Solid state nuclear magnetic resonance最新文献

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Deuteron-proton isotope correlation spectroscopy at high magnetic fields 强磁场下氘核-质子同位素相关光谱
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2025-02-04 DOI: 10.1016/j.ssnmr.2025.101993
Neethu Thomas , Claire Welton , Tomasz Pawlak , Parth Raval , Julien Trébosc , Sheetal K. Jain , G.N. Manjunatha Reddy
{"title":"Deuteron-proton isotope correlation spectroscopy at high magnetic fields","authors":"Neethu Thomas ,&nbsp;Claire Welton ,&nbsp;Tomasz Pawlak ,&nbsp;Parth Raval ,&nbsp;Julien Trébosc ,&nbsp;Sheetal K. Jain ,&nbsp;G.N. Manjunatha Reddy","doi":"10.1016/j.ssnmr.2025.101993","DOIUrl":"10.1016/j.ssnmr.2025.101993","url":null,"abstract":"<div><div>A cross-polarization <sup>2</sup>H–<sup>1</sup>H isotope correlation spectroscopy (CP-iCOSY) approach is presented for characterizing a deuterated amino acid, pharmaceutical compound and a solid formulation. This can be achieved by isotopic enrichment in conjunction with high magnetic field (28.2 T) and fast magic-angle spinning (MAS), enabling the rapid detection of <sup>2</sup>H NMR spectra in a few seconds to minutes. Specifically, two-dimensional (2D) <sup>2</sup>H–<sup>1</sup>H CP-iCOSY experiment allows the local structures and through-space interactions in a partially deuterated compounds to be elucidated. In doing so, we compare conventional spin-lock and rotor-echo-short-pulse-irradiation <sup>RESPIRATION</sup>CP sequences for acquiring 2D <sup>1</sup>H–<sup>2</sup>H correlation spectra. The <sup>RESPIRATION</sup>CP sequence allows the detection of 2D peaks at lower CP contact times (0.1–1 ms) than the conventional CP (0.2–4 ms) sequence. Analysis of partially deuterated L-histidine·HCl·H<sub>2</sub>O and dopamine.HCl is presented, in which the detection of 2D peaks corresponding to <sup>2</sup>H–<sup>1</sup>H pairs separated by greater than 4 Å distance demonstrates the potential of the presented approach for the characterization of packing interactions. These results are corroborated by NMR crystallography analysis using the Gauge-Including Projector Augmented-Wave (GIPAW) approach.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"136 ","pages":"Article 101993"},"PeriodicalIF":1.8,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143418551","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Optimal control: From sensitivity improvement to alternative pulse-sequence design in solid-state NMR 最优控制:从灵敏度改进到固体核磁共振脉冲序列设计。
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2025-02-01 DOI: 10.1016/j.ssnmr.2024.101984
Jan Blahut , Zdeněk Tošner
{"title":"Optimal control: From sensitivity improvement to alternative pulse-sequence design in solid-state NMR","authors":"Jan Blahut ,&nbsp;Zdeněk Tošner","doi":"10.1016/j.ssnmr.2024.101984","DOIUrl":"10.1016/j.ssnmr.2024.101984","url":null,"abstract":"<div><div>Exciting developments in new experimental methods for multidimensional solid-state NMR spectroscopy have recently been achieved using optimal-control theory. These results, in turn, have triggered the development of new pulse sequences based on traditional analytical theories. This trend article summarises the key steps leading to these advancements. It also describes additional applications of optimal control beyond structural biology and envisions similar progress in the NMR of solid materials. Despite attractive features of optimal-control pulse sequences demonstrated in the proof-of-concept studies, their experimental utilization remains sparse, probably due to the lack of awareness among experimentalists. We hope this mini-review helps to spread optimal-control methods into routine experimental workflows. Furthermore, we offer a personal outlook on how numerical optimisations could in general enhance the experimental capabilities of solid-state NMR in the near future, with optimal control serving as a pioneer exploring new possibilities.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"135 ","pages":"Article 101984"},"PeriodicalIF":1.8,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142915579","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Spin-dynamics and efficiency of single 14N-1H cross-polarization at fast magic angle spinning in solids 固体中快速魔角自旋下单14N-1H交叉极化的自旋动力学和效率
