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Direct, Pretreatment-Free Surface-Enhanced Raman Scattering (SERS) Detection of Uric Acid in Urine Facilitated by Efficient Hydrogen Bonding-Driven Capture. 直接,无预处理的表面增强拉曼散射(SERS)检测尿液中的尿酸通过高效氢键驱动捕获。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-06 DOI: 10.1021/acs.analchem.5c06098
Supriya Atta, Tuan Vo-Dinh

Uric acid, a vital circulating metabolite, is a key biomarker for various health conditions including gout, preeclampsia, and kidney disorders. This underscores the need for noninvasive, rapid, sensitive, and cost-effective methods for monitoring uric acid to enable early preventive interventions. This study introduces a simple and sensitive separation-free "mix-and-detect" method for the direct surface-enhanced Raman scattering (SERS) detection of uric acid in urine, using bimetallic gold-silver nanostars functionalized with sodium dodecyl sulfate (BGNS@SDS). The SDS capping layer facilitates efficient uric acid capture through multiple hydrogen bonds under alkaline conditions, as confirmed by density functional theory (DFT) analysis. Using the optimized nanostar morphology (BGNS-3@SDS), uric acid was detected in water and spiked artificial urine samples with limits of detection of 2.2 and 3 μg/mL, respectively. These detection limits are substantially lower than the clinically relevant concentration range of uric acid in urine and well below the pathological threshold (∼750 μg/mL). The platform also successfully quantified uric acid levels in urine from ten healthy volunteers without sample pretreatment, enabling differentiation between healthy individuals and those at risk. This straightforward and sensitive SERS strategy holds strong promise for rapid, point-of-care diagnostics targeting low-affinity biomarkers.

尿酸是一种重要的循环代谢物,是各种健康状况的关键生物标志物,包括痛风、先兆子痫和肾脏疾病。这强调了对无创、快速、敏感和具有成本效益的尿酸监测方法的需求,以实现早期预防干预。本研究介绍了一种简单灵敏的无分离“混合检测”方法,用于直接表面增强拉曼散射(SERS)检测尿液中的尿酸,该方法使用十二烷基硫酸钠功能化的双金属金银纳米星(BGNS@SDS)。密度泛函理论(DFT)分析证实,SDS封盖层有助于在碱性条件下通过多个氢键有效捕获尿酸。利用优化后的纳米星形态(BGNS-3@SDS)对水中和加标人工尿液中的尿酸进行检测,检出限分别为2.2和3 μg/mL。这些检测限大大低于尿中尿酸的临床相关浓度范围,远低于病理阈值(~ 750 μg/mL)。该平台还成功地量化了10名健康志愿者尿液中的尿酸水平,而无需样品预处理,从而能够区分健康个体和有风险的个体。这种简单而敏感的SERS策略为针对低亲和力生物标志物的快速、即时诊断提供了强有力的希望。
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引用次数: 0
MS/MS Mass Spectrometry Filtering Tree for Bile Acid Regio- and Stereoisomer Annotation 胆汁酸区域和立体异构体注释的MS/MS质谱过滤树
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.analchem.5c05677
Ipsita Mohanty, Shipei Xing, Vanessa Castillo, Julius Agongo, Abubaker Patan, Yasin El Abiead, Helena Mannochio-Russo, Wilhan D. Gonçalves Nunes, Jasmine Zemlin, Itzhak Mizrahi, Dionicio Siegel, Mingxun Wang, Lee R. Hagey, Pieter C. Dorrestein
Bile acids are essential steroids with a wide range of biological roles, including the regulation of immunity, nutrient absorption, insulin signaling, appetite, and body temperature. However, due to similarities in their MS/MS spectra, spectral matching with reference MS/MS libraries generally fails to differentiate between isomers. This study introduces a proof-of-concept workflow that uses a mass spectrometry query language filtering tree to distinguish isomeric bile acids in untargeted LC-MS/MS data by leveraging intensity ratios of ions that are close to one another in the MS/MS spectrum. It can be retrospectively applied to existing LC-MS/MS data in data repositories. The filtering tree concept provides the opportunity to annotate and distinguish previously unknown bile acid isomers across LC-MS/MS data sets. To facilitate the ease of applying these filters to LC-MS/MS data sets, we developed a web-based application that simplifies the stepwise filtering tree workflow, removing the need for coding expertise. Here, we apply the multistep filtering application to a representative public data set, which revealed distinct patterns of bile acids associated with different diet types across diverse mammalian species. We further identified the previously uncharacterized bile acid deoxycholyl-N-acetyl-putrescine, which was elevated in carnivores.
