Analytical Chemistry最新文献

{"title":"Cantilever-Enhanced Fiber-Optic Photoacoustic Spectrophone for Low-Pressure Gas Detection.","authors":"Chenxi Li, Xiao Han, Min Guo, Hongchao Qi, Jingya Zhang, Xinyu Zhao, Ke Chen","doi":"10.1021/acs.analchem.4c05422","DOIUrl":"10.1021/acs.analchem.4c05422","url":null,"abstract":"<p><p>A cantilever-enhanced fiber-optic photoacoustic (PA) spectrophone is reported for trace gas detection at a low-pressure environment. A cantilever-based fiber-optic Fabry-Perot (F-P) interferometer (FPI) is utilized for simultaneous measurement of air pressure and PA pressure. Since the cantilever resonance frequency follows air pressure linearly, the fundamental frequency intensity modulation (1<i>f</i>-IM) technique is applied to scan the frequency response of the solid PA signal from tube wall absorption for tracking the cantilever resonance frequency in real time. The second-harmonic wavelength modulation spectroscopy (2<i>f</i>-WMS) technique is used to measure the gas PA pressure wave at the cantilever resonance. According to the inverse restriction relationship of air pressure on the PA excitation and cantilever detection, the measured gas PA signal at the low-pressure environment is enhanced. The target gas concentration is corrected by the measured air pressure, which makes the spectrophone generally applicable under any pressure. The experimental results indicate that the normalized noise equivalent absorption (NNEA) coefficients of the spectrophone in the standard atmospheric pressure and the low-pressure environment of 60 kPa are 2.2 × 10^-9 and 2.0 × 10^-9 cm^-1·W·Hz^-1/2, respectively. 0.1 ppm acetylene (C₂H₂) can be detected at any air pressure. The detected maximum relative error of 10 ppm C₂H₂ gas under different pressures is less than ±9% and the error is reduced to less than ±2% when the concentration rises to 70 ppm. In the pressure range of 60-100 kPa, the cantilever-enhanced fiber-optic PA spectrophone has extremely high accuracy and pressure stability, covering the pressure range of most ground gas detection scenes.</p>","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"838-847"},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142913088","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}

{"title":"Smart and Noninvasive SERS Immunosensors for Monitoring Dynamic Expression of Cytokines during Cell Pyroptosis","authors":"Chenyu Zhang, Zutao Chen, Guohua Qi, Yu Tian, Xiongjian Zheng, Xingkang Diao, Jiao Kong, Xingkai Ju, Jing Li, Shaojun Dong, Yongdong Jin","doi":"10.1021/acs.analchem.4c05539","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05539","url":null,"abstract":"Accompanying the occurrence of inflammatory reaction to release cytokines, pyroptosis can activate an immune response for resistance against cancer. Consequently, elevated levels of cytokines released by cancer cells are highly correlated with the effectiveness of cancer treatment. Herein, a noninvasive surface-enhanced Raman spectroscopy (SERS) immunosensor was developed to sensitively and specifically measure the tumor necrosis factor-α (TNF-α), a proinflammatory cytokine, during the cell pyroptosis process. The sandwiched structure of the sensor is functionalized with a TNF-α binding antibody for detecting TNF-α at concentrations as low as 1 pg/mL. Importantly, electrical stimulation (ES) can fleetly trigger cancer cell pyroptosis to induce the overexpression of receptor interacting protein 3 (RIP3), which is a significant protein that regulates the inflammatory response. The overexpression of RIP3 can activate caspase-1 to promote the upregulation of cytokine levels. Notably, the cytokine levels of TNF-α released from cancer cells (MCF-7 cells) were apparently higher than those of normal cells (MCF-10A cells) during pyroptosis detected by the SERS immunosensors. Due to its obvious superiorities of simple fabrication and fast readout without sample pretreatment, the developed SERS platform has a potential application value for diagnosis and treatment of cancer.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"43 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981261","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}