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2025-01-28 DOI: 10.1016/j.ssnmr.2025.101992
Vipin Agarwal , Sreejith Raran-Kurussi , Yusuke Nishiyama
{"title":"Spin-dynamics and efficiency of single 14N-1H cross-polarization at fast magic angle spinning in solids","authors":"Vipin Agarwal ,&nbsp;Sreejith Raran-Kurussi ,&nbsp;Yusuke Nishiyama","doi":"10.1016/j.ssnmr.2025.101992","DOIUrl":"10.1016/j.ssnmr.2025.101992","url":null,"abstract":"<div><div>The naturally abundant <sup>14</sup>N isotope (&gt;99 %) is sparingly employed for characterization in solid-state nuclear magnetic resonance (NMR) despite the importance of nitrogen atoms in shaping molecular structures and properties. This inhibition can be attributed to large quadrupolar couplings (∼several MHz), resulting in more involved spin methodologies for <sup>14</sup>N nuclei. Experimentally, spin-½ nuclei are utilized for excitation and detection through two-way (<sup>1</sup>H→<sup>14</sup>N→<sup>1</sup>H) polarization transfer between spin-½ nuclei and <sup>14</sup>N. Herein, we show direct <sup>14</sup>N spin excitation followed by <sup>14</sup>N→<sup>1</sup>H cross-polarization (CP) is an efficient method for polarization transfer even for <sup>14</sup>N spins with a large quadrupolar coupling constant (3–4 MHz). This contrasts previous studies, which indicate that <sup>1</sup>H-<sup>14</sup>N spectra can only be observed with a pair of at least a rotor period-long symmetric <sup>14</sup>N pulses (<em>J. Chem. Phys. 151</em> (2019) <em>154202</em>). The <sup>14</sup>N→<sup>1</sup>H CP spin dynamics have been experimentally established and can be explained in analogy to spin-½ Hartmann-Hahn CP if visualized in the quadrupolar jolting frame. The <sup>14</sup>N→<sup>1</sup>H CP is ∼1.9–2.7 times more efficient in polarization transfer than other <sup>14</sup>N edited experiments. Considering shorter <sup>14</sup>N T<sub>1</sub> relaxation times compared to protons, <sup>14</sup>N edited spectra were recorded using <sup>14</sup>N→<sup>1</sup>H CP, resulting in enhanced sensitivity per unit of time.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"136 ","pages":"Article 101992"},"PeriodicalIF":1.8,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143376888","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Applications of NMR based methodologies investigating the behavior of lignin and cellulose towards bio-based carbon fibers production 应用基于核磁共振的方法研究木质素和纤维素在生物基碳纤维生产中的行为
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-11-21 DOI: 10.1016/j.ssnmr.2024.101977
Feryal Guerroudj , Lukas Fliri , Jenny Bengtsson , Leandro Cid Gomes , Tristan Gazzola , Michael Hummel , Diana Bernin
{"title":"Applications of NMR based methodologies investigating the behavior of lignin and cellulose towards bio-based carbon fibers production","authors":"Feryal Guerroudj ,&nbsp;Lukas Fliri ,&nbsp;Jenny Bengtsson ,&nbsp;Leandro Cid Gomes ,&nbsp;Tristan Gazzola ,&nbsp;Michael Hummel ,&nbsp;Diana Bernin","doi":"10.1016/j.ssnmr.2024.101977","DOIUrl":"10.1016/j.ssnmr.2024.101977","url":null,"abstract":"<div><div>Cellulose–lignin blends are proposed as alternative precursors for carbon fiber (CF) production, offering a potential sustainable and cost-effective alternative to the expensive fossil-based polymers currently used. The characteristics of the precursor fibers including their crystallinity, the incorporated chemical structures and the distribution of the biopolymers have a significant influence on their carbonization behavior and the properties of the CFs. They are partly determined by the composition of the bio-based resources and the conditions used during the fiber fixation, i.e. the coagulation, an important processing step. In this work, <sup>13</sup>C solid and 2D solution NMR methodologies were applied to investigate the impact of coagulation and thermostabilization conditions on cellulose and cellulose-lignin blends using a thin film model. Solid state NMR spectroscopy showed that the