胆汁酸是一种必需的类固醇,具有广泛的生物学作用,包括调节免疫、营养吸收、胰岛素信号、食欲和体温。然而,由于它们的MS/MS光谱相似,与参考MS/MS库的光谱匹配通常无法区分异构体。本研究介绍了一个概念验证工作流,该工作流使用质谱查询语言过滤树,通过利用MS/MS光谱中彼此接近的离子强度比,在非靶向LC-MS/MS数据中区分异构体胆汁酸。它可以回顾性地应用于数据存储库中现有的LC-MS/MS数据。过滤树概念提供了在LC-MS/MS数据集上注释和区分以前未知的胆汁酸异构体的机会。为了方便将这些过滤器应用于LC-MS/MS数据集,我们开发了一个基于web的应用程序,简化了逐步过滤树的工作流程,消除了对编码专业知识的需求。在这里,我们将多步过滤应用于一个有代表性的公共数据集,该数据集揭示了不同哺乳动物物种中与不同饮食类型相关的胆汁酸的不同模式。我们进一步鉴定了先前未被鉴定的胆汁酸脱氧胆酰- n -乙酰-腐胺,它在食肉动物中升高。
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引用次数: 0
Rational Design of a Dual-Locked Fluorescent Probe for Precise Imaging of Tumor via β-Galactosidase/Viscosity Activation. 基于β-半乳糖苷酶/粘度激活的肿瘤精确成像双锁相荧光探针的合理设计
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.analchem.5c07416
Xiaoyi Zhang, Jiaoru Chen, Bo Wei, Lu Wang, Lingfeng Xie, Xueling Ding, Shilong Zhu, Dezhong Guan, Jinpei Zhou, Mian Wang, Huibin Zhang

Fluorescence imaging is widely applied in oncology owing to its cost-effectiveness, noninvasiveness, and real-time imaging capability. Many activatable fluorescent probes targeting tumor biomarkers, such as β-galactosidase (β-gal) and viscosity, have been developed. However, the reliance on a single-response mechanism limits their ability to capture the dynamic alterations within tumors during cancer progression and chemotherapy. In this study, we rationally designed and developed ZW-gal, a dual-locked near-infrared (NIR) probe activated by both β-gal activity and viscosity. ZW-gal exhibited favorable photophysical properties, such as a large Stokes shift (125 nm), rapid enzymatic activation (within 2 min), and a strong viscosity-dependent fluorescence enhancement (up to 24.6-fold). Leveraging this dual-responsiveness, ZW-gal successfully distinguished cancer from normal cells, visualized doxorubicin-induced cancer cell senescence, and monitored cell death. In a mouse model of liver cancer, ZW-gal enabled precise tumor localization and identified senescent tumors. Moreover, through in situ spraying, ZW-gal provided real-time surgical navigation, facilitating complete tumor resection. Building on these advantages, ZW-gal represents a powerful tool with broad potential to advance both basic cancer research and personalized clinical applications.

