Ligang Xu , Wenda Zhang , Chenjie Lou , Chenxu Geng , Yuxiu Sun , Jie Liu , Yongchao Shi , Huajie Luo , Jipeng Fu , Haiyan Zheng , Mingxue Tang
{"title":"Revealing structure correlation between ionic liquid and metal-organic framework matrix","authors":"Ligang Xu , Wenda Zhang , Chenjie Lou , Chenxu Geng , Yuxiu Sun , Jie Liu , Yongchao Shi , Huajie Luo , Jipeng Fu , Haiyan Zheng , Mingxue Tang","doi":"10.1016/j.mrl.2023.12.003","DOIUrl":"10.1016/j.mrl.2023.12.003","url":null,"abstract":"<div><p>Solid-state batteries are rising rapidly in response to the fast-increasing energy demand. Metal-organic framework (MOF) loaded with ionic liquids has brought new opportunities for solid-state batteries owing to its good interfacial compatibility and high ionic conductivity. MOF-808 is selected to be filled with Li-contained ionic liquid for structure and ion dynamics investigation using nuclear magnetic resonance (NMR) and X-ray diffraction. This study finds that the introduced ionic liquid would partially soften the matrix of MOF-808 and thus yield amorphous phase. By selective isotope replacement under cycling symmetric <sup>6</sup>Li metal cell, Li<sup>+</sup> ion is observed to mainly go cross ionic liquid in the open channel of matrix under potential polarization.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 2","pages":"Article 100095"},"PeriodicalIF":0.0,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516224000020/pdfft?md5=b55282bb5d9072c27f0c79257107412f&pid=1-s2.0-S2772516224000020-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139394408","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Operando NMR methods for studying electrocatalysis","authors":"Zhiyu Zhu, Ruipeng Luo, Evan Wenbo Zhao","doi":"10.1016/j.mrl.2023.12.004","DOIUrl":"10.1016/j.mrl.2023.12.004","url":null,"abstract":"<div><p>The combination of electrochemical measurements with spectroscopic characterizations provides valuable insights into reaction mechanisms. Nuclear magnetic resonance (NMR) spectroscopy, as a powerful technique due to its atomic specificity and versatility in studying gas, liquid, and solid, allows the study of electrolyte solution, catalyst and catalyst-adsorbate interfaces. When applied in <em>operando</em>, NMR can offer molecular-level insights into various electrochemical processes. <em>Operando</em> NMR has been applied extensively in battery research, but relatively underexplored for electrocatalysis in the past two decades. In this mini review, we first introduce the <em>operando</em> electrochemical NMR setups, categorized by different probe designs. Then we review the applications of <em>operando</em> NMR for monitoring the electrolyte solution and the catalyst-adsorbate interface. Considering the high environmental impact of electrochemical conversion of CO<sub>2</sub> into value-added products, we zoom in to the use of <em>operando</em> NMR in studying electrochemical CO<sub>2</sub> reduction. Finally, we provide our perspective on further developing and applying <em>operando</em> NMR methods for understanding the complex reaction network of Cu-catalyzed electrochemical CO<sub>2</sub> reduction.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 2","pages":"Article 100096"},"PeriodicalIF":0.0,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516224000032/pdfft?md5=6e8045bc26f18bbbb054d13d27f355ad&pid=1-s2.0-S2772516224000032-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139454451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Solid-state NMR study on sodium intercalation at low voltage window for Na3V2(PO4)3 as an anode","authors":"Yuxin Liao, Fushan Geng, Ming Shen, Bingwen Hu","doi":"10.1016/j.mrl.2023.12.001","DOIUrl":"https://doi.org/10.1016/j.mrl.2023.12.001","url":null,"abstract":"<div><p><em>In-situ</em> XRD, <sup>31</sup>P NMR and <sup>23</sup>Na NMR were used to analyze the interaction behavior of Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> at low voltage, and then a new intercalation model was proposed. During the transition from Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> to Na<sub>4</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>, Na ions insert into M1, M2 and M3 sites simultaneously. Afterwards, during the transition of Na<sub>4</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> to Na<sub>5</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>, Na ions mainly insert into M3 site.