choice of the anti-solvent influenced the proportion of cellulose II <em>versus</em> amorphous regions in the coagulated films. Independent of the presence of lignin, the choice of anti-solvent seems to impact the rate of thermal reactions. After thermostabilization at 245 °C, the samples were investigated using a solution NMR protocol devised for cellulosic materials. At 275 °C, most of the samples became insoluble for solution NMR. However, solid state NMR revealed further changes in the chemical composition, which were dependent on both the presence of lignin and the choice of anti-solvent. This multi-faceted approach combining solid state and 2D solution NMR techniques provides a comprehensive understanding of the cellulose structure and the products formed for cellulose-lignin-based CFs, which is crucial for optimizing their properties and potential applications.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"134 ","pages":"Article 101977"},"PeriodicalIF":1.8,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142703422","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Solid-state NMR compositional analysis of sputum from people with cystic fibrosis 囊性纤维化患者痰液的固态核磁共振成分分析。
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-10-25 DOI: 10.1016/j.ssnmr.2024.101975
Kathy Duong , Evan Moss , Courtney Reichhardt
{"title":"Solid-state NMR compositional analysis of sputum from people with cystic fibrosis","authors":"Kathy Duong ,&nbsp;Evan Moss ,&nbsp;Courtney Reichhardt","doi":"10.1016/j.ssnmr.2024.101975","DOIUrl":"10.1016/j.ssnmr.2024.101975","url":null,"abstract":"<div><div>People with the genetic disease cystic fibrosis (CF) often have chronic airway infections and produce airway secretions called sputum. A better understanding of sputum composition is desired in order to track changes in response to CF therapeutics and to improve laboratory models for the study of CF airway infections. The glycosylated protein mucin is a primary component. Along with extracellular DNA, mucin gives rise to the high viscoelasticity of sputum, which inhibits airway clearance and is thought to promote chronic airway infections in people with CF. Past studies of sputum composition identified additional biomolecular components of sputum including other proteins, both glycosylated and not glycosylated, free amino acids, and lipids. Typically, studies of sputum, as well as other complex biological materials, have focused on soluble or isolated components. Solid-state NMR is not limited to the study of soluble components. Instead, it can provide molecular-level information about insoluble biological samples. Additionally, solid-state NMR can provide information about sample composition without requiring any processing of the sample, eliminating the possibility of misestimating certain components due to insolubility or potential sample loss in isolation steps. In this study, we used both <sup>13</sup>C and <sup>31</sup>P CPMAS to investigate the total composition of sputum samples obtained from six people with CF. We compared these spectra to those of commercially available mucin, DNA, and phospholipid samples. Lastly, we performed complementary biochemical analyses to identify specific proteins present in the sputum samples. Overall, our findings provide insight into the composition of unprocessed sputum samples from people with CF, which can be used as a benchmark for future investigations of CF and infections in the airways of people with CF. Further, this study provides opportunities to expand the solid-state NMR approach to include dynamic nuclear polarization (DNP) to obtain high-resolution information of sputum and similar biological samples that are not feasible to isotopically enrich.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"134 ","pages":"Article 101975"},"PeriodicalIF":1.8,"publicationDate":"2024-10-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142569403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Elucidating structure and metabolism of insect biomaterials by solid-state NMR 利用固态核磁共振阐明昆虫生物材料的结构和新陈代谢。
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-10-14 DOI: 10.1016/j.ssnmr.2024.101974