荧光成像具有成本效益高、无创、实时成像等优点,在肿瘤学领域得到了广泛的应用。许多靶向肿瘤生物标志物的可激活荧光探针,如β-半乳糖苷酶(β-gal)和粘度,已经被开发出来。然而,对单一反应机制的依赖限制了它们在癌症进展和化疗期间捕捉肿瘤内动态变化的能力。在本研究中,我们合理设计并开发了一种双锁相近红外(NIR)探针ZW-gal,该探针由β-gal活性和粘度共同激活。ZW-gal表现出良好的光物理特性,如大的Stokes位移(125 nm),快速的酶激活(2分钟内),以及强的粘度依赖性荧光增强(高达24.6倍)。利用这种双重反应性,ZW-gal成功地区分了癌细胞和正常细胞,可视化了阿霉素诱导的癌细胞衰老,并监测了细胞死亡。在小鼠肝癌模型中,ZW-gal能够精确定位肿瘤并识别衰老肿瘤。此外,ZW-gal通过原位喷涂提供实时手术导航,促进肿瘤的完全切除。基于这些优势,ZW-gal代表了一个强大的工具,在推进基础癌症研究和个性化临床应用方面具有广泛的潜力。
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引用次数: 0
pH-Switchable Multienzymatic Activities of an Fe Single-Atom Nanozyme Enable Dual-Cascade Catalysis for Robust Dual-Mode Biosensing. 铁单原子纳米酶的ph可切换多酶活性使双级联催化成为强大的双模式生物传感。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.analchem.5c06857
Huifang Zhang, Yuhang Zhang, Xiang Xu, Shaobin Tang, Yan Hu, Huanhuan Wu, Xiaoming Ma, Yuexiang Li, Zhenyu Lin

Nanozymes with multienzymatic activities provide synergistic effects for diverse biosensing applications. However, precise manipulation of their functionalities without cross-reactivity for advanced multimode sensing remains challenging. Herein, we employed a cytochrome c (Cyt c)-templated pyrolysis strategy to construct Fe single-atom nanozymes (FeSAN) featuring Fe-N5 moieties with pH-switchable multienzymatic activities. Notably, the oxidase and peroxidase-like activities of FeSAN exhibit acid-dependent catalytic behavior, enabling a self-supplying oxidative catalytic cascade in acidic conditions. Conversely, in alkaline media, FeSAN demonstrates superoxide dismutase and catalase-like activity, forming a complementary antioxidant pathway for superoxide anion scavenging. The enzyme-mimicking mechanism and potential cascade pathways were investigated through comprehensive experiments and theoretical calculations. Capitalizing on the divergent pH requirements of colorimetric (acidic) and electrochemiluminescence (alkaline) systems, this pH-switchable dual-cascade catalytic platform enables amplified colorimetric response via TMB oxidation in acidic media while suppressing electrochemiluminescence intensity in alkaline circumstances. Using an organophosphorus pesticide (e.g., trichlorfon) as a proof-of-concept target, this platform with inverse signal correction achieved at least 10-fold higher sensitivity and improved accuracy compared to conventional methods. This work establishes a novel paradigm for advanced biosensing by fully utilizing the multienzymatic functionalities of single-atom nanozymes to construct dual-cascade catalysis in dual-mode platforms.

具有多种酶活性的纳米酶为多种生物传感应用提供了协同效应。然而,精确的操作他们的功能,没有交叉反应的先进多模传感仍然具有挑战性。在此,我们采用细胞色素c (Cyt c)模板热解策略构建了铁单原子纳米酶(FeSAN),其特征是铁- n5基团具有ph可切换的多酶活性。值得注意的是,FeSAN的氧化酶和过氧化物酶样活性表现出酸依赖的催化行为,在酸性条件下实现自供应的氧化催化级联。相反,在碱性培养基中,FeSAN表现出超氧化物歧化酶和过氧化氢酶样活性,形成了清除超氧化物阴离子的互补抗氧化途径。通过综合实验和理论计算,研究了酶模拟机制和潜在的级联途径。利用比色(酸性)和电化学发光(碱性)系统的不同pH要求,这种pH可切换的双级联催化平台可以通过酸性介质中的TMB氧化放大比色响应,同时抑制碱性环境下的电化学发光强度。使用有机磷农药(如敌百虫)作为概念验证目标,与传统方法相比,该平台具有反向信号校正,其灵敏度和准确性至少提高了10倍。本工作通过充分利用单原子纳米酶的多酶功能,在双模式平台上构建双级联催化,为先进的生物传感建立了一个新的范例。
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引用次数: 0
