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Autore: Grafiati
Pubblicato: 25 maggio 2024

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1

Maryunina, Kseniya Yu, Xiao Zhang, Sadafumi Nishihara, Katsuya Inoue, Vitaly A. Morozov, Galina V. Romanenko e Victor I. Ovcharenko. "A heterospin pressure sensor". Journal of Materials Chemistry C 3, n. 30 (2015): 7788–91. http://dx.doi.org/10.1039/c5tc01005e.

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2

Bonesteel, Jo-Anne K., Babul Borah e Richard D. Bates. "Effects of nitroxide free radicals on proton donor chemical shifts". Journal of Magnetic Resonance (1969) 98, n. 3 (luglio 1992): 475–82. http://dx.doi.org/10.1016/0022-2364(92)90002-o.

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3

Kirste, B. "EPR and ENDOR Investigations of a Cholestane Spin Probe in Liquid Crystals". Zeitschrift für Naturforschung A 42, n. 11 (1 novembre 1987): 1296–304. http://dx.doi.org/10.1515/zna-1987-1112.

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Abstract (sommario):
A detailed ENDOR study of anisotropic proton hyperfine shifts in the nitroxide spin probe 3-doxylcholestane (CSL) in liquid-crystalline solution is described. The data are interpreted by means of theoretically calculated proton hyperfine tensors (McConnell-Strathdee-Derbyshire treatment), providing an independent check of the ordering matrix. The orientational order and the dynamic behavior of the nematic and smectic phases of the liquid crystals (40,6), (50,6), and 8CB are investigated by EPR using CSL and phenalenyl as spin probes.
4

Maupu, Alexandre, Yara Kanawati, Adrien Métafiot e Milan Maric. "Ethylene Glycol Dicyclopentenyl (Meth)Acrylate Homo and Block Copolymers via Nitroxide Mediated Polymerization". Materials 12, n. 9 (11 maggio 2019): 1547. http://dx.doi.org/10.3390/ma12091547.

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Nitroxide-mediated polymerization (NMP), (homo and block copolymerization with styrene (S) and butyl methacrylate/S) of ethylene glycol dicyclopentenyl ether (meth)acrylates (EGDEA and EGDEMA) was studied using BlocBuilder alkoxyamines. EGDEA homopolymerization was not well-controlled, independent of temperature (90–120 °C), or additional free nitroxide (0–10 mol%) used. Number average molecular weights (Mn) achieved for poly(EGDEA) were 4.0–9.5 kg mol−1 and were accompanied by high dispersity (Ð = Mw/Mn = 1.62–2.09). Re-initiation and chain extension of the poly(EGDEA) chains with styrene (S) indicated some block copolymer formation, but a high fraction of chains were terminated irreversibly. EGDEA-stat-S statistical copolymerizations with a low mol fraction S in initial feed, fS,0 = 0.05, were slightly better controlled compared to poly(EGDEA) homopolymerizations (Ð was reduced to 1.44 compared to 1.62 at similar conditions). EGDEMA, in contrast, was successfully polymerized using a small fraction of S (fS,0 ~ 10 mol%) to high conversion (72%) to form well-defined EGDEMA-rich random copolymer (molar composition = FEGDEMA = 0.87) of Mn = 14.3 kg mol−1 and Ð = 1.38. EGDEMA-rich compositions were also polymerized with the unimolecular succinimidyl ester form of BlocBuilder initiator, NHS-BlocBuilder with similar results, although Ðs were higher ~1.6. Chain extensions resulted in monomodal shifts to higher molecular weights, indicating good chain end fidelity.
5

Sweger, Sarah R., Vasyl P. Denysenkov, Lutz Maibaum, Thomas F. Prisner e Stefan Stoll. "The effect of spin polarization on double electron–electron resonance (DEER) spectroscopy". Magnetic Resonance 3, n. 1 (1 luglio 2022): 101–10. http://dx.doi.org/10.5194/mr-3-101-2022.