Christine Chrissian , Michael L. Stawski , Andrew P. Williams , Ruth E. Stark
{"title":"Elucidating structure and metabolism of insect biomaterials by solid-state NMR","authors":"Christine Chrissian ,&nbsp;Michael L. Stawski ,&nbsp;Andrew P. Williams ,&nbsp;Ruth E. Stark","doi":"10.1016/j.ssnmr.2024.101974","DOIUrl":"10.1016/j.ssnmr.2024.101974","url":null,"abstract":"<div><div>Among the many natural biomaterials for which information on atomic-level structure and reorientational motion can offer essential clues to function, insoluble multi-component composites with limited degrees of order are among the most challenging to study. Despite its limited sensitivity, solid-state NMR (ssNMR) is often the technique of choice to ferret out these details in carbon- and nitrogen-rich materials: this spectroscopic approach can probe many biomaterials in their native or near-native states, either with or without the introduction of stable NMR-active isotopes, or with the assistance of dynamic nuclear polarization technology. During a span of close to four decades, such research targets and ssNMR approaches have been exemplified by insects, a diverse and evolutionarily agile group of organisms with global impacts that include ecology, agriculture, and human disease. In this short review, we present case studies on insect cuticles that range from protective exoskeletons and egg capsules to the wing structures that enable flight and showcase nature's awe-inspiring beauty, highlighting the use of ssNMR spectroscopy to profile chemical composition, elucidate macromolecular architecture, and monitor metabolic development in these fascinating biological assemblies.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"134 ","pages":"Article 101974"},"PeriodicalIF":1.8,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142508285","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Glucose hydrochar consists of linked phenol, furan, arene, alkyl, and ketone structures revealed by advanced solid-state nuclear magnetic resonance 先进的固态核磁共振技术揭示的葡萄糖水碳由连接的苯酚、呋喃、芳香族化合物、烷基和酮结构组成
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-10-10 DOI: 10.1016/j.ssnmr.2024.101973
Shichen Yuan , Avery Brown , Zhaoxi Zheng , Robert L. Johnson , Karen Agro , Andrea Kruse , Michael T. Timko , Klaus Schmidt-Rohr
{"title":"Glucose hydrochar consists of linked phenol, furan, arene, alkyl, and ketone structures revealed by advanced solid-state nuclear magnetic resonance","authors":"Shichen Yuan ,&nbsp;Avery Brown ,&nbsp;Zhaoxi Zheng ,&nbsp;Robert L. Johnson ,&nbsp;Karen Agro ,&nbsp;Andrea Kruse ,&nbsp;Michael T. Timko ,&nbsp;Klaus Schmidt-Rohr","doi":"10.1016/j.ssnmr.2024.101973","DOIUrl":"10.1016/j.ssnmr.2024.101973","url":null,"abstract":"<div><div>The molecular structure of hydrochars produced from <sup>13</sup>C-enriched glucose under various conditions has been elucidated based on advanced one- and two-dimensional (2D) <sup>1</sup>H-<sup>13</sup>C and <sup>13</sup>C–<sup>13</sup>C solid-state nuclear magnetic resonance (NMR) with spectral editing. Regardless of synthesis conditions, hydrochars consist mostly of oxygen-substituted arene rings (including diphenols) and furans connected by alkyl linkers rich in ketones. Cross-linking nonprotonated and methyne (C-H) alkyl carbons have been identified through spectrally edited 2D NMR. Alkenes and ‘quaternary’ C-O are observed only at low synthesis temperature, while some clusters of fused arene rings are generated at high temperature. Hydrochar composition is nearly independent of reaction time in the range from 1 to 5 h. Equilibration of <sup>13</sup>C magnetization within 1 s shows that the materials are homogeneous on the 5-nm scale, refuting core–shell models of hydrochar microspheres. While furan C-O carbons bonded to alkyl groups or ketones show distinctive cross peaks in 2D NMR, phenolic C-OH is observed unambiguously by hydroxyl-proton selection. While methylene-linked furan rings are fairly common, the signal previously assigned to furan Cα-Cα linkages is shown to arise from abundant, stable catecholic <em>ortho</em>-diphenols, whose HO-C=C-OH structure is proved by 2D<sup>13</sup>C–<sup>13</sup>C NMR after hydroxyl-proton selection. Quantitative <sup>13</sup>C NMR spectra of low- and high-temperature hydrochars have been matched by chemical-shift simulations for representative structural models. Mixed phenol and furan rings connected by ketones and alkyl linkers provide good fits of the experimental spectra, while literature models dominated by large clusters of fused rings and with few phenols or alkyl-linked ketones do not.