Analytical Chemistry最新文献_第2页

Microflow Liquid Chromatography Coupled to Multinozzle Electrospray Ionization for Improved Lipidomics Coverage of 3D Clear Cell Renal Cell Carcinoma

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-25 DOI: 10.1021/acs.analchem.4c06337

Sergey Girel, Mathieu Galmiche, Mathis Fiault, Valentin Mieville, Patrycja Nowak-Sliwinska, Serge Rudaz, Isabel Meister

{"title":"Microflow Liquid Chromatography Coupled to Multinozzle Electrospray Ionization for Improved Lipidomics Coverage of 3D Clear Cell Renal Cell Carcinoma","authors":"Sergey Girel, Mathieu Galmiche, Mathis Fiault, Valentin Mieville, Patrycja Nowak-Sliwinska, Serge Rudaz, Isabel Meister","doi":"10.1021/acs.analchem.4c06337","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06337","url":null,"abstract":"In most bioanalytical laboratories, high-resolution mass spectrometry (HRMS) systems with electrospray ionization (ESI) are hyphenated to liquid chromatography platforms. The latter typically operate under analytical flow (AF; 0.2–1 mL/min) regimes. Hence, AF/ESI-HRMS methods prioritize the detection of analytes of higher abundances or ionizability and tend to suffer from matrix effects or ion suppression. A far higher sensitivity can be obtained with electrospray at nanoflow (10–1000 nL/min) thanks to a better ionization efficiency and significant decrease in matrix effects. Both advantages are crucial to reliably accessing low-abundance compounds or weakly ionizable analytes. This work presents a microflow (μF) chromatographic setup coupled to a novel microfabricated multinozzle electrospray (mnESI) emitter with five nozzles spraying at 600 nL/min per nozzle for untargeted HRMS lipidomic profiling. With a runtime of 19 min, similar to our established analytical flow (AF/ESI) lipidomics platform, μF/mnESI produced a 16-fold median increase across 69 deuterated lipid standards. The performance of this new configuration was also evaluated in the context of the profiling of a 3D clear cell renal cell carcinoma (ccRCC) model exposed to a multidrug combination therapy. The processing of the acquired data resulted in 1270 (μF/mnESI) vs 752 (AF/ESI) MS2-annotated lipids. Among those, 762 achieved <10% variation on pooled QC samples for μF/mnESI compared to only 361 for the AF method. In addition, the measurements of ccRCC samples confirmed the improvements in ionization efficiency and adduct patterns observed with standards, enabling to annotate 79 oxidized triglycerides, 38 cholesterol esters (only five and four detected in AF/ESI, respectively), and 12 sitosterol esters, not yet reported in mammalian cell cultures.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"27 7 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486570","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Application of Surface-Enhanced Raman Spectroscopy in Head and Neck Cancer Diagnosis.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-14 DOI: 10.1021/acs.analchem.4c02796

Bowen Yang, Xiaobo Dai, Shuai Chen, Chunjie Li, Bing Yan

{"title":"Application of Surface-Enhanced Raman Spectroscopy in Head and Neck Cancer Diagnosis.","authors":"Bowen Yang, Xiaobo Dai, Shuai Chen, Chunjie Li, Bing Yan","doi":"10.1021/acs.analchem.4c02796","DOIUrl":"10.1021/acs.analchem.4c02796","url":null,"abstract":"Surface-enhanced Raman spectroscopy (SERS) has emerged as a crucial analytical tool in the field of oncology, particularly presenting significant challenges for the diagnosis and treatment of head and neck cancer. This Review provides an overview of the current status and prospects of SERS applications, highlighting their profound impact on molecular biology-level diagnosis, tissue-level identification, HNC therapeutic monitoring, and integration with emerging technologies. The application of SERS for single-molecule assays such as epidermal growth factor receptors and PD-1/PD-L1, gene expression analysis, and tumor microenvironment characterization is also explored. This Review showcases the innovative applications of SERS in liquid biopsies such as high-throughput lateral flow analysis for ctDNA quantification and salivary diagnostics, which can offer rapid and highly sensitive assays suitable for immediate detection. At the tissue level, SERS enables cancer cell visualization and intraoperative tumor margin identification, enhancing surgical precision and decision-making. The role of SERS in radiotherapy, chemotherapy, and targeted therapy is examined along with its use in real-time pharmacokinetic studies to monitor treatment response. Furthermore, this Review delves into the synergistic relationship between SERS and artificial intelligence, encompassing machine learning and deep learning algorithms, marking the dawn of a new era in precision oncology. The integration of SERS with genomics, metabolomics, transcriptomics, proteomics, and single-cell omics at the multiomics level will revolutionize our comprehension and management of HNC. This Review offers an overview of the transformative impacts of SERS and examines future directions as well as challenges in this dynamic research field.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"3781-3798"},"PeriodicalIF":6.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143416719","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Fortified Donor–Acceptor Spectral Overlap Facilitated Fluorescence Quenching Efficiency for Developing Sensitive Nanometal Surface Energy Transfer-Based Immunochromatographic Test Strips