Long-Lived Phosphorescent CDs@SiO2 Coupled with Magnetic Quencher Fe3O4@PDA: A Dual-Mode Lateral Flow Immunochromatographic Assay for Sensitive Determination of Acetamiprid. 长寿命磷光CDs@SiO2与磁猝灭器耦合Fe3O4@PDA:双模式横向流动免疫层色谱法对啶虫脒的敏感测定。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.analchem.5c07389
Qianqian Jiang, Renlong Chen, Tong Zhang, Hao Shen, Cheng Zhang, Kui Zhang, Zhongping Zhang

Lateral flow immunochromatographic assay (LFIA) features advantages such as a rapid analysis process, interpretable detection results, and low cost, making it an effective method for on-site detection of pesticides. However, the existing LFIA technologies still face bottleneck issues, including strong background fluorescence interference from the substrate and insufficient detection sensitivity for low pesticide residue levels. Here, long-lived room-temperature phosphorescent carbon dots embedded in silica (CDs@SiO2) were developed to overcome background fluorescence interference. Fe3O4 coated with dopamine (Fe3O4@PDA) was utilized for the enrichment of target pesticide molecules. Meanwhile, by virtue of the quenching effect of Fe3O4@PDA on CDs@SiO2, colorimetric and phosphorescent dual-mode LFIA technology was designed for the detection of the pesticide acetamiprid. Through the integration of the advantages of CDs@SiO2 and Fe3O4@PDA, the limit of detection (LOD) for acetamiprid was as low as 0.271 ng/mL, and satisfactory recoveries were achieved in real samples. This research breaks through the millisecond-level lifetime limitation in traditional time-resolved fluorescence immunoassays, providing novel insight for the development of labeling materials for LFIA.

横向流动免疫层析分析(LFIA)具有分析过程快速、检测结果可解释、成本低等优点,是一种有效的农药现场检测方法。然而,现有的LFIA技术仍然面临瓶颈问题,包括底物的本底荧光干扰强,对低农药残留水平的检测灵敏度不足。在这里,长寿命的室温磷光碳点嵌入二氧化硅(CDs@SiO2)被开发克服背景荧光干扰。利用包被多巴胺(Fe3O4@PDA)的Fe3O4富集目标农药分子。同时,利用Fe3O4@PDA对CDs@SiO2的猝灭作用,设计了比色法和磷光双模LFIA技术用于农药啶虫脒的检测。结合CDs@SiO2和Fe3O4@PDA两种方法的优点,对乙酰脒的检出限(LOD)低至0.271 ng/mL,在实际样品中可获得满意的回收率。该研究突破了传统时间分辨荧光免疫测定的毫秒级寿命限制,为LFIA标记材料的开发提供了新的见解。
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引用次数: 0
Exploring Photoacoustic Vibration of Quartz for Constructing a Versatile Photoacoustic Sensor. 探索石英的光声振动,构建多功能光声传感器。
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.analchem.5c05747
Jie Wang, Kaitong Yang, Lasse Hyldgaard Klausen, Judith Zubia Aranburu, Chenglong Song, Zhihao Ma, Hongxing Zhang, Lei Liu, Mingdong Dong

The conventional photoacoustic effect is based on the photothermal mechanism in semiconductors, where light absorption is converted to heat within photoacoustic materials. In this study, we introduce a novel, heat-independent phototriggered vibration on a quartz plate under a broad spectrum of light irradiation. Through a series of experiments, we elucidate the underlying mechanism and demonstrate its potential as an innovative photodetector and photoacoustic sensor. This approach enables applications in small-molecule self-assembly, DNA hybridization, and protein interactions, offering superior sensitivity and accuracy. These findings highlight the promise of this unconventional photoacoustic effect for the development of highly sensitive biosensors.