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Abstract (sommario):
Abstract. Double electron–electron resonance (DEER) spectroscopy measures the distribution of distances between two electron spins in the nanometer range, often on doubly spin-labeled proteins, via the modulation of a refocused spin echo by the dipolar interaction between the spins. DEER is commonly conducted under conditions where the polarization of the spins is small. Here, we examine the DEER signal under conditions of high spin polarization, thermally obtainable at low temperatures and high magnetic fields, and show that the signal acquires a polarization-dependent out-of-phase component both for the intramolecular and intermolecular contributions. For the latter, this corresponds to a phase shift of the spin echo that is linear in the pump pulse position. We derive a compact analytical form of this phase shift and show experimental measurements using monoradical and biradical nitroxides at several fields and temperatures. The effect highlights a novel aspect of the fundamental spin physics underlying DEER spectroscopy.
6

Bales, Barney L., Francis L. Harris, Mirna Peric e Miroslav Peric. "Electron Paramagnetic Resonance Line Shifts and Line Shape Changes Due to Spin Exchange of Nitroxide Free Radicals in Liquids. 7. Singly Charged Surfactant Nitroxide". Journal of Physical Chemistry A 113, n. 33 (20 agosto 2009): 9295–303. http://dx.doi.org/10.1021/jp905335r.

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7

Romanenko, G. V., S. E. Tolstikov, E. V. Tretyakov, S. V. Fokin, V. N. Ikorskii e V. I. Ovcharenko. "Shift of stereochemical nonrigidity from coordination units to polymethylene fragments in heterospin copper(II) hexafluoroacetylacetonate complexes with nitronyl nitroxide biradicals". Russian Chemical Bulletin 56, n. 9 (settembre 2007): 1795–804. http://dx.doi.org/10.1007/s11172-007-0279-6.

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8

Bales, Barney L., e Miroslav Peric. "EPR Line Shifts and Line Shape Changes Due to Spin Exchange of Nitroxide Free Radicals in Liquids". Journal of Physical Chemistry B 101, n. 43 (ottobre 1997): 8707–16. http://dx.doi.org/10.1021/jp970995g.

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9

Hwang, Jimmy S., e Ghassan A. Oweimreen. "Relating static shifts in the ESR spectra of a nitroxide radical in solution to second order perturbation theory". Concepts in Magnetic Resonance Part A 30A, n. 6 (2007): 349–57. http://dx.doi.org/10.1002/cmr.a.20096.

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10

Mancini, Giordano, Marco Fusè, Filippo Lipparini, Michele Nottoli, Giovanni Scalmani e Vincenzo Barone. "Molecular Dynamics Simulations Enforcing Nonperiodic Boundary Conditions: New Developments and Application to the Solvent Shifts of Nitroxide Magnetic Parameters". Journal of Chemical Theory and Computation 18, n. 4 (8 marzo 2022): 2479–93. http://dx.doi.org/10.1021/acs.jctc.2c00046.

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11

Schibli, David J., Raquel F. Epand, Hans J. Vogel e Richard M. Epand. "Tryptophan-rich antimicrobial peptides: comparative properties and membrane interactions". Biochemistry and Cell Biology 80, n. 5 (1 ottobre 2002): 667–77. http://dx.doi.org/10.1139/o02-147.