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-25 DOI: 10.1021/acs.analchem.4c06702

Xiya Zhang, Qianqian Cui, Mingyue Ding, Yexuan Mao, Xianqing Huang, Lianjun Song, Tong Bu

{"title":"Fortified Donor–Acceptor Spectral Overlap Facilitated Fluorescence Quenching Efficiency for Developing Sensitive Nanometal Surface Energy Transfer-Based Immunochromatographic Test Strips","authors":"Xiya Zhang, Qianqian Cui, Mingyue Ding, Yexuan Mao, Xianqing Huang, Lianjun Song, Tong Bu","doi":"10.1021/acs.analchem.4c06702","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06702","url":null,"abstract":"Constructing a fluorescence quenching immunochromatography test strip (FQ-ICTS) is conducive to sensitive point-of-care testing, yet inefficient quenching efficiency (QE) confines the progress of the FQ-ICTS. Herein an innovative nanometal surface energy transfer (NSET)-based FQ-ICTS with magnificent QE was proposed for the highly sensitive detection of T2 toxin utilizing time-resolved fluorescent microspheres (TRFMs) conjugated with T2-BSA as donors and monoclonal antibodies (mAbs) labeled with spherical and flower-shaped gold particles (AuNPs) as acceptors. As the key to biosensors, by regulating the distinct absorption wavelengths of AuNPs-mAb (520–605 nm), the effect of the donor–acceptor overlapping area on the QE was explored, and the NEST pair with the highest QE was screened out to achieve perfect sensitivity. It was found that the QE increased with the enlargement of the overlapping integral area. At the maximum spectral overlap area (4.68 × 1023 M–1 cm–1 nm4), the AuNPs-605 and TRFMs were the optimized NSET pair with the QE of up to 92.7%, and the described FQ-ICTS revealed a limit of detection reaching down to 0.034 ng/mL, which was a 13.2-fold improvement over that of a conventional AuNPs-ICTS, possessing favorable specificity and repeatability. Importantly, the proposed platform could be well-applied in a real maize sample for T2 monitoring with satisfactory recoveries (95.5% to 108.7%), correlating well with the results from HPLC-MS/MS. Concisely, this work demonstrates that the expansion of the donor–acceptor spectral overlap opens up distinct opportunities for the exploration of high QE acceptors and superior performance for an ICTS.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"15 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496130","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

N-Deficient B-Doped g-C₃N₄/CdS Heterojunction-Based PEC-FL Biosensor Assisted by CRISPR-Cas12a System for Ultrasensitive Determination of microRNA.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-13 DOI: 10.1021/acs.analchem.4c05841

Qingyu Du, Haoyu Zhang, Yingna Bi, Huijie Wang, Xuemin Zhou, Pengfei Shi, Shuzhen Lv, Sai Bi