传统的光声效应是基于半导体中的光热机制,其中光吸收在光声材料中转化为热。在这项研究中,我们引入了一种新的、热无关的光触发振动在石英板上的广谱光照射。通过一系列的实验,我们阐明了其潜在的机制,并证明了它作为一种创新的光探测器和光声传感器的潜力。这种方法可以应用于小分子自组装,DNA杂交和蛋白质相互作用,提供卓越的灵敏度和准确性。这些发现突出了这种非常规光声效应在高灵敏度生物传感器开发中的前景。
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引用次数: 0
A General Approach Based on "Recognizing-Releasing" Strategy to Design Norepinephrine-Responsive Photoacoustic Probes for Depression Detection. 基于“识别-释放”策略的去甲肾上腺素响应光声探针抑郁检测的一般方法
IF 6.7 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-05 DOI: 10.1021/acs.analchem.5c06992
Guiting Zheng, Kaikai Duan, Qin Yang, Huayu Wang, Xiang Li, Chong-Hua Zhang, Zhenkun Wu, Xianjun Liu

The precise detection of norepinephrine (NE) is critically important for understanding depression pathology and improving clinical diagnosis. Current strategies for designing NE-responsive photoacoustic (PA) probes, such as the "protect-deprotect" and the "hunting-shooting", are limited by slow kinetics, susceptibility to interference, or poor generalizability. Here, we report a novel "Recognizing-Releasing" strategy for designing NE-responsive photoacoustic (PA) probes and present QSH-NE as a proof-of-concept probe to demonstrate the generalizability of this strategy for in vivo imaging of depression. This rationally designed probe incorporates a quinolinium-derived sulfur-substituted hemicyanine (QSH-OH) as the PA reporter and a 2-hydroxy-5-(hydroxymethyl) benzaldehyde-derived unit as the recognition moiety. The PA activation mechanism initiates with aldehyde-amino recognition to form a five-membered ring, followed by a releasing step through carbamate cleavage and 1,6-elimination. QSH-NE exhibited favorable sensitivity, high activation fold, and a good response rate for NE in vitro. Notably, QSH-NE enabled noninvasive monitoring of depression progression and drug intervention efficacy through quantitative PA signal analysis in live animal brains. This general design strategy not only advances NE detection specificity but also provides a versatile platform for depression research and clinical diagnosis.

准确检测去甲肾上腺素(NE)对理解抑郁症病理和提高临床诊断水平至关重要。目前设计ne响应光声(PA)探针的策略,如“保护-去保护”和“狩猎-射击”,受到动力学缓慢、易受干扰或通用性差的限制。在这里,我们报告了一种新的“识别-释放”策略,用于设计ne响应光声(PA)探针,并将QSH-NE作为概念验证探针,以证明该策略在抑郁症的体内成像中的普遍性。这种合理设计的探针包含一个喹啉衍生的硫取代半苯胺(QSH-OH)作为PA报告基因,一个2-羟基-5-(羟甲基)苯甲醛衍生的单元作为识别片段。PA的激活机制始于醛-氨基识别,形成一个五元环,然后通过氨基甲酸酯裂解和1,6消除释放。QSH-NE对NE具有良好的敏感性、高的激活倍数和良好的体外反应率。值得注意的是,QSH-NE通过活体动物脑内定量PA信号分析,实现了无创监测抑郁进展和药物干预效果。这种通用的设计策略不仅提高了NE检测的特异性,而且为抑郁症的研究和临床诊断提供了一个通用的平台。
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引用次数: 0
Cyclic Peptide–Polymer Conjugate Characterization Using 193 nm Ultraviolet Photodissociation Tandem Mass Spectrometry 193nm紫外光解串联质谱法表征环肽-聚合物共轭物
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-04 DOI: 10.1021/acs.analchem.5c03375
Tomos E. Morgan, Alina Theisen, Sean Ellacott, Anisha Haris, Christopher A. Wootton, Julia Y. Rho, Mark P. Barrow, Anthony W. T. Bristow, Sébastien Perrier, Peter B. O’Connor
Cyclic peptide–polymer conjugates offer a unique biocompatible system with many advantages but come at the cost of being analytically challenging. Developing further analytical techniques of complex polymer-conjugate systems is key to understanding synthetic and medicinal properties. In this contribution, a synthetic cyclic peptide–polymer conjugate is analyzed using electron capture dissociation (ECD), infrared multiphoton absorption dissociation (IRMPD), and 193 nm ultraviolet photodissociation (UVPD) on the same mass spectrometry system. IRMPD and UVPD were shown to effectively characterize unconjugated cyclic peptide species. ECD was less informative during cyclic peptide analysis due to the production of multiple sequence scrambling fragments and radical side chain losses. ECD was shown to produce extensive fragmentation and enable the characterization of conjugated side chains of cyclic species. ECD and IRMPD thus provided complementary data, enabling the target analysis of conjugated systems. UVPD effectively characterized both the cyclic peptide and the conjugating polymer in one experiment, being able to produce complete cyclic peptide fragmentation via b/y fragment pathways and polymer fragmentation via a/x poly(2-ethyl-2-oxazoline) fragment pathways.