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Abstract (sommario):
The interaction of several tryptophan (Trp)-rich cationic antimicrobial peptides with membranes was investigated. These peptides included tritrpticin, indolicidin, lactoferricin B (Lfcin B), and a shorter fragment of lactoferricin (LfcinB4–9). The average environment of the Trp residues of these peptides was assessed from their fluorescence properties, both the wavelength of maximal emission as well as the red edge effect. The insertion of the peptides into vesicles of differing composition was examined using quenching of the Trp fluorescence, with both soluble acrylamide and nitroxide-labelled phospholipids as well as by chemical modification of the Trp residues with N-bromosuccinimide. The results were consistent with the Trp side chains positioned mostly near the membrane–water interface. The extent of burial of the Trp side chains appears to be greater in vesicles containing phospholipids with the anionic phosphatidylglycerol headgroup. Leakage of the aqueous contents of liposomes was also measured using the 8-aminonaphthalene-1,3,6-trisulfonic acid – p-xylene-bis-pyridinium bromide assay. Tritrpticin, which demonstrated the greatest red edge shift, also displayed the largest amount of leakage from liposomes. Taken together, the results illustrate that cationic Trp-rich antimicrobial peptides preferentially disrupt large unilamellar vesicles with a net negative charge following their insertion into the interfacial region of the phospholipid bilayer.Key words: lactoferricin B, indolicidin, tritrpticin, antimicrobial peptide, membrane, vesicle, fluorescence, spin-label, quenching.
12

Zhang, Chun-Xia, Mei-Hao Xiang, Xian-Jun Liu, Fenglin Wang, Ru-Qin Yu e Jian-Hui Jiang. "Development of large Stokes shift, near-infrared fluorescence probe for rapid and bioorthogonal imaging of nitroxyl (HNO) in living cells". Talanta 193 (febbraio 2019): 152–60. http://dx.doi.org/10.1016/j.talanta.2018.09.062.

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13

Chen, Lei, Jonilyn G. Longenecker, Eric W. Moore e John A. Marohn. "Long-lived frequency shifts observed in a magnetic resonance force microscope experiment following microwave irradiation of a nitroxide spin probe". Applied Physics Letters 102, n. 13 (aprile 2013): 132404. http://dx.doi.org/10.1063/1.4795018.

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14

Bales, Barney L., Michelle Meyer, Steve Smith e Miroslav Peric. "EPR Line Shifts and Line Shape Changes Due to Spin Exchange of Nitroxide-Free Radicals in Liquids 4. Test of a Method to Measure Re-Encounter Rates in Liquids Employing15N and14N Nitroxide Spin Probes". Journal of Physical Chemistry A 112, n. 11 (marzo 2008): 2177–81. http://dx.doi.org/10.1021/jp7107494.

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15

Wei, Chao, Xiaofen Wang, Xueyan Li, Xu Jia, Xinya Hao, Jiangyan Zhang, Pingzhu Zhang e Xiaoliu Li. "An isophorone-fused near-infrared fluorescent probe with a large Stokes shift for imaging endogenous nitroxyl in living cells and zebrafish". Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 227 (febbraio 2020): 117765. http://dx.doi.org/10.1016/j.saa.2019.117765.

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16

Carter, Jennifer, Michael H. Fenwick, Wen-wei Huang, Vladimir V. Popik e Thomas T. Tidwell. "Addition of the nitroxyl radical TEMPO to 1-naphthylketene: formation of an unusual adduct". Canadian Journal of Chemistry 77, n. 5-6 (1 giugno 1999): 806–9. http://dx.doi.org/10.1139/v99-043.

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Abstract (sommario):
1-Naphthylketene (2), generated by thermal Wolff-rearrangement, is trapped in situ by 2,2,6,6-tetramethylpiridinyloxy radical (TEMPO, TO·) to form the adduct 1-naphthCH(OT)CO2T (4), whose structure is confirmed by an X-ray determination. The 1H NMR spectrum of 4 displays three CH3 groups with very high field chemical shifts (δ 0.10-0.47), and this is attributed to the location of these groups in the shielding region above the π system of the naphthyl ring. At -40°C, doubling of most of the 1H NMR signals occurs, and this is attributed to a freezing out of two conformations differing by rotation around the naphthyl—CH bond.Key words: ketene, TEMPO, restricted rotation, 1H NMR, conformational analysis, free radicals.
17

Shoji, Yoshimi, Yuri Terashima, Kei Ohkubo, Hiromu Ito, Kouichi Maruyama, Shunichi Fukuzumi e Ikuo Nakanishi. "Scandium Ion-Promoted Electron-Transfer Disproportionation of 2-Phenyl-4,4,5,5-tetramethylimidazoline-1-oxyl 3-Oxide (PTIO•) in Acetonitrile and Its Regeneration Induced by Water". International Journal of Molecular Sciences 25, n. 8 (17 aprile 2024): 4417. http://dx.doi.org/10.3390/ijms25084417.