{"title":"N-Deficient B-Doped g-C3N4/CdS Heterojunction-Based PEC-FL Biosensor Assisted by CRISPR-Cas12a System for Ultrasensitive Determination of microRNA.","authors":"Qingyu Du, Haoyu Zhang, Yingna Bi, Huijie Wang, Xuemin Zhou, Pengfei Shi, Shuzhen Lv, Sai Bi","doi":"10.1021/acs.analchem.4c05841","DOIUrl":"10.1021/acs.analchem.4c05841","url":null,"abstract":"Near-infrared light (NIR)-driven photoelectrochemical (PEC) processes are mainly faced with the limitation of weak photocurrents. Here, N-deficient B-doped g-C3N4/CdS (NB-g-C3N4/CdS) is proposed to construct a NIR-driven PEC biosensor assisted by CRISPR-Cas12a system for the determination of microRNA-21 (miRNA-21). To promote the optical absorption as well as the separation of photogenerated electrons and holes of g-C3N4, NB-g-C3N4/CdS is constructed via engineering the electronic and band structure in terms of N defect, B doping, and heterojunction, achieving high PEC performance. To obtain the high luminescence efficiency for exciting NB-g-C3N4/CdS under NIR, the core-shell NaYF4:Yb3+, Tm3+@NaYF4 upconversion nanoparticles (UCNPs) with repaired defects are prepared. Furthermore, the rolling circle amplification (RCA)-assisted CRISPR-Cas12a system is integrated to fragment the DNA on UCNPs, achieving sensitive detection of miRNA-21. On the one hand, the uncleavaged signal probes on UCNPs combined with NB-g-C3N4/CdS through π-π stacking interaction, generating photocurrents under the irradiation of NIR. On the other hand, the cleavaged signal probes which cannot link with NB-g-C3N4/CdS exhibited the fluorescence (FL) signals. The proposed PEC-FL dual-mode biosensor provides a mutual authentication of testing results and demonstrates ultrasensitivity (the detection limit of 1.1 fM for PEC mode and 7.0 fM for FL mode) and excellent specificity, which is promising in the clinical analysis of miRNA.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"4049-4056"},"PeriodicalIF":6.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Counterexample to Luminescent Metal Nanocluster Paradigm: Reactive Au(I) Complexes from His-Au(III) Synthetic Reactions and Their Chemistry for Direct Analysis of d-Penicillamine.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-14 DOI: 10.1021/acs.analchem.4c06202

Yuan Tong, Yanping Sun, Yelan Xiao, Yue Zou, Jingyang Guan, Xueji Zhang, Tong Shu

{"title":"Counterexample to Luminescent Metal Nanocluster Paradigm: Reactive Au(I) Complexes from His-Au(III) Synthetic Reactions and Their Chemistry for Direct Analysis of d-Penicillamine.","authors":"Yuan Tong, Yanping Sun, Yelan Xiao, Yue Zou, Jingyang Guan, Xueji Zhang, Tong Shu","doi":"10.1021/acs.analchem.4c06202","DOIUrl":"10.1021/acs.analchem.4c06202","url":null,"abstract":"There is a widely accepted material characterization paradigm in the success of synthesis of luminescent metal nanoclusters (NCs) in the aqueous phase: new emission, metal reduction, and ultrasmall particles (size < 3 nm). Herein, we falsified well-known fluorescent histidine (His)-directed Au NCs and a new model of metastable His-Au(I) complexes with emissive His oxidation products has been established. The redox reaction of His and Au(III) yields His oligomers with blue-green fluorescence and reducible Au(I) self-assemblies, which can form ultrasmall particles at electron bombardment. The resultant Au(I) complexes can be further reduced by d-penicillamine (DPA) via forming anisotropic Au nanoparticles with distinct local surface plasmon resonance absorption. The emerging absorption can quench the fluorescence of the His oxidation products through the inner filter effect pathway. A facile dual-model analytical approach is thus proposed to directly detect DPA fluorometrically and colorimetrically without interference from common biothiols, including cysteine and glutathione. Thus, with the help of a smartphone app, a highly sensitive and selective point-of-care testing for DPA direct detection can be realized. Our study warrants the importance of thinking twice about characterization results and supports corrective models for finding new reactions and possible applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"4092-4100"},"PeriodicalIF":6.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143416772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Exploring a New Ruthenium(II) Complex with High DNA Binding Ability as a Novel Efficient Luminescent Intercalation Agent to Construct a Label-Free ECL/PL Dual-Mode Biosensor

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-25 DOI: 10.1021/acs.analchem.5c00173

