ANALYTICAL CHEMISTRY
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2024
·
IF 6.7
Chang Liu,Yanan Wu,Mengying Li,Fang Liu,Pengfei Kong,Haifeng Yang,Xinling Liu
Salivary d-alanine (d-Ala) and d-proline (d-Pro) are of concern for their potential in the noninvasive diagnosis of gastric cancer (GC). Most reports have succeeded in determining the total concentration of d-Ala and d-Pro. However, for personalized diagnosis and better elucidation of the underlying specific correlation of d-Ala (or d-Pro) with GC, it is desirable to determine the specific concentration of d-Ala or d-Pro. Herein, we propose an enantiomer-specific tandem assay of d-Ala based on the colorimetric reaction between 2,4-dinitrophenylhydrazine and pyruvic acid generated from the deamination of d-Ala catalyzed by d-amino acid oxidase, which is easily distinguished from l-form amino acids, d-Pro, and many other species. A linear concentration range is established from 20 to 400 μmol/L with a limit of detection of 1.01 μmol/L. Real saliva sample tests reveal that the levels of d-Ala in GC cases are remarkably higher than those in healthy individuals, which offers a simple and low-cost strategy for GC diagnosis. Simultaneously, the total concentrations of d-Ala and d-Pro in saliva are determined. Hence, the concentration of d-Pro and the proportion of d-Ala could be calculated, which further provides more molecule- and individual-specific information. This research may offer a convenient method for noninvasive diagnosis of GC and pave a new route to explore the potentials of rare d-form amino acids in disease diagnosis and treatment.
研究领域:
生物化学
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医学诊断
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癌症研究
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PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Chenyang Liu,Shuxiang Jiao,Yuhua Liu,Tao Wu,Leilei Xie,Lijuan Zhang,Yun Zhang,Wenming Wang,Hongfei Wang
Three isomeric nitrosylruthenium complexes [RuCl(Qn)(Pro)(NO)] ( 1 – 3) were prepared, where Qn is 8-hydroxyquinoline and Pro is D-proline. The complexes 1 – 3 were characterized by 1 H-NMR, 13 C-NMR, ESI-MS, and their crystal structure were further determined with X-ray diffraction techniques. In complexes 1 and 3 , the O atom of D-proline coordinated trans to NO, while the O atom of 8-quinolinol coordinated trans to NO in complexes 2 , and the complexes 1 and 3 are the Ru-centered enantiomers. The photo induced NO release of the complexes were explored using time-resolved infrared spectroscopy (FT-IR) and electron paramagnetic resonance spectroscopy (EPR) in solution and the released NO was successfully imaged in living cells using a NO selective fluorescent probe. Furthermore, the cytotoxicity of the isomeric complexes against HeLa, HepG2 and A549 cells were evaluated. Among them, the selectivity for HeLa cells is significant (SI ≥ 5) with IC 50 values in the range of 1.15–1.94 μM. Moreover, the three complexes spontaneously bind to human serum albumin (HSA) through hydrogen bonding and van der Waals forces, the binding constants K b of 1 – 3 are 1.528 × 10 4 , 2.390 × 10 4 and 2.694 × 10 4 M −1 at 298 K, respectively. Molecular docking analyses reveals that 1 – 3 bind within subdomain IB of the protein, which suggest that HSA could be a delivery vehicel for these complexes. This study provides insight into the potential biological and pharmaceutical applications for these isomeric nitrosylruthenium complexes.
研究领域:
无机化学
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生物化学
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药学
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癌症研究
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Haiyan Fu,Ou Hu,Yao Fan,Ying Hu,Jiahao Huang,Zhao Wang,Yuanbin She
Interests in the recognition of chiral amino acids have grown tremendously in recent years, particularly in the fields of food analysis and pharmaceutical studies. Herein, an innovative “on-off-on” fluorescent assay has been developed for the sensitive and selective determination of chiral Proline (Pro), Lysine (Lys), and Serine (Ser). This detection platform is constructed by exploiting the fluorescence quenching ability of chiral self-assembly zinc 5, 10, 15, 20-tetra(4-pyridyl)-21 H -23 H -porphine (ZnTPyP) to CdTe quantum dots (CdTe QDs). CdTe QDs can act as signal switches whose fluorescence signals can effectively quenched by chiral nano ZnTPyP and then restored in the presence of enantiomer amino acids. The coupling use of CdTe QDs and chiral nano ZnTPyP also permits quantitative analysis of d -Pro, d -Lys, l -Ser with detection limits of 4.46 × 10 −10 mol L −1 , 7.13 × 10 −11 mol L −1 , and 3.35 × 10 −11 mol L −1 , respectively. The approach is also suitable for the effective detection of the three amino acids in complex biological matrices. This rapid, robust and reliable strategy for recognizing enantiomer amino acids has not been reported. The proposed method can be a powerful and valuable technology in the areas of drug discovery and food chemistry.