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 2","pages":"Article 100093"},"PeriodicalIF":0.0,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516223000670/pdfft?md5=2860728b32267e08ac7b745c97e5b038&pid=1-s2.0-S2772516223000670-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141078046","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Experimental aspects of 14N overtone RESPDOR solid-state NMR spectroscopy under MAS beyond 60 kHz","authors":"Yutaro Ogaeri, Yusuke Nishiyama","doi":"10.1016/j.mrl.2023.12.002","DOIUrl":"10.1016/j.mrl.2023.12.002","url":null,"abstract":"<div><p>Nitrogen-14 (<sup>14</sup>N) overtone (OT) spectroscopy under fast magic angle spinning (MAS) conditions (>60 kHz) has emerged as a powerful technique for observing correlations and distances between <sup>14</sup>N and <sup>1</sup>H, owing to the absence of the first-order quadrupolar broadenings. In addition, <sup>14</sup>N<sup>OT</sup> allows selective manipulation of <sup>14</sup>N nuclei for each site. Despite extensive theoretical and experimental studies, the spin dynamics of <sup>14</sup>N<sup>OT</sup> remains under debate. In this study, we conducted experimental investigations to assess the spin dynamics of <sup>14</sup>N<sup>OT</sup> using the rotational-echo saturation-pulse double-resonance (RESPDOR) sequence, which monitors population transfer induced by a<sup>14</sup>N<sup>OT</sup> pulse. The <sup>14</sup>N<sup>OT</sup> spin dynamics is well represented by a model of a two-energy-level system. Unlike spin-1/2, the maximum excitation efficiency of <sup>14</sup>N<sup>OT</sup> coherences of powdered solids, denoted by <em>p</em>, depends on the radiofrequency field (rf-field) strength due to orientation dependence of effective nutation fields even when pulse lengths are optimized. It is also found that the <em>p</em> factor, contributing to the <sup>14</sup>N<sup>OT</sup> spin dynamics, is nearly independent of the <em>B</em><sub>0</sub> field. Consequently, the filtering efficiency of RESPDOR experiments exhibits negligible dependence on <em>B</em><sub>0</sub> when the <sup>14</sup>N<sup>OT</sup> pulse length is optimized. The study also identifies the optimal experimental conditions for <sup>14</sup>N<sup>OT</sup>/<sup>1</sup>H RESPDOR correlation experiments.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 1","pages":"Article 100094"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516224000019/pdfft?md5=9a4f60e3a6dca75955692e66d827a99f&pid=1-s2.0-S2772516224000019-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139393896","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Andrés Ramírez Aguilera , Florin Marica , Kevin J. Sanders , Md Al Raihan , C. Adam Dyker , Gillian R. Goward , Bruce J. Balcom
{"title":"Multinuclear MR and MRI study of lithium-ion cells using a variable field magnet and a fixed frequency RF probe","authors":"Andrés Ramírez Aguilera , Florin Marica , Kevin J. Sanders , Md Al Raihan , C. Adam Dyker , Gillian R. Goward , Bruce J. Balcom","doi":"10.1016/j.mrl.2023.11.002","DOIUrl":"10.1016/j.mrl.2023.11.002","url":null,"abstract":"<div><p>An exploratory multinuclear magnetic resonance (MR) and magnetic resonance imaging (MRI) study was performed on lithium-ion battery cells with <sup>7</sup>Li, <sup>19</sup>F, and <sup>1</sup>H measurements. A variable field superconducting magnet with a fixed frequency parallel-plate radiofrequency (RF) probe was employed in the study. The magnetic field was changed to set the resonance frequency of each nucleus to the fixed RF probe frequency of 33.7 MHz. Two cartridge-like lithium-ion cells, with graphite anodes and LiNi<sub>0.5</sub>Mn<sub>0.3</sub>Co<sub>0.2</sub>O<sub>2</sub> (NMC) cathodes, were interrogated. One cell was pristine, and one was charged to a cell voltage of 4.2 V. The results presented demonstrate the great potential of the variable field magnet approach in multinuclear measurement of lithium-ion batteries. These methods open the door for developing faster and simpler methods for detecting, quantifying, and interpreting MR and MRI data from lithium-ion and other batteries.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 1","pages":"Article 100090"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516223000645/pdfft?md5=09065aef35eb0cafacf873c791cc09e0&pid=1-s2.0-S2772516223000645-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138608341","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenbo Dong , Qi Zhao , Jiancheng Zhao , Jiarong Zhang , Yingxiong Wang , Yan Qiao