{"title":"DACH-Based Chiral Sensing Platforms as Tunable Benzamide-Chiral Solvating Agents for NMR Enantioselective Discrimination","authors":"Shuai-Hua Shi, Xiao-Juan Wang, Yuan-Yuan Gao, Tao Wang, Chun-Yu Wang, Zi Wang, Qiang Wang, Fei Li, Gao-Wei Li","doi":"10.1021/acs.analchem.4c06024","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06024","url":null,"abstract":"Chiral discrimination is an indispensable tool that has pivotal importance in the assignment of absolute configuration and determination of enantiomeric excess in chiral compounds. A series of enantiomerically pure <i>trans</i>-1,2-diaminocyclohexane (<i>trans</i>-DACH)-derived benzamides were first synthesized by simple chemical steps, and 14 variated derivatives <b>6a–6n</b> have been assessed as NMR chiral solvating agents (CSAs) for discrimination of the signals of mandelic acid (MA) in ¹H NMR analysis. The highly efficient chiral recognition of CSA <b>6e</b> on different substrates, including MAs, carboxylic acids, amino acid derivatives, and phosphoric acids (32 examples), was expanded via ¹H, ¹⁹F, and ³¹P NMR spectroscopy. The quality of enantiodiscrimination was evaluated by means of the enantioresolution parameter <i>R</i>_s. Single-crystal X-ray analysis of three derivatives <b>6c</b>, <b>6e</b>, and <b>6h</b> helped to understand enantiomeric recognition for the promising NMR analysis. Interestingly, the NMR signals of nonequivalent protons between the <i>R</i> and <i>S</i> configurations were completely opposite in the presence of CSA <b>6e</b> and its stereoisomer, which can be utilized to establish a straightforward method for the configuration assignment of diverse hydroxy acid substrates.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"1 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981256","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}

{"title":"A Highly Selective Probe for Real-Time Monitoring of Ethylenediamine with Ratiometric Luminescent and Colorimetric Dual-Mode Responses","authors":"Qian Zhou, Xiurong Ma, Xian Meng, Runying He, Caihong Shi, Yonggang Shi, Qiue Cao, Liyan Zheng","doi":"10.1021/acs.analchem.4c04080","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04080","url":null,"abstract":"Ethylenediamine (EDA), as an important chemical raw material and fine chemical intermediate, has been widely applied in various industries. Real-time monitoring of EDA is highly desirable in daily life due to its potential threat to human health. Herein, we report a molecular probe named 4,4′-(9<i>H</i>-carbazole-3,6-diyl)bis(1-(naphthalen-2-ylmethyl)pyridin-1-ium) iodide (p-N-DPC·I₂) with ratiometric luminescent and colorimetric dual-mode responses toward EDA, endowing a highly sensitive and selective detection method for its real-time monitoring. The experimental and theoretical calculation results revealed that the response mechanism was due to forming a charge transfer (CT) state when p-N-DPC·I₂ met with EDA. In addition, a hydrogel-based sensing chip was developed to achieve the ultrasensitive recognition of EDA vapor with the naked eye at a concentration as low as 10 ppm. This study developed a new probe with ratiometric fluorescent and colorimetric modes to detect EDA both in solution and vapor.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"68 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975339","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}

{"title":"Unveiling Microscopic Variations during Photodynamic Therapy via Polarity-Responsive Fluorescence Lifetime Imaging","authors":"Wei Quan, Qian Zhang, Huawei Huang, Weiying Lin","doi":"10.1021/acs.analchem.4c04615","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04615","url":null,"abstract":"Photodynamic therapy is a highly promising method for cancer adjuvant treatment. However, the current research on the microscopic changes during the photodynamic therapy process is still quite limited, which seriously impedes the deep understanding of the procedure. For this purpose, a novel polarity-responsive probe, <b>MI-PPF</b>, with excellent mitochondrial targeting and anchoring capabilities has been rationally designed and synthesized. Notably, <b>MI-PPF</b> has successfully realized the <i>in situ</i> detection of mitochondrial morphology and polarity alterations during the photodynamic therapy process in cancer cells through fluorescence lifetime imaging. The results showed that a series of phenomena such as deformation, shrinkage, vacuolation, and aggregation occurred in the mitochondrial morphology during photodynamic therapy. Concurrently, a decline in mitochondrial polarity is also noted, which may be closely linked to the mitochondrial oxidative stress response during this process. Furthermore, <b>MI-PPF</b> can be used for photodynamic therapy on tumor mouse models and has successfully achieved fluorescence lifetime imaging of tumor sections before and after photodynamic therapy, uncovering multifaceted changes in cell morphology, polarity, and polarity distribution within the mouse tumor model during the process. It is anticipated that this study will offer valuable insights and guidance to the research of mitochondrial-related fields and will boost the advancement of diagnostic and therapeutic areas for associated diseases.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"52 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975341","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}