环肽-聚合物缀合物提供了一种独特的生物相容性体系,具有许多优点,但代价是分析上的挑战。进一步发展复杂聚合物偶联体系的分析技术是了解其合成性质和药用性质的关键。本文采用电子捕获解离(ECD)、红外多光子吸收解离(IRMPD)和193nm紫外光解离(UVPD)在同一质谱系统上对合成的环肽-聚合物共轭物进行了分析。IRMPD和UVPD可以有效地表征非共轭环肽。由于产生多个序列混乱片段和自由基侧链损失,ECD在环肽分析中信息较少。ECD被证明可以产生广泛的碎片化,并能够表征环物种的共轭侧链。因此,ECD和IRMPD提供了互补的数据,使共轭系统的目标分析成为可能。UVPD在一次实验中有效地表征了环肽和共轭聚合物,能够通过b/y片段途径产生完整的环肽片段,通过a/x聚(2-乙基-2-恶唑啉)片段途径产生完整的聚合物片段。
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引用次数: 0
Investigating the Effect of Isoelectric Points on the Gas-Phase Stability of Native-like Proteins Analyzed in Positive- versus Negative-Ion Mode by IMS-MS 用IMS-MS研究等电点对正负离子模式下天然样蛋白气相稳定性的影响
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-04 DOI: 10.1021/acs.analchem.5c04295
Alexis N. Edwards,Madeline G. Bannon,Michael S. Cordes,Elyssia S. Gallagher
Native ion mobility spectrometry-mass spectrometry (IMS-MS) is routinely used for analysis of folded proteins and protein complexes. For many proteins, the three-dimensional structure is maintained during electrospray ionization (ESI) as the protein transitions to the gas phase, allowing for detailed investigation of the gaseous, ionic protein’s structure and stability. Much of the native IMS-MS research has been conducted in positive-ion mode (+ESI), even when the protein of interest has a net-negative charge in solution at physiological pH. We hypothesize that analyzing a protein in the polarity that is opposite to its solution-phase charge, such as analyzing net-negative proteins by +ESI-MS, disrupts the network of noncovalent-bonding interactions within the protein to a greater extent than using the polarity that matches the protein’s solution-phase charge, resulting in differences in protein stability. Herein, we show that while most protein ions have similar initial, folded structures in +ESI and negative-ion mode (−ESI), positive and negative ions exhibit significant differences in gas-phase stability. Furthermore, the energy required to cause this unfolding is often greater in the polarity corresponding to the solution-phase charge of the protein, indicating that the protein is more stable in that polarity. Thus, this work highlights the necessity of considering polarity when conducting native IMS-MS experiments.
天然离子迁移谱-质谱法(IMS-MS)通常用于折叠蛋白质和蛋白质复合物的分析。对于许多蛋白质来说,在电喷雾电离(ESI)过程中,当蛋白质过渡到气相时,三维结构保持不变,从而可以详细研究气态、离子蛋白质的结构和稳定性。许多原生IMS-MS研究都是在正离子模式(+ESI)下进行的,即使感兴趣的蛋白质在生理ph下的溶液中具有净负电荷。我们假设,分析与溶液相电荷相反极性的蛋白质,例如用+ESI- ms分析净负电荷蛋白质,与使用与蛋白质溶液相电荷相匹配的极性相比,在更大程度上破坏蛋白质内部的非共价键相互作用网络,导致蛋白质稳定性的差异。本文表明,虽然大多数蛋白质离子在+ESI和负离子模式(- ESI)下具有相似的初始折叠结构,但正离子和负离子在气相稳定性方面存在显著差异。此外,导致这种展开所需的能量通常在与蛋白质溶液相电荷相对应的极性中更大,这表明蛋白质在该极性中更稳定。因此,这项工作强调了在进行本地IMS-MS实验时考虑极性的必要性。
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引用次数: 0
Porphyrinic Metal–Organic Frameworks with Longitudinal Pt Deposition Referenced as Opto/Catalytic Adjuvants for Dual-Path Glycoprotein Assay 具有纵向铂沉积的卟啉金属-有机框架作为光/催化佐剂用于双路糖蛋白测定
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2026-02-04 DOI: 10.1021/acs.analchem.5c06805