Yaoyao Xu, Rongxiu Deng, Junli Jia, Weiqiang Guo, Yuyang Zhou

{"title":"Exploring a New Ruthenium(II) Complex with High DNA Binding Ability as a Novel Efficient Luminescent Intercalation Agent to Construct a Label-Free ECL/PL Dual-Mode Biosensor","authors":"Yaoyao Xu, Rongxiu Deng, Junli Jia, Weiqiang Guo, Yuyang Zhou","doi":"10.1021/acs.analchem.5c00173","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00173","url":null,"abstract":"Ruthenium(II) complexes with special ligands have been widely recognized in numerous fields and attributed to their outstanding DNA binding capacity. Hybridization chain reaction (HCR), as an enzyme-free amplification technique, forms long double-stranded DNA (dsDNA) structures, which provides an intercalation platform for these complexes and obtains an effective enhancement of luminescent signals to a significant extent and enhances the sensitivity of detection. Hence, Ru(dip)2(tpphz) [dip = 4,7-diphenyl-1,10-phenanthroline, tpphz = tetrapyrido[3,2-a:2′,3′-c:3″,2″-h:2‴,3‴-j]phenazine] confirmed to possess high DNA binding capacity via UV–vis absorption spectroscopy and AutoDock theoretical simulation calculations was synthesized as a luminescence probe. As a proof of concept, the label-free ECL/PL dual-mode biosensor was further constructed. In this design, magnetic silica spheres with trigger DNA were amplified by HCR with hairpin DNA, forming large amounts of dsDNA on the surface, and Ru(dip)2(tpphz) was incorporated to generate robust signals. Trigger DNA was cleaved owing to the activation of Cas12a cleavage ability in the presence of the target, HCR amplification disappeared, and the signals reduced. The biosensor exhibited high selectivity, and the LOD was as low as 69 fM (S/N = 3). The results proved that Ru(dip)2(tpphz) has excellent DNA binding ability and ECL and PL dual properties, which has huge potential to establish label-free dual-mode biosensors and simultaneously offers a tremendous prospect in the fields of anticancer, gene therapy, and molecular probes beyond label-free biosensors in the future.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496136","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Voltammetry Prediction and Electrochemical Analysis of Carbon Material from "Salt-In-Water" to "Water-In-Salt".

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-01-31 DOI: 10.1021/acs.analchem.4c04764

Sukanlaya Kornnum, Praeploy Chomkhuntod, Nick Schwaiger, Kanwara Limcharoen, Krittapong Deshsorn, Kulpavee Jitapunkul, Pawin Iamprasertkun

{"title":"Voltammetry Prediction and Electrochemical Analysis of Carbon Material from \"Salt-In-Water\" to \"Water-In-Salt\".","authors":"Sukanlaya Kornnum, Praeploy Chomkhuntod, Nick Schwaiger, Kanwara Limcharoen, Krittapong Deshsorn, Kulpavee Jitapunkul, Pawin Iamprasertkun","doi":"10.1021/acs.analchem.4c04764","DOIUrl":"10.1021/acs.analchem.4c04764","url":null,"abstract":"Cyclic voltammetry (CV) is a standard method for assessing electrochemical properties in the electrochemical cells, typically in conventional aqueous contexts like 1 m solutions (\"salt-in-water\"). However, recent advancements have extended electrochemistry into superconcentrated regimes, such as \"water-in-salt\" solutions with concentrations above 10 to 20 m, which require large amounts of salt for experiments. To address this, machine learning (ML) has been applied, coupled with in-house data collection using lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) electrolytes. This work demonstrates the electrochemistry of YEC-8B in LiTFSI, given their broad potential window of up to 3.0 V across concentrations from 1 to 20 m. The CV profiles were divided into two models: the upper curve for charging and the lower curve for discharging. Data were normalized and segmented by percentiles, and a decision tree model was developed to predict outputs based on input parameters like LiTFSI concentration, scan rates, and potential window. The model predicted nine target variables with a mean absolute percentage error of approximately 2% for both the upper and the lower CV profile curves. Trapezoidal rule was then used to calculate the system's capacitance. Additionally, tests showed a 75% accuracy in predicting the potential window and a suitable scan rate. Overall, the model effectively demonstrated the relationship between \"water-in-salt\" electrolytes and CV profiles in an electrochemical context using a simple machine learning (ML) algorithm, which continues to expand the integration of data science and electrochemistry.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"3881-3891"},"PeriodicalIF":6.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143062179","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Reactive Oxygen Species (ROS)-Tyrosinase Cascade-Activated Near-Infrared Fluorescent Probe for the Precise Imaging of Melanoma.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-13 DOI: 10.1021/acs.analchem.5c00018

Ruidian Lv, Sitong Hang, Yuran Zhao, Weijie Gao, Peng Zhang, Ke Zheng, Qian Zhang, Caifeng Ding