{"title":"Correction to “Controlled Release of Drugs from Gradient Hydrogels for High-Throughput Analysis of Cell–Drug Interactions”","authors":"Serge Ostrovidov, Nasim Annabi, Azadeh Seidi, Murugan Ramalingam, Fariba Dehghani, Hirokazu Kaji, Ali Khademhosseini","doi":"10.1021/acs.analchem.5c00172","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00172","url":null,"abstract":"In the original version of this article, some of the representative live/dead images were inadvertently repeated in Figure 4B–D. These panels were composed of several individual images that the authors manually stacked together to display the entire hydrogel area from top to bottom. To validate our data, we repeated the experiments presented in Figure 4B–D and would like to include the new data to address this concern. The incorporation of these updated panels does not alter the interpretation of the data or the conclusions of the study but serves to confirm the accuracy of the published work by the authors. We apologize for this error. Figure 4. Effect of drug on cell viability. Fluorescent micrographs of 3T3 cells cultured in a multiwell plate and treated with (B) PEGDA hydrogel without OA (negative control), (C) with 2 μM OA (positive control), and (D) with an OA concentration gradient. Dead cells are marked in red by ethidium bromide, while living cells are marked in green by calcein-AM. This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"205 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975462","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}

{"title":"Exploring the Chiral Match–Mismatch Effect in the Chiral Discrimination of Nitriles","authors":"Guangxing Gu, Yining Sun, Chenyang Wang, Yilin Zeng, Tianci Peng, Byungjin Koo, Yanchuan Zhao","doi":"10.1021/acs.analchem.4c06117","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06117","url":null,"abstract":"This study tackles the challenge of enantiodifferentiation of nitrile compounds, which is typically difficult to resolve using nuclear magnetic resonance (NMR) due to the significant distance between the chiral center and the nitrogen atom involved in molecular interactions. We have developed novel chiral ¹⁹F-labeled probes, each featuring two chiral centers, to exploit the “match–mismatch” effect, thereby enhancing enantiodiscrimination. This strategy effectively differentiates chiral analytes with quaternary chiral carbon centers as well as those with similar substituents at the chiral center. Our approach not only provides a novel method for precise probe performance optimization but also offers a rapid and efficient technique for screening reaction conditions in asymmetric synthesis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"36 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981260","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}

{"title":"Welcome to 2025","authors":"Jonathan Sweedler","doi":"10.1021/acs.analchem.4c07065","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c07065","url":null,"abstract":"As I look forward to 2025, which marks the publication of &lt;i&gt;Analytical Chemistry’s&lt;/i&gt; 97th volume, I find myself also reflecting on some recent successes. I am in my 19th year with &lt;i&gt;Analytical Chemistry&lt;/i&gt;─14 as the Editor-in-Chief (EIC) and five as an Associate Editor (AE)─and the one constant over this period has been growth. The number of manuscript submissions has more than doubled since I become EIC, with an 18% increase in 2024 alone! To give a little historical perspective to how much we have grown, in 1930, 1960, and 1990, we published 420, 2400, and 4000 pages, respectively. In 2020, we published more than 16,000 pages and 2024 is the first year to ever exceed 20,000 pages! &lt;i&gt;Analytical Chemistry&lt;/i&gt; has played an important role in helping us keep up with our field over the last century─and in three years, we will be celebrating our 100th anniversary! But that is a topic for a future editorial (and some fun celebrations). Not only has the journal experienced continued growth, the demographics of our corresponding authors have shifted. In 2011, 46% of our publications were from the Western Hemisphere, 28% from Europe, and 26% from Asia. In 2024, Asia accounted for more than two-thirds of our manuscript’s corresponding authors. In keeping with our increase in manuscript submissions, we have further expanded our editorial team. Jürgen Popp from Friedrich Schiller University (Germany) became an AE in 2024, and in January 2025 we welcome two new AEs from China, Lihua Zhang, Dalian Institute of Chemical Physics and Xiaobing Zhang, Hunan University. I expect one more AE to join us during 2025 so that we reach our full complement of talented editors to handle the breadth and number of submissions. I am also pleased to say that the measurement science brand at ACS Publications continues to thrive. In 2023, the new journal &lt;i&gt;Chemical &amp; Biomedical Imaging&lt;/i&gt; was started; this is a partnership between the ACS and Nanjing University. In 2024, &lt;i&gt;ACS Electrochemistry&lt;/i&gt; was launched, with its first full issue published in January 2025. Congratulations to its new Editor-in-Chief Patrick Unwin, and here is to the journal’s successful first year! Besides publishing research articles advancing chemical measurement science, &lt;i&gt;Analytical Chemistry&lt;/i&gt; partners with other ACS measurement science journals to award the Advances in Measurement Science Lectureships. In addition, &lt;i&gt;Analytical Chemistry&lt;/i&gt; and &lt;i&gt;ACS Measurement Science&lt;/i&gt; Au sponsor the Early Career Investigator Award in Analytical Chemistry. Let me congratulate our 2024 winners, Jeffrey Dick (Early Career Award), and Boris Mizaikoff, Juyoung Yoon, and Peter Nemes (ACS Measurement Science Lectureship Awards). While 2025 nominations have closed, stay tuned for the 2025 Winners to be announced in the near future! As part of a collaborative effort, we published a special issue in 2024 to mark the 50th anniversary of the first published surface-enhanced Raman scattering experiments. ","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"5 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975463","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}

