4.6 Article

Influence of deuteration in the glassing matrix on 13C dynamic nuclear polarization

期刊

PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 15, 期 19, 页码 7032-7035

出版社

ROYAL SOC CHEMISTRY
DOI: 10.1039/c3cp50750e

关键词

-

资金

  1. National Institutes of Health (NIH) [R21EB009147, NIBIB RR02584]
  2. CPRIT [RP-101243]

向作者/读者索取更多资源

Replacement of protons by deuterons in the glassing solvents led to 2-3-fold improvement of the C-13 dynamic nuclear polarization (DNP) solid-state NMR signal for samples doped with large electron spin resonance (ESR) linewidth free radicals galvinoxyl, DPPH, and 4-oxo-TEMPO. Meanwhile, the reverse effect is observed for C-13 DNP using small ESR linewidth free radicals BDPA and trityl OX063.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.6
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Multidisciplinary Sciences

ROS and hypoxia signaling regulate periodic metabolic arousal during insect dormancy to coordinate glucose, amino acid, and lipid metabolism

Chao Chen, Rohit Mahar, Matthew E. Merritt, David L. Denlinger, Daniel A. Hahn

Summary: Metabolic suppression is a key feature of animal dormancy, helping animals save energy. Previous studies have shown that periodic arousal is driven by an increase in aerobic metabolism, with predictable fluctuations in molecules related to energy metabolism during these cycles. ROS signaling regulates periodic arousal by changing the activity of critical metabolic enzymes, suggesting its potential importance in regulating other metabolic cycles during dormancy.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2021)

Article Biochemistry & Molecular Biology

Application of Carbon-13 Isotopomer Analysis to Assess Perinatal Myocardial Glucose Metabolism in Sheep

Mukundan Ragavan, Mengchen Li, Anthony G. Giacalone, Charles E. Wood, Maureen Keller-Wood, Matthew E. Merritt

Summary: Ovine models have been widely used for studying maternal-fetal interactions and congenital heart diseases. This study demonstrates a comprehensive assessment of heart function and metabolism in a perinatal model, with the use of [U-C-13]glucose as a tracer to study central energy metabolism. The methodology presented can be applied to investigate acute and chronic effects of hormonal signaling in future studies.

METABOLITES (2021)

Article Radiology, Nuclear Medicine & Medical Imaging

Deuterated water imaging of the rat brain following metabolism of [2H7]glucose

Rohit Mahar, Huadong Zeng, Anthony Giacalone, Mukundan Ragavan, Thomas H. Mareci, Matthew E. Merritt

Summary: This study demonstrates for the first time the metabolic imaging of HDO as a marker of glucose, lactate, and glutamate/glutamine metabolism. The generation of HDO in the brain is linearly related to the appearance of lactate and glutamate/glutamine in the appropriate pseudo-steady state window. Selective imaging of HDO and glucose can be easily achieved using a gradient-echo method.

MAGNETIC RESONANCE IN MEDICINE (2021)

Article Endocrinology & Metabolism

Insulin resistance is mechanistically linked to hepatic mitochondrial remodeling in non-alcoholic fatty liver disease

Chris E. Shannon, Mukundan Ragavan, Juan Pablo Palavicini, Marcel Fourcaudot, Terry M. Bakewell, Ivan A. Valdez, Iriscilla Ayala, Eunsook S. Jin, Muniswamy Madesh, Xianlin Han, Matthew E. Merritt, Luke Norton

Summary: Insulin resistance and altered hepatic mitochondrial function are key features of type 2 diabetes (T2D) and non-alcoholic fatty liver disease (NAFLD). This study found that insulin sensitization with pioglitazone can mitigate mitochondrial dysfunction in the liver, which is independent of changes in hepatic lipid accumulation. The research highlights potential therapeutic targets for T2D and NAFLD, emphasizing the benefits of insulin sensitization in managing obesity-related diseases.

MOLECULAR METABOLISM (2021)

Article Biochemical Research Methods

Comparison of selective excitation and multi-echo chemical shift encoding for imaging of hyperpolarized [1-13C]pyruvate

Keith A. Michel, Mukundan Ragavan, Christopher M. Walker, Matthew E. Merritt, Stephen Y. Lai, James A. Bankson

Summary: This study compared two commonly used HP spectroscopic imaging methods for HP [1-C-13]pyruvate imaging scans at 7T, finding that images acquired with spectral-spatial excitation and CSE had effectively equivalent SNR with identical effective excitation angles.