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Abstract (sommario):
2-Phenyl-4,4,5,5-tetramethylimidazoline-1-oxyl 3-oxide (PTIO•), a persistent nitronyl nitroxide radical, has been used for the detection and trapping of nitric oxide, as a redox mediator for batteries, for the activity estimation of antioxidants, and so on. However, there is no report on the reactivity of PTIO• in the presence of redox-inactive metal ions. In this study, it is demonstrated that the addition of scandium triflate, Sc(OTf)3 (OTf = OSO2CF3), to an acetonitrile (MeCN) solution of PTIO• resulted in an electron-transfer disproportionation to generate the corresponding cation (PTIO+) and anion (PTIO−), the latter of which is suggested to be stabilized by Sc3+ to form [(PTIO)Sc]2+. The decay of the absorption band at 361 nm due to PTIO•, monitored using a stopped-flow technique, obeyed second-order kinetics. The second-order rate constant for the disproportionation, thus determined, increased with increasing the Sc(OTf)3 concentration to reach a constant value. A drastic change in the cyclic voltammogram recorded for PTIO• in deaerated MeCN containing 0.10 M Bu4NClO4 was also observed upon addition of Sc(OTf)3, suggesting that the large positive shift of the one-electron reduction potential of PTIO• (equivalent to the one-electron oxidation potential of PTIO−) in the presence of Sc(OTf)3 may result in the disproportionation. When H2O was added to the PTIO•–Sc(OTf)3 system in deaerated MeCN, PTIO• was completely regenerated. It is suggested that the complex formation of Sc3+ with H2O may weaken the interaction between PTIO− and Sc3+, leading to electron-transfer comproportionation to regenerate PTIO•. The reversible disproportionation of PTIO• was also confirmed by electron paramagnetic resonance (EPR) spectroscopy.
18

Bales, Barney L., Miroslav Peric e Ileana Dragutan. "Electron Paramagnetic Resonance Line Shifts and Line Shape Changes Due to Spin Exchange between Nitroxide Free Radicals in Liquids. 3. Extension to Five Hyperfine Lines. Additional Line Shifts Due to Re-encounters". Journal of Physical Chemistry A 107, n. 43 (ottobre 2003): 9086–98. http://dx.doi.org/10.1021/jp030726s.

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19

Bales, Barney L., Michelle Meyer, Steve Smith e Miroslav Peric. "EPR Line Shifts and Line Shape Changes due to Spin Exchange of Nitroxide Free Radicals in Liquids: 6. Separating Line Broadening due to Spin Exchange and Dipolar Interactions". Journal of Physical Chemistry A 113, n. 17 (30 aprile 2009): 4930–40. http://dx.doi.org/10.1021/jp8093947.

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20

Bales, Barney L., e Miroslav Peric. "EPR Line Shifts and Line Shape Changes Due to Spin Exchange of Nitroxide Free Radicals in Liquids 2. Extension to High Spin Exchange Frequencies and Inhomogeneously Broadened Spectra". Journal of Physical Chemistry A 106, n. 19 (maggio 2002): 4846–54. http://dx.doi.org/10.1021/jp014518g.

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21

Bales, Barney L., e Miroslav Peric. "EPR Line Shifts and Line Shape Changes Due to Spin Exchange Between Nitroxide Free Radicals in Liquids 10. Spin-Exchange Frequencies of the Order of the Nitrogen Hyperfine Interaction: A Hypothesis". Applied Magnetic Resonance 48, n. 2 (3 dicembre 2016): 175–200. http://dx.doi.org/10.1007/s00723-016-0854-9.