研究领域:
分析化学
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生物技术
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药学
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食品科学
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DOI
高影响因子
TALANTA
·
2026
·
IF 6.7
Zifeng Wang,Cong Dai
The dual-channel fluorescent sensing of hydroxyl radicals (·OH) is of great importance for environment and life. Organic cage for fluorescence sensing suffers from short excitation/emission wavelength and poor water solubility, while the application of carbon quantum dots is also hindered by the time-consuming preparation in high pressure and temperature conditions. Herein, we report a red emitted carbon dots derived from cationic organic cage for dual-channel fluorescent sensing of ·OH. The abundant flexible methylene within the cationic organic cage leads to remarkable collapse of intrinsic cavity. The ring-opening of imidazole structure occurs via redox reaction at acidic condition, resulting in the simple formation of carbon dots with the emission at 640 nm. Under acidic conditions, the ·OH generated via Fenton reaction exhibits strong affinity toward the prepared carbon dots. The mild oxidation at pH 1 significantly enhances the fluorescence, whereas the severe oxidative degradation at pH 6 leads to obvious fluorescence quenching. Based on the mutual verification of dual signals, a dual-channel fluorescent sensing method is established for ·OH in environmental samples and biological fluids. The sensing at pH 6 and 1 respectively achieves the linearity range of 1-50 and 5-50 μM, the limit of detection of 7.3 and 11.8 nM, and the relative standard deviation of 0.76% and 0.83% for 10 replicate analysis. The proposed method gives the recoveries of spiked ·OH ranged from 97.3% to 103.4% in real samples, demonstrating excellent accuracy and reliability. This study underscores the promising application potential of organic cage and carbon dots in fluorescent sensing. Furthermore, combined with Fenton reaction, the proposed dual-channel sensing platform can also be utilized to the detection of hazardous substances or biomarkers capable of H 2 O 2 generation.
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DIAMOND AND RELATED MATERIALS
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2026
·
IF 5.2
Lu Sun,Jie Wei,Qing Hu,Xiuquan Xu,Jing Wu,Yaoyao Cao,Yao Zhang,Haoyan Wu
A Fe/V-CN nanozyme with synergistically enhanced POD-like activity was rationally designed. • A sensitive cascade colorimetric platform for detecting gastric cancer-related D-amino acids was successfully constructed. • The assay supports reliable quantification of D-amino acids in complex human saliva matrices. The development of a practical and reliable cascade colorimetric method for detecting D-amino acids (DAAs) provides a promising tool for the prevention and preliminary diagnosis of gastric cancer. Herein, a bimetallic Fe V supported on graphitic carbon nitride (Fe/V-CN) nanozyme was rationally designed and synthesized via a simple annealing strategy. The atomic dispersion of Fe and V species, along with their coexisting multivalent states (Fe 2+ / 3+ , V 4+ / 5+ ) synergistically boosted the intrinsic peroxidase-like (POD) activity to Fe/V-CN, which were characterized by a high substrate affinity ( K m of 0.078 and 0.083 mM for TMB and H 2 O 2 ) and an accelerated catalytic turnover ( V max of 4.94 × 10 −7 and 7.76 × 10 −7 M·s −1 , respectively). Leveraging this improved activity, a cascade colorimetric sensing system was developed by integrating Fe/V-CN with D-amino acid oxidase (DAAO) for the specific detection of DAAs. The platform exhibited favorable analytical performance for D-proline (D-Pro) and D-alanine (D-Ala), offering wide linear ranges of 0–200 μM and 0–160 μM and low detection limits of 0.93 μM and 1.45 μM, respectively, combined with acceptable selectivity against common interferents. For real-sample analysis, the platform was successfully implemented in determine DAAs in human saliva, delivering satisfactory recoveries (95.8–105.7%) and good precision (RSD < 3.5%). This work presented a synergistic Fe/V bimetallic nanozyme and a practical sensing strategy, demonstrating the feasibility of DAAs detection in complex biological matrices. Download: Download high-res image (70KB) Download: Download full-size image
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JOURNAL OF CHROMATOGRAPHY A
·
2025
·
IF 4
Lei Ding,Chundan Ye,Junchen Zhu,Cuirong Sun
Chiral impurity analysis presents significant challenges due to limitations of detection methods. Levodopa (L-Dopa) is the primary medication for Parkinson's disease treatment for over 50 years. However, the detection of its chiral impurity is difficult due to the similarity of polarity. This study presents a novel analytical method for the quantitative detection of trace amount of D-Dopa, as well as other three impurities. The method demonstrated excellent chromatographic resolution for D-Dopa and L-Dopa (resolution = 4.15) and achieved a derivatization efficiency of 97% using a chlorine-labeled chiral probe (D-BPCl) for chemical derivatization, followed by analysis with liquid chromatography-tandem mass spectrometry (LC-MS/MS) on a conventional C18 column. Meanwhile, D-BPCl showed strong chiral selectivity on D-Dopa, and the ratio of mass spectrometric response for labeled D-Dopa to that of L-enantiomers was 2.78-fold under the same condition. The developed method demonstrates high sensitivity with detection limits of 7.88 μ g L -1 for D-Dopa, and 9.85 μ g L -1 for L-Dopa, with good linearity for every analyte (R 2 > 0.99), recoveries ranging from 94.1% to 106.8%, and high repeatability with relative standard deviation (RSD) values predominantly below 5%. Then the method was applied to analyze fifteen batches of levodopa tablets from five manufacturers. D-Dopa was successfully detected with the corresponding content ranging from 0.15% to 0.44%, which suggests that D-Dopa are more likely generated during the production process. The study underscores the significant safety concerns regarding Dopa-containing medications.