JOURNAL OF MAGNETIC RESONANCE (2021)

Article Endocrinology & Metabolism

Intraspecific variation in polar and nonpolar metabolite profiles of a threatened Caribbean coral

Joseph A. Henry, Ram B. Khattri, Joy Guingab-Cagmat, Matthew E. Merritt, Timothy J. Garrett, Joshua T. Patterson, Kathryn E. Lohr

Summary: This study focused on comparing metabolomic profiles of unique genotypes of the threatened coral Acropora cervicornis, aiming to identify key metabolites driving separation among genotypes and improve restoration efforts. Results showed significant variation in metabolite profiles among A. cervicornis genotypes, indicating differences in metabolome structure could influence phenotypic variation among genotypes.

METABOLOMICS (2021)

Article Biotechnology & Applied Microbiology

INCA 2.0: A tool for integrated, dynamic modeling of NMR- and MS-based isotopomer measurements and rigorous metabolic flux analysis

Mohsin Rahim, Mukundan Ragavan, Stanislaw Deja, Matthew E. Merritt, Shawn C. Burgess, Jamey D. Young

Summary: Metabolic flux analysis is a method that combines experimental measurements and computational modeling to determine reaction rates in biological systems. This study introduces a software tool called INCA 2.0, which can integrate isotopomer measurements from both MS and NMR platforms and estimate metabolic fluxes with flexibility. The results demonstrate that INCA 2.0 accurately simulates and analyzes NMR datasets, outperforming other established tools. Additionally, combining NMR and MS datasets improves the precision of estimated fluxes.

METABOLIC ENGINEERING (2022)

Article Physiology

Detecting de novo Hepatic Ketogenesis Using Hyperpolarized [2-13C] Pyruvate

Mukundan Ragavan, Marc A. McLeod, Anna Rushin, Matthew E. Merritt

Summary: The role of ketones in metabolic health has evolved over time, from being considered a simple byproduct to playing a central role in various diseases. This study found that ketones can be produced from carbohydrates, but only when the activity of pyruvate dehydrogenase is upregulated.

FRONTIERS IN PHYSIOLOGY (2022)

Article Engineering, Electrical & Electronic

Application of Counter-Wound Multi-Arm Spirals in HTS Resonator Design

Taylor L. Johnston, Arthur S. Edison, Vijaykumar Ramaswamy, Nicolas Freytag, Matthew E. Merritt, Jeremy N. Thomas, Jerris W. Hooker, Ilya M. Litvak, William W. Brey

Summary: Significant sensitivity improvements have been achieved by using high temperature superconducting resonators in nuclear magnetic resonance probes. This study investigates the use of multi-arm spiral resonators to increase the excitation field for C-13 nuclei and preliminary tests show that they may produce a stronger excitation field.

IEEE TRANSACTIONS ON APPLIED SUPERCONDUCTIVITY (2022)

Editorial Material Radiology, Nuclear Medicine & Medical Imaging

Editorial for Whole-Abdomen Metabolic Imaging of Healthy Volunteers Using Hyperpolarized [1-13C]pyruvate MRI

Matthew E. Merritt

JOURNAL OF MAGNETIC RESONANCE IMAGING (2022)

Article Cell Biology

Lipogenesis mediated by OGR1 regulates metabolic adaptation to acid stress in cancer cells via autophagy

Smitha Pillai, Iqbal Mahmud, Rohit Mahar, Crystal Griffith, Michael Langsen, Jonathan Nguyen, Jonathan W. Wojtkowiak, Pawel Swietach, Robert A. Gatenby, Marilyn M. Bui, Matthew E. Merritt, Patricia McDonald, Timothy J. Garrett, Robert J. Gillies

Summary: The accumulation of cytoplasmic lipid droplets in malignant tumors is an adaptive response to extracellular acidity, with the acid-sensing receptor OGR1 playing a crucial role in triggering this process. Depletion of OGR1 inhibits the formation of lipid droplets under acidic conditions, impacting cell survival.

CELL REPORTS (2022)

Article Multidisciplinary Sciences

Ex Vivo Hepatic Perfusion through the Portal Vein in Mouse

Anthony G. Giacalone, Matthew E. Merritt, Mukundan Ragavan

Summary: Metabolic diseases are on the rise, and understanding liver metabolism is crucial. Ex vivo liver perfusion combined with NMR allows for comprehensive analysis and reproducible results.