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22

Peric, Mirna, Barney L. Bales e Miroslav Peric. "Electron Paramagnetic Resonance Line Shifts and Line Shape Changes Due to Heisenberg Spin Exchange and Dipole–Dipole Interactions of Nitroxide Free Radicals in Liquids 8. Further Experimental and Theoretical Efforts to Separate the Effects of the Two Interactions". Journal of Physical Chemistry A 116, n. 11 (9 marzo 2012): 2855–66. http://dx.doi.org/10.1021/jp210057x.

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23

Bales, Barney L., Michelle Meyer e Miroslav Peric. "EPR Line Shifts and Line Shape Changes Due to Heisenberg Spin Exchange and Dipole–Dipole Interactions of Nitroxide Free Radicals in Liquids: 9. An Alternative Method to Separate the Effects of the Two Interactions Employing 15N and 14N". Journal of Physical Chemistry A 118, n. 32 (5 agosto 2014): 6154–62. http://dx.doi.org/10.1021/jp505346g.

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24

Sowiński, Mateusz P., Sahil Gahlawat, Bjarte A. Lund, Anna-Luisa Warnke, Kathrin H. Hopmann, Janet E. Lovett e Marius M. Haugland. "Conformational tuning improves the stability of spirocyclic nitroxides with long paramagnetic relaxation times". Communications Chemistry 6, n. 1 (5 giugno 2023). http://dx.doi.org/10.1038/s42004-023-00912-7.

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Abstract (sommario):
AbstractNitroxides are widely used as probes and polarization transfer agents in spectroscopy and imaging. These applications require high stability towards reducing biological environments, as well as beneficial relaxation properties. While the latter is provided by spirocyclic groups on the nitroxide scaffold, such systems are not in themselves robust under reducing conditions. In this work, we introduce a strategy for stability enhancement through conformational tuning, where incorporating additional substituents on the nitroxide ring effects a shift towards highly stable closed spirocyclic conformations, as indicated by X-ray crystallography and density functional theory (DFT) calculations. Closed spirocyclohexyl nitroxides exhibit dramatically improved stability towards reduction by ascorbate, while maintaining long relaxation times in electron paramagnetic resonance (EPR) spectroscopy. These findings have important implications for the future design of new nitroxide-based spin labels and imaging agents.
25

Munuera-Javaloy, C., R. Puebla, B. D’Anjou, M. B. Plenio e J. Casanova. "Detection of molecular transitions with nitrogen-vacancy centers and electron-spin labels". npj Quantum Information 8, n. 1 (30 novembre 2022). http://dx.doi.org/10.1038/s41534-022-00653-w.

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AbstractWe present a protocol that detects molecular conformational changes with two nitroxide electron-spin labels and a nitrogen-vacancy (NV) center in diamond. More specifically, we demonstrate that the NV can detect energy shifts induced by the coupling between electron-spin labels. The protocol relies on the judicious application of microwave and radiofrequency pulses in a range of parameters that ensures stable nitroxide resonances. Furthermore, we demonstrate that our scheme is optimized by using nitroxides with distinct nitrogen isotopes. We develop a simple theoretical model that we combine with Bayesian inference techniques to demonstrate that our method enables the detection of conformational changes in ambient conditions including strong NV dephasing rates as a consequence of the diamond surface proximity and nitroxide thermalization mechanisms. Finally, we counter-intuitively show that with our method the small residual effect of random molecular tumbling becomes a resource that can be exploited to extract inter-label distances.
26

Chandrasekaran, Siddarth, Connor M. Schneps, Robert Dunleavy, Changfan Lin, Cristina C. DeOliveira, Abir Ganguly e Brian R. Crane. "Tuning flavin environment to detect and control light-induced conformational switching in Drosophila cryptochrome". Communications Biology 4, n. 1 (26 febbraio 2021). http://dx.doi.org/10.1038/s42003-021-01766-2.