{"title":"Efficient and Rapid Enrichment of Extracellular Vesicles Using DNA Nanotechnology-Enabled Synthetic Nano-Glue","authors":"Lizhuan Zhang, Cai Yang, Juncai Li, Lu Wang, Ziwen Zhang, Minhui Su, Mengyuan Jiang, Qiuxia Yang, Ting Fu, Lei He, Weihong Tan","doi":"10.1021/acs.analchem.4c03842","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03842","url":null,"abstract":"Swift and efficient enrichment and isolation of extracellular vesicles (EVs) are crucial for enhancing precise disease diagnostics and therapeutic strategies, as well as elucidating the complex biological roles of EVs. Conventional methods of isolating EVs are often marred by lengthy and laborious processes. In this study, we introduce an innovative approach to enrich and isolate EVs by leveraging the capabilities of DNA nanotechnology. We have developed a novel multivalent cholesterol-modified paranemic crossover DNA (PX-DNA-chol) construct, which is a four-stranded DNA structure containing adjacent double helices intertwined with their local helix axes parallel and serves as an effective synthetic nano-glue. This construct promotes the rapid coalescence of nanoscale EVs into clusters of micrometer scale, thereby streamlining their enrichment. Utilizing a conventional low-speed centrifuge, this intriguing methodology achieves a rapid concentration of EVs within minutes, bypassing the laborious and high-speed centrifugation steps typically required. The quality of EVs isolated by our technique is comparable to that obtained through ultracentrifugation methods. Given these advancements, our PX-DNA-chol-facilitated EVs enrichment protocol is poised to advance the field of EVs research, providing a robust and accessible tool for in-depth studies of EVs.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"8 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975338","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}

{"title":"Simultaneous Profiling of Multiple Phosphorylated Metabolites in Typical Biological Matrices via Ion-Pair Reversed-Phase Ultrahigh-Performance Liquid Chromatography and Mass Spectrometry","authors":"Huan Wang, Qinsheng Chen, Yuanpeng Wu, Li Xu, Qi Wang, Qingyu Hu, Huiru Tang","doi":"10.1021/acs.analchem.4c04692","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04692","url":null,"abstract":"Simultaneous analysis of multiple phosphorylated metabolites (phosphorylated metabolome) in biological samples is vital to reveal their physiological and pathophysiological functions, which is extremely challenging due to their low abundance in some biological matrices, high hydrophilicity, and poor chromatographic behavior. Here, we developed a new method with ion-pair reversed-phase ultrahigh-performance liquid chromatography and mass spectrometry using BEH C18 columns modified with hybrid surface technology. This method demonstrated good performances for various phosphorylated metabolites, including phosphorylated sugars and amino acids, nucleotides, NAD-based cofactors, and acyl-CoAs in a single run using standard LC systems. Specifically, the method showed good retention (capacity factor &gt; 2) and reproducibility (Δ<i>t</i>_R &lt; 0.09 min, <i>n</i> = 6), peak symmetry (tailing factor &lt; 2), and sensitivity (limit-of-detection &lt; 238 fmol-on-column with QTOFMS) for all tested analytes especially for the medium- and/or long-chain acyl-CoAs. The method demonstrated reproducible applicability across numerous biological matrices, including tissue (liver), human biofluids (urine, plasma), cells, and feces, and revealed significant molecular phenotypic differences in phosphorylated metabolite composition.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"87 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968413","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}