JOVE-JOURNAL OF VISUALIZED EXPERIMENTS (2022)

Article Chemistry, Analytical

Segmented Flow Strategies for Integrating Liquid Chromatography-Mass Spectrometry with Nuclear Magnetic Resonance for Lipidomics

Jiajun Lei, Rohit Mahar, Mario C. Chang, James Collins, Matthew E. Merritt, Timothy J. Garrett, Richard A. Yost

Summary: Building an accurate lipid inventory requires coordinated information from different analytical capabilities. Integrating LC, HRMS, MS/MS, and 1H NMR would be ideal for this purpose. LC-HRMS/MS provides lower-level structural information with high sensitivity, while 1H NMR provides higher-order structural information for the differentiation of isomers. Digitizing the LC eluent and splitting it into two flows for HRMS/MS and NMR allows for correlation of MS and NMR data based on chromatographic retention time.

ANALYTICAL CHEMISTRY (2023)

Article Nutrition & Dietetics

Metabolomic Profiling of Asparagine Deprivation in Asparagine Synthetase Deficiency Patient-Derived Cells

Mario C. Chang, Stephen J. Staklinski, Vinay R. Malut, Geraldine L. Pierre, Michael S. Kilberg, Matthew E. Merritt

Summary: The natural amino acid asparagine (Asn) is essential for cell function and proliferation. While healthy cells can synthesize Asn, cancer and genetically diseased cells rely on extracellular sources. Deficiency in asparagine synthetase (ASNS), the enzyme responsible for Asn synthesis, leads to congenital microcephaly, seizures, and brain atrophy. In this study, metabolomics analysis of ASNS-deficient cells revealed disruptions in various metabolites, along with decreased TCA cycle intermediates and anaplerotic substrates in response to Asn deprivation. Pantothenate, phenylalanine, and aspartate were identified as potential biomarkers of Asn deprivation, suggesting the possibility of a novel diagnostic method for ASNS deficiency using targeted biomarker analysis from a blood draw.

NUTRIENTS (2023)

Article Biochemical Research Methods

A method for measurement of human asparagine synthetase (ASNS) activity and application to ASNS protein variants associated with ASNS deficiency

Mario C. Chang, Stephen J. Staklinski, Matthew E. Merritt, Michael S. Kilberg

Summary: Asparagine synthetase deficiency (ASNSD) is an inborn error of metabolism caused by mutations in the ASNS gene, resulting in insufficient production of asparagine and impacting fetal brain development. This study presents a simple method to evaluate the effect of ASNS variants on enzymatic activity.

BIOLOGY METHODS & PROTOCOLS (2023)

Article Chemistry, Physical

Effect of a single methyl substituent on the electronic structure of cobaltocene studied by computationally assisted MATI spectroscopy

Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng

Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Review Chemistry, Physical

Polymer mechanochemistry: from single molecule to bulk material

Qifeng Mu, Jian Hu

Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Complex oiling-out behavior of procaine with stable and metastable liquid phases

Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li

Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Breaking the size constraint for nano cages using annular patchy particles

Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu

Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Effect of the charge rate on the mechanical response of composite graphite electrodes: in situ experiment and mathematical analysis

Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li

Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

The effect of weak π-π interactions on single-molecule electron transport properties of the tetraphenylethene molecule and its derivatives: a first-principles study

Zhiye Wang, Yunchuan Li, Mingjun Sun

Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Designed fabrication of MoS2 hollow structures with different geometries and the comparative investigation toward capacitive properties

Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang

Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Exploiting the photophysical features of DMAN template in ITQ-51 zeotype in the search for FRET energy transfer

Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez

Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Insights into the multi-functional lithium difluoro(oxalate)borate additive in boosting the Li-ion reaction kinetics for Li3VO4 anodes

Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni

Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

New insights into the structure of the Ag(111)-p(4 x 4)-O phase: high-resolution STM and DFT study

B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga

Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

ClO-driven degradation of graphene oxide: new insights from DFT calculations

S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez

Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Composition dependence of X-ray stability and degradation mechanisms at lead halide perovskite single crystal surfaces

Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel

Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Effect of porosity on rapid dynamic compaction of nickel nanopowder

Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov

Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

The effect of temperature and oxygen partial pressure on the concentration of iron and manganese ions in La1/3Sr2/3Fe1-xMnxO3-δ

Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev

Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)

Article Chemistry, Physical

Perovskenes: two-dimensional perovskite-type monolayer materials predicted by first-principles calculations

Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub

Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2024)