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AbstractLight-induction of an anionic semiquinone (SQ) flavin radical in Drosophila cryptochrome (dCRY) alters the dCRY conformation to promote binding and degradation of the circadian clock protein Timeless (TIM). Specific peptide ligation with sortase A attaches a nitroxide spin-probe to the dCRY C-terminal tail (CTT) while avoiding deleterious side reactions. Pulse dipolar electron-spin resonance spectroscopy from the CTT nitroxide to the SQ shows that flavin photoreduction shifts the CTT ~1 nm and increases its motion, without causing full displacement from the protein. dCRY engineered to form the neutral SQ serves as a dark-state proxy to reveal that the CTT remains docked when the flavin ring is reduced but uncharged. Substitutions of flavin-proximal His378 promote CTT undocking in the dark or diminish undocking in the light, consistent with molecular dynamics simulations and TIM degradation activity. The His378 variants inform on recognition motifs for dCRY cellular turnover and strategies for developing optogenetic tools.
27

Arasimowicz-Jelonek, M., J. Floryszak-Wieczorek, S. Suarez, F. Doctorovich, E. Sobieszczuk-Nowicka, S. Bruce King, G. Milczarek et al. "Discovery of endogenous nitroxyl as a new redox player in Arabidopsis thaliana". Nature Plants, 23 dicembre 2022. http://dx.doi.org/10.1038/s41477-022-01301-z.

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Abstract (sommario):
AbstractNitroxyl (HNO) is the one-electron reduced and protonated congener of nitric oxide (•NO), owning a distinct chemical profile. Based on real-time detection, we demonstrate that HNO is endogenously formed in Arabidopsis. Senescence and hypoxia induce shifts in the redox balance, triggering HNO decay or formation mediated by non-enzymatic •NO/HNO interconversion with cellular reductants. The stimuli-dependent HNO generation supports or competes with •NO signalling, depending on the local redox environment.
28

Labazi, Hicham, Brandi M. Wynne e R. Clinton Webb. "Abstract 261: Nitroxyl Anion Induced Vasorelaxation in Pudendal Arteries is Partially Mediated via the Large Conductance Calcium-activated Potassuim Channel". Hypertension 60, suppl_1 (settembre 2012). http://dx.doi.org/10.1161/hyp.60.suppl_1.a261.

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Abstract (sommario):
Nitroxyl anion (HNO) - a redox congener of nitric oxide (NO) - has been demonstrated to be a potent vasodilator of both conduit and resistance vessels. Previous data from our laboratory have demonstrated that the mechanism of HNO-mediated vasorelaxation varied according to the vascular bed. However, no studies address the role of HNO in erectile function. We have demonstrated that the corpus cavernosum does not exhibit a relaxation response to HNO. However, we have shown that the pudendal artery (PA), which supplies blood flow to the penis, does exhibit a relaxation response to HNO and that ACh-mediated relaxation responses may be partially attributed to HNO as compared to NO. We hypothesized that HNO mediates vasorelaxation in pudendal arteries via activation of potassium (K + ) channels. PAs were isolated from Sprague-Dawley rats and concentration-response curves (CRC) to an HNO donor: Angeli’s Salt (AS) were performed in phenylephrine contracted vessels (1μM) in the absence and the presence of the calcium (Ca 2+ ) -activated K + channel inhibitors: TRAM-34 (intermediate Ca 2+ -activated K + -channel inhibitor, IK Ca , 10 μM) , UCL-1689 (Small conductance calcium-activated potassium channel, SK Ca ,1 μM), iberiotoxin (large conductance Ca 2+ -activated K + -channel inhibitor, BK Ca ,0.1μM). There were no observed differences in relaxation responses to AS with IK Ca and SK Ca channel inhibition. In contrast, inhibition of BK Ca channels resulted in a rightward shift in the CRC to AS (logEC 50 -4.74±0.11 vs . -5.26±0.11, p<0.01) with no differences in R max . These data suggest that AS-dependent vasorelaxation in PA is partially mediated via BK Ca channel activation.

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