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"134 ","pages":"Article 101973"},"PeriodicalIF":1.8,"publicationDate":"2024-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142432093","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cryogenic probe technology enables multidimensional solid-state NMR of the stratum corneum without isotope labeling 低温探针技术无需同位素标记即可对角质层进行多维固态核磁共振成像。
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-09-21 DOI: 10.1016/j.ssnmr.2024.101972
Barbara Perrone , Maria Gunnarsson , Diana Bernin , Emma Sparr , Daniel Topgaard
{"title":"Cryogenic probe technology enables multidimensional solid-state NMR of the stratum corneum without isotope labeling","authors":"Barbara Perrone ,&nbsp;Maria Gunnarsson ,&nbsp;Diana Bernin ,&nbsp;Emma Sparr ,&nbsp;Daniel Topgaard","doi":"10.1016/j.ssnmr.2024.101972","DOIUrl":"10.1016/j.ssnmr.2024.101972","url":null,"abstract":"<div><div>Solid-state NMR has great potential for investigating molecular structure, dynamics, and organization of the <em>stratum corneum</em>, the outer 10–20 μm of the skin, but is hampered by the unfeasibility of isotope labelling as generally required to reach sufficient signal-to-noise ratio for the more informative multidimensional NMR techniques. In this preliminary study of pig <em>stratum corneum</em> at 35 °C and water-free conditions, we demonstrate that cryogenic probe technology offers sufficient signal boost to observe previously undetectable minor resonances that can be uniquely assigned to fluid cholesterol, ceramides, and triacylglycerols, as well as enables <sup>1</sup>H–<sup>1</sup>H spin diffusion monitored by 2D <sup>1</sup>H-<sup>13</sup>C HETCOR to estimate 1–100 nm distances between specific atomic sites on proteins and lipids. The new capabilities open up for future multidimensional solid-state NMR studies to answer long-standing questions about partitioning of additives, such as pharmaceutically active substances, between solid and liquid domains within the protein and lipid phases in the <em>stratum corneum</em> and the lipids of the sebum.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"134 ","pages":"Article 101972"},"PeriodicalIF":1.8,"publicationDate":"2024-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142366563","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
High-resolution 2D solid-state NMR provides insights into nontuberculous mycobacteria 高分辨率二维固态核磁共振有助于深入了解非结核分枝杆菌。
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-09-18 DOI: 10.1016/j.ssnmr.2024.101970
Chang-Hyeock Byeon , Kasper Holst Hansen , William DePas , Ümit Akbey
{"title":"High-resolution 2D solid-state NMR provides insights into nontuberculous mycobacteria","authors":"Chang-Hyeock Byeon ,&nbsp;Kasper Holst Hansen ,&nbsp;William DePas ,&nbsp;Ümit Akbey","doi":"10.1016/j.ssnmr.2024.101970","DOIUrl":"10.1016/j.ssnmr.2024.101970","url":null,"abstract":"<div><div>We present a high-resolution magic-angle spinning (MAS) solid-state NMR (ssNMR) study to characterize nontuberculous mycobacteria (NTM). We studied two different NTM strains, <em>Mycobacterium smegmatis</em>, a model, non-pathogenic strain, and <em>Mycobacterium abscessus</em>, an emerging and important human pathogen. Hydrated NTM samples were studied at natural abundance without isotope-labelling, as whole-cells versus cell envelope isolates, and native versus fixed sample preparations. We utilized 1D<sup>13</sup>C and 2D <sup>1</sup>H-<sup>13</sup>C ssNMR spectra and peak deconvolution to identify NTM cell-wall chemical sites. More than ∼100 distinct <sup>13</sup>C signals were identified in the ssNMR spectra. We provide tentative assignments for ∼30 