Yi Yang,Licheng Yu,Haiyang Wang,Liang He,Pengli Bai,Xiwen He,Langxing Chen,Yukui Zhang
In this work, porphyrinic metal–organic frameworks (MOFs) with longitudinal Pt deposition were developed for the inspired establishment of opto/catalytic adjuvants referenced for a dual-path glycoprotein assay. In the compositional cooperation, porphyrinic MOFs were synthesized through Zr oxoclusters and polytopic porphyrin ligands into a benchmark template (PCN-222), followed by catalytic Pt nanowire deposition (PtNW@PCN-222). As for signal reflection, the fluorogenic species (i.e., resazurin and amplex red) were integrated into zeolitic imidazolate framework-8 (ZIF-8) via epitaxial shell growth to guide lectin integration. The specific performance toward glycoprotein recognition was guaranteed by both antibody–antigen interaction as well as glycan epitope binding through lectin affinity, and the signal response was initiated by textural decomposition of the ZIF-8 skeleton in a controllable manner. On one hand, PtNW@PCN-222 can function as the catalytic adjuvant to exert the fluorogenic reactions: a reductive N-deoxygenation of resazurin and an oxidative N-deacetylation of amplex red, in which both the redox reactions generated the fluorescent species of resorufin products. On the other hand, PtNW@PCN-222 with endogenous periodical arrangement of porphyrin ligands can be tailored as an optical adjuvant for reporting signal reference. For benefits, the comprehensive functions leaned on the catalytic performance and optical reference property from PtNW@PCN-222 can be harvested for a ratiometric glycoprotein assay. Besides, due to the variant catalytic converter of PtNW@PCN-222 involved in the two fluorogenic reactions, the proposed glycoprotein assay exhibited a range of 0.03–3 nM with a detection limit of 7.91 pM in the reductive pathway, and showed a linear range from 0.06 to 10 nM with a detection limit of 21.64 pM in the oxidative pathway. Collectively, our proposed glycoprotein assay may provide a new thought in opto/catalytic MOF adjuvant-empowered ratiometric sensing in the dual-path reflection manner, which may also reinforce the accurate detection capability for the glycoprotein assay.
在这项工作中,开发了具有纵向Pt沉积的卟啉金属有机框架(MOFs),用于建立双路糖蛋白分析参考的光/催化佐剂。在组成合作中,通过Zr氧簇和多聚卟啉配体合成卟啉类mof,形成基准模板(PCN-222),然后催化沉积Pt纳米线(PtNW@PCN-222)。在信号反射方面,通过外延壳生长将荧光物质(即resazurin和amplex red)整合到沸石咪唑酸框架-8 (ZIF-8)中,引导凝集素整合。通过抗体-抗原相互作用和凝集素亲和力与糖聚糖表位结合,保证了ZIF-8对糖蛋白识别的特异性性能,信号响应是由ZIF-8骨架的结构分解以可控的方式启动的。一方面,PtNW@PCN-222可以作为催化佐剂,发挥reazurin的还原性n -脱氧反应和amplex红的氧化性n -去乙酰化反应的荧光反应,这两种氧化还原反应都产生了间苯二酚的荧光产物。另一方面,具有内源性周期性排列的卟啉配体PtNW@PCN-222可以被定制为报告信号参考的光学佐剂。为了方便起见,从PtNW@PCN-222获得的催化性能和光学参考性质的综合功能可以用于比率糖蛋白测定。此外,由于PtNW@PCN-222的变型催化转化器参与了两种荧光反应,所建立的糖蛋白检测在还原途径上的检测范围为0.03-3 nM,检出限为7.91 pM;在氧化途径上的检测范围为0.06 - 10 nM,检出限为21.64 pM。总的来说,我们提出的糖蛋白检测方法可能为光/催化MOF佐剂增强双路反射方式的比例传感提供了新的思路,这也可能增强糖蛋白检测的准确检测能力。
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Analytical Chemistry
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