 13C solid-state NMR spectroscopy, with Naomaohu coal as the experimental sample. The fractions of different carbons in coal were divided by analyzing the change of polarization transfer with contact time. The results obtained from this study are in agreement with previous literature and provide insight into the carbon structure of coal.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2021)
Review
Chemistry, Multidisciplinary
Zongyan Gao, Israel Temprano, Jiang Lei, Linbin Tang, Junjian Li, Clare P. Grey, Tao Liu
Summary: This article reviews the development of LiOH-based nonaqueous lithium-air batteries (LABs). Various catalytic systems that can activate LiOH-based electrochemistry are compared, with a focus on the oxygen reduction and evolution reactions in nonaqueous media. Key factors that can switch the cell chemistry between Li2O2 and LiOH are identified, and the debate and potential causes for opposing opinions are discussed.
ADVANCED MATERIALS
(2023)
Article
Polymer Science
Chibueze V. Amanchukwu, Anna B. Gunnarsdottir, Snehashis Choudhury, Tamsin L. Newlove, Pieter C. M. M. Magusin, Zhenan Bao, Clare P. Grey
Summary: Lithium metal batteries have the potential to revolutionize energy storage and electric transportation, but face challenges in morphology and electro-chemo-mechanics. Polymer-based solid-state electrolytes show promise in replacing liquid electrolytes, but have issues with ionic conductivity and stability. Perfluoropolyether (PFPE)-based electrolytes have improved oxidative stability, but little is known about their lithium solvation and transport mechanism. This study uses solid-state magic angle spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy to investigate lithium cation environment and mobility in PFPE electrolytes and compare it to polyethylene glycol (PEG) electrolytes. The results show weaker interaction between lithium cation and PFPE polymer backbone, resulting in stronger ion pairing. The mobility of lithium ions is lower in PFPE electrolytes, attributed to polymer backbone fluctuations. Differences in polymer backbones have a greater effect on mobility than differences in ion binding modes within each polymer class. The ability to study polymer electrolytes in their native state opens opportunities for development of next-generation lithium metal batteries.
Article
Chemistry, Physical
Dongxun Lyu, Yanting Jin, Pieter C. M. M. Magusin, Simone Sturniolo, Evan Wenbo Zhao, Shunsuke Yamamoto, Scott T. Keene, George G. Malliaras, Clare P. Grey
Summary: Operando NMR spectroscopy is used to quantify cation and water movement in organic mixed conductors, providing insights into charge-compensating interactions and ionic dynamics. The study sheds light on the working principles of organic mixed conductors and demonstrates the utility of operando NMR spectroscopy in revealing structure-property relationships in electroactive polymers.
Article
Multidisciplinary Sciences
Shunsuke Sasaki, Souvik Giri, Simon J. Cassidy, Sunita Dey, Maria Batuk, Daphne Vandemeulebroucke, Giannantonio Cibin, Ronald I. Smith, Philip Holdship, Clare P. Grey, Joke Hadermann, Simon J. Clarke
Summary: This article introduces a method called topochemistry, which enables step-by-step conversions of solid-state materials leading to metastable structures that retain initial structural motifs. Recent advances in this field have revealed examples where bulky anionic constituents actively participate in redox reactions during (de)intercalation processes, accompanied by anion-anion bond formation. This opens up possibilities for designing novel structure types in a controlled manner.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Dominic Hey, Rajesh B. Jethwa, Nadia L. Farag, Bernardine L. D. Rinkel, Evan Wenbo Zhao, Clare P. Grey
Summary: This study demonstrates how an understanding of the degradation processes in aqueous organic redox flow batteries (RFBs) can lead to significant performance improvements. By studying the redox-active biomolecule FMN, derived from vitamin B2, the researchers identify its hydrolysis products and show their impact on charging of an FMN-cyanoferrate battery. The addition of cheap electrolyte salts to lower the pH improves battery efficiency and solubility, bringing RFBs closer to commercial viability.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Sundeep Vema, Farheen N. Sayed, Supreeth Nagendran, Burcu Karagoz, Christian Sternemann, Michael Paulus, Georg Held, Clare P. Grey
Summary: Garnet solid-electrolyte-based Li-metal batteries have the potential to be used in high-energy density and thermally stable energy storage devices. However, the formation of lithium hydroxide and carbonate on the garnet surface in an ambient atmosphere poses processing challenges. This study investigates the decomposition of surface layers under different gas environments and identifies that heating under an oxygen atmosphere leads to a clean garnet surface, while low oxygen partial pressures result in additional carbon deposits. The clean garnet surface reacts with moisture and carbon dioxide, indicating a need for control over CO2 concentration during garnet handling. Symmetric cells with low interface resistance and dendrite-free plating currents are achieved by heating under O₂ and avoiding H₂O and CO₂.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Adam J. Lovett, Venkateswarlu Daramalla, Farheen N. Sayed, Debasis Nayak, Muireann de h-Ora, Clare P. Grey, Sian E. Dutton, Judith L. MacManus-Driscoll