{"title":"Qualitative analysis of aromatic compounds via 1D TOCSY techniques","authors":"Wenbo Dong , Qi Zhao , Jiancheng Zhao , Jiarong Zhang , Yingxiong Wang , Yan Qiao","doi":"10.1016/j.mrl.2023.11.003","DOIUrl":"10.1016/j.mrl.2023.11.003","url":null,"abstract":"<div><p>The aromatic compounds, including <em>o</em>-xylene, <em>m</em>-xylene, <em>p</em>-xylene, and ethylbenzene, primarily originate from the catalytic reforming of crude oil, and have a wide variety of applications. However, because of similar physical and chemical properties, these compounds are difficult to be identified by gas chromatography (GC) without standard samples. With the development of modern nuclear magnetic resonance (NMR) techniques, NMR has emerged as a powerful and efficient tool for the rapid analysis of complex and crude mixtures without purification. In this study, the parameters of one-dimensional (1D) total correlation spectroscopy (TOCSY) NMR techniques, including 1D selective gradient TOCSY and 1D chemical-shift-selective filtration (CSSF) with TOCSY, were optimized to obtain comprehensive molecular structure information. The results indicate that the overlapped signals in NMR spectra of nonpolar aromatic compounds (including <em>o</em>-xylene, <em>m</em>-xylene, <em>p</em>-xylene and ethylbenzene), polar aromatic compounds (benzyl alcohol, benzaldehyde, benzoic acid), and aromatic compounds with additional conjugated bonds (styrene) can be resolved in 1D TOCSY. More importantly, full molecular structures can be clearly distinguished by setting appropriate mixing time in 1D TOCSY. This approach simplifies the NMR spectra, provides structural information of entire molecules, and can be applied for the analysis of other structural isomers.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 1","pages":"Article 100091"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516223000657/pdfft?md5=79c75a54fe173e6197e711ad69a543fd&pid=1-s2.0-S2772516223000657-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138625366","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuqi Xiong , Zishuo Wu , Lei Wu , Chengyan Li , Wei Chen
{"title":"Rheo-NMR: A versatile hyphenated technique for capturing molecular dynamics and structure under flow","authors":"Yuqi Xiong , Zishuo Wu , Lei Wu , Chengyan Li , Wei Chen","doi":"10.1016/j.mrl.2023.10.002","DOIUrl":"10.1016/j.mrl.2023.10.002","url":null,"abstract":"<div><p>The general development of Rheo-NMR during the last four decades as well as selective hyphenated apparatuses is presented. Based on different magnet types, the current review is divided into two categories, namely low-field and high-field NMR, while the time-domain NMR is normally applied in the former case and the frequency-domain NMR is adopted in the latter one. Depending on different rheometer cells, it can be further divided into tensile and shear mode Rheo-NMR. The combination of various rheometer cells and NMR facility guarantees our acquisition of molecular level structure and dynamics information under flow conditions, which is crucial for our understanding of the molecular origin of complex fluids. A personal perspective is also presented at last to highlight possible development in this direction.</p></div>","PeriodicalId":93594,"journal":{"name":"Magnetic Resonance Letters","volume":"4 1","pages":"Article 100088"},"PeriodicalIF":0.0,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772516223000621/pdfft?md5=74b31f694e678e0b709496cd82b70e83&pid=1-s2.0-S2772516223000621-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136093842","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}