polysaccharides by using well resolved <sup>1</sup>H/<sup>13</sup>C chemical shifts from the 2D INEPT-based <sup>1</sup>H-<sup>13</sup>C ssNMR spectrum. The signals originating from both the flexible and rigid fractions of the whole-cell bacteria samples were selectively analyzed by utilizing either CP or INEPT based <sup>13</sup>C ssNMR spectra. CP buildup curves provide insights into the dynamical similarity of the cell-wall components for NTM strains. Signals from peptidoglycan, arabinogalactan and mycolic acid were identified. The majority of the <sup>13</sup>C signals were not affected by fixation of the whole cell samples. The isolated cell envelope NMR spectrum overlap with the whole-cell spectrum to a large extent, where the latter has more signals. As an orthogonal way of characterizing these bacteria, electron microscopy (EM) was used to provide spatial information. ssNMR and EM data suggest that the <em>M. abscessus</em> cell-wall is composed of a smaller peptidoglycan layer which is more flexible compared to <em>M. smegmatis</em>, which may be related to its higher pathogenicity. Here in this work, we used high-resolution 2D ssNMR first time to characterize NTM strains and identify chemical sites. These results will aid the development of structure-based approaches to combat NTM infections.</div></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"134 ","pages":"Article 101970"},"PeriodicalIF":1.8,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142308575","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cooperative β-sheet coassembly controls intermolecular orientation of amphiphilic peptide-polydiacetylene conjugates β片协同组装控制着两亲肽-聚二乙烯共轭物的分子间取向
IF 1.8 3区 化学
Solid state nuclear magnetic resonance Pub Date : 2024-08-22 DOI: 10.1016/j.ssnmr.2024.101959
Tarunya Rao Sudarshan , Sujeung Lim , Jeffrey Li , Alicia S. Robang , Leel Mazal Liberty , Herdeline Ann M. Ardoña , Anant K. Paravastu
{"title":"Cooperative β-sheet coassembly controls intermolecular orientation of amphiphilic peptide-polydiacetylene conjugates","authors":"Tarunya Rao Sudarshan ,&nbsp;Sujeung Lim ,&nbsp;Jeffrey Li ,&nbsp;Alicia S. Robang ,&nbsp;Leel Mazal Liberty ,&nbsp;Herdeline Ann M. Ardoña ,&nbsp;Anant K. Paravastu","doi":"10.1016/j.ssnmr.2024.101959","DOIUrl":"10.1016/j.ssnmr.2024.101959","url":null,"abstract":"<div><p>In this work, we elucidated the structural organization of stimuli-responsive peptide-polydiacetylene (PDA) conjugates that can self-assemble as 1D nanostructures under neutral aqueous conditions. The amino acid sequences bear positively or negatively charged domains at the periphery of the peptide segments to promote solubility in water while also driving assembly of the individual and combined components into β-sheets. The photopolymerization of PDA, as well as the sensitivity of the resulting optical properties of the polymeric material to external stimuli, highly depends on the structural organization of the assembly of amphiphilic peptide-diacetylene units into 1D-nanostructures. Solid-state NMR measurements on <sup>13</sup>C-labeled and <sup>15</sup>N-labeled samples show that positively charged and negatively charged peptide amphiphiles are each capable of self-assembly, but self-assembly favors antiparallel β-sheet structure. When positively and negatively charged peptide amphiphiles interact in stoichiometric solutions, cooperative coassembly dominates over self-assembly, resulting in the desired parallel β-sheet structure with a concomitant increase in structural order. These results reveal that rational placement of oppositely charged residues can control β-strand organization in a peptide amphiphile coassembly, which would have implications on the adaptive properties of stimuli-responsive biomaterials such as the peptide-PDAs studied here.</p></div>","PeriodicalId":21937,"journal":{"name":"Solid state nuclear magnetic resonance","volume":"133 ","pages":"Article 101959"},"PeriodicalIF":1.8,"publicationDate":"2024-08-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142096517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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