Summary: Epitaxial cathodes in lithium-ion microbatteries are ideal model systems for studying mass and charge transfer across interfaces and degradation processes. In this study, we report the growth of epitaxial LiMn2O4 (LMO) thin films on a new current collector material, NiCo2O4 (NCO), at a low temperature of 360°C. Our films show a discharge capacity of >100 mAh g(-1) for >6000 cycles, indicating long-term electrochemical stability of our NCO current collector. This research offers a route towards high-performance microbatteries for miniaturized electronic devices.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Arvind Pujari, Byung-Man Kim, Farheen N. Sayed, Kate Sanders, Wesley M. Dose, Angus Mathieson, Clare P. Grey, Neil C. Greenham, Michael De Volder
Summary: Light-rechargeable photobatteries are a solution to the intermittency of solar irradiation. This study analyzes the thermal contributions to the increase in capacity of two promising photoactive cathode materials under different charging conditions. The results show that the increase in capacity is mainly due to thermal effects.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Ioan-Bogdan Magdau, Daniel J. Arismendi-Arrieta, Holly E. Smith, Clare P. Grey, Kersti Hermansson, Gabor Csanyi
Summary: In this study, a powerful machine learning approach is presented for simulating the molecular behavior of the EC:EMC binary solvent in liquid electrolytes. This method accurately captures the key properties of the organic molecule mixture and addresses the challenge of scale separation between intra- and inter-molecular interactions in condensed phase molecular systems.
NPJ COMPUTATIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Laura L. Driscoll, Elizabeth H. Driscoll, Bo Dong, Farheen N. Sayed, Jacob N. Wilson, Christopher A. O'Keefe, Dominic J. Gardner, Clare P. Grey, Phoebe K. Allan, Adam A. L. Michalchuk, Peter R. Slater
Summary: The synthesis of Li ion battery materials via ball milling has seen significant growth, resulting in the discovery of new high-capacity electrode materials. This study challenges the commonly assumed local heating effects during the milling process, showing that other factors, such as shockwaves and localized pressure, play a crucial role in phase transformations. The research provides a greater understanding of milling as a synthetic pathway and suggests alternative strategies for material preparation.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
James H. J. Ellison, Clare P. Grey
Summary: This paper discusses the short lifespan issue and electrolyte stability problem of lithium-air batteries and suggests the possibility of optimizing cell design and exploring new molecules for electrolyte construction.
FARADAY DISCUSSIONS
(2023)
Article
Materials Science, Multidisciplinary
Hrishit Banerjee, Clare P. Grey, Andrew J. Morris
Summary: Using ab initio dynamical mean-field theory, this study explores the electronic and magnetic states of layered LixMnO2 as a function of x, the state-of-charge. The results show different states of the system during delithiation at various charge states, and the presence of high-spin state is observed to be most likely.
Article
Chemistry, Physical
Svetlana Menkin, Jana B. Fritzke, Rebecca Larner, Cas de Leeuw, Yoonseong Choi, Anna B. Gunnarsdottir, Clare P. Grey
Summary: This study reveals the presence of soft shorts, which are often overlooked due to their indistinguishable electrochemical signatures, in realistic conditions using impedance spectroscopy and operando NMR. It also demonstrates the predictability of soft shorts and the potential use of electrochemical impedance spectroscopy for early detection of catastrophic shorts and battery failure.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Physical
Erlendur Jonsson, Astrid H. Berge, Clare P. Grey, Israel Temprano
Summary: In this study, the role of electrolyte composition in the solvation of I- in iodide-based redox mediation in Li-O-2 batteries was investigated using a molecular dynamics approach. The results showed that shorter glymes allow for a closer packing of I- redox mediator, and increasing the concentration of I- reduces the solvation of Li+ in glymes. The presence of water further facilitates the interaction between I- and Li+, with a more pronounced effect in monoglyme. The competition between Li+ and I- for water coordination is modulated by different solvents, with longer chain lengths being less affected by increases in water concentrations.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Rosa Muller, Olivia Georghiades, Joshua D. Bocarsly, Farheen N. Sayed, Victor Riesgo-Gonzalez, Andrew D. Bond, Clare P. Grey, Dominic S. Wright
Summary: This study investigates the potential of lanthanide-containing polyoxotitanates as single-source precursors for hybrid oxides. The properties of the compounds were characterized using magnetic measurements, and their stability at high temperatures was observed.
DALTON TRANSACTIONS
(2023)