引用次数: 0

Computer-Aided Design of 3D Non-Enzymatic Catalytic Cascade Systems for In Situ Multiplexed mRNA Imaging in Single-Cells.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-14 DOI: 10.1021/acs.analchem.4c06589

Yun Wen, Li-Ping Wang, Jian-Hua Wang, Yong-Liang Yu, Shuai Chen

{"title":"Computer-Aided Design of 3D Non-Enzymatic Catalytic Cascade Systems for In Situ Multiplexed mRNA Imaging in Single-Cells.","authors":"Yun Wen, Li-Ping Wang, Jian-Hua Wang, Yong-Liang Yu, Shuai Chen","doi":"10.1021/acs.analchem.4c06589","DOIUrl":"10.1021/acs.analchem.4c06589","url":null,"abstract":"mRNA, a critical biomarker for various diseases and a promising target for cancer therapy, is central to biological and medical research. However, the development of multiplexed approaches for in situ monitoring of mRNA in live cells are limited by their reliance on enzyme-based signal amplification, challenges with in situ signal diffusion, and the complexity of nucleic acid design. In this study, we introduce a nonenzymatic catalytic DNA assembly (NEDA) technique to address these limitations. NEDA facilitates the precise in situ imaging of intracellular mRNA by assembling three free hairpin DNA amplifiers into a low-mobility, three-dimensional DNA spherical structure. This approach also enables the simultaneous detection of four distinct targets via the combination of fluorescent signals, with a detection limit as low as 141.2 pM for target mRNA. To enhance the efficiency of nucleic acid design, we employed computer-aided design (CAD) to rapidly generate feasible sequences for highly multiplexed detection. By integrating various machine learning algorithms, we achieved impressive accuracy of nearly 96.66% in distinguishing multiple cell types and 87.80% in identifying the same cell type under different drug stimulation conditions. Notably, our platform can also identify drug stimuli with similar mechanisms of action, highlighting its potential in drug development. This multiplexed 3D assembly sensing strategy with CAD not only enhances the ability to image nucleic acid sequences in situ simultaneously but also provides a novel platform for efficient molecular diagnostics and personalized therapy.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"4176-4184"},"PeriodicalIF":6.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412338","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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

Exploring the Effect of Nanopore Microstructures on Crystallization and the Evolution of Molecular Assembly Structure by ¹⁹F Solid-State Nuclear Magnetic Resonance Spectroscopy.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-13 DOI: 10.1021/acs.analchem.4c06353

Keke Zhang, Mengyang Cai, Mengwei Wang, Pengpeng Yang, Kongying Zhu, Zhenfu Wang, Junbo Gong, Hanjie Ying

{"title":"Exploring the Effect of Nanopore Microstructures on Crystallization and the Evolution of Molecular Assembly Structure by 19F Solid-State Nuclear Magnetic Resonance Spectroscopy.","authors":"Keke Zhang, Mengyang Cai, Mengwei Wang, Pengpeng Yang, Kongying Zhu, Zhenfu Wang, Junbo Gong, Hanjie Ying","doi":"10.1021/acs.analchem.4c06353","DOIUrl":"10.1021/acs.analchem.4c06353","url":null,"abstract":"The pore microstructure of mesoporous materials has a vital influence on molecular movement and assembly as well as crystallization. Nonetheless, previous studies have predominantly concentrated on the impact of pore size and pore shape on molecular assembly and nucleation outcomes; investigations delving into the effects of more complex pore structures on molecular assembly and nucleation behaviors were absent. In this study, evolution of the molecular self-assembly process of flufenamic acid (FFA) confined in mesoporous materials with different microstructures was monitored by in situ 19F solid-state NMR spectroscopy. It was demonstrated that tortuosity, as a microstructural parameter of porous materials, has the ability to determine the molecular assembly process and nucleation behaviors of FFA. The results indicated that molecules in pores with high tortuosity tend to aggregate to an amorphous plug, while those in less tortuous nanopores are inclined to adsorb on the pore surface forming molecular layers. Besides that, this work provides the first direct proof that a mixture of two molecular layer structures exists on the FFA-silica surface through 19F solid-state NMR spectroscopy. This study explores the relationship between the microstructure of porous materials and molecular assembly, which can inform drug delivery, electronic deposition, and biomineralization.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"4120-4127"},"PeriodicalIF":6.7,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143412340","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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