研究领域:
药物分析
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药物质量控制
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手性分离
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药物代谢
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分析化学
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PubMed
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CRYSTAL GROWTH & DESIGN
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2025
·
IF 3.4
Detao Li,Zichen Ning,Feiqiang He,Zhi Gao,Limin Zhou,Li Xu,Zhijian Zheng,Jerry Heng,Shichao Du,Jinbo Ouyang
To enable efficient separation of chiral drugs and enhance their practical utility, this study investigates cocrystallization as a novel separation and purification strategy. Using R/S-mandelic acid and d/l-prolinamide as model compounds, we screened potential cocrystal/salt coformers and successfully synthesized seven novel chiral salts. The proton transfer was elucidated by analyzing molecular electrostatic potential differences at the hydrogen-bonding sites. Moreover, the formation mechanism of salts was explored through structural analyses, such as Hirshfeld surface calculations, energy framework assessments, and crystal void analysis. Considering the distinct properties of various chiral salts, we conducted competitive cocrystallization experiments, establishing a complementary chiral pairing principle that provides a theoretical foundation for cocrystallization-based chiral resolution. Based on these findings, we developed multiple processes for the separation of R- and S-mandelic acid as well as l- and d-prolinamide, achieving product purities exceeding 80%, which strongly demonstrate the feasibility of cocrystallization separation technology for chiral resolution. This work not only introduces a groundbreaking approach to chiral separation but also highlights the vast potential of cocrystallization technology in pharmaceutical purification and beyond.
研究领域:
药物化学
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晶体工程
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手性分离技术
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超分子化学
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材料科学
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高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2024
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IF 4.3
Wenrong Cai,Yanjing Shi,Ning Liu,Zheng-Zhi Yin,Junyao Li,Laidi Xu,Datong Wu,Yong Kong
Chiral analysis with simple devices is of great importance for analytical chemistry. Based on the photothermal (PT) effect, a simple chiral sensor with a portable laser device as the light source and a thermometer as the detection tool was developed for the chiral recognition of tryptophan (Trp) isomers and the sensitive sensing of one isomer (L-Trp). Gold nanorods (GNRs), which have outstanding photo-thermal conversion ability due to their localized surface plasma resonance (LSPR) effect, are used as PT reagents, and biomacromolecules bovine serum albumin (BSA) are used as natural chiral sources, and thus, GNRs@BSA was obtained through Au–S bonds. The resultant GNRs@BSA displays higher affinity toward L-Trp than D-Trp owing to the inherent chirality of BSA. Under the irradiation of near-infrared (NIR) light, the temperature of GNRs@BSA//L-Trp is greatly lower than that of GNRs@BSA//D-Trp due to its greatly decreased thermal conductivity, and thus chiral discrimination of Trp isomers can be achieved. In addition, the developed PT effect-based chiral sensor can be used for sensitive detection of L-Trp, and the linear range and limit of detection (LOD) are 1 μM–10 mM and 0.43 μM, respectively.
研究领域:
分析化学
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纳米技术
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生物传感
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DOI
PubMed
高影响因子
TALANTA
·
2025
·
IF 6.1
Ying Xu,Cong Dai,Zhifeng Xu
The accurate and sensitive quantification of hydroxyl radical (·OH) and glucose is necessary for disease diagnosis and health guidance, but still challenging owing to the low concentration of ·OH and poor water solubility of fluorescent probes. In addition, fluorescent probes may cause secondary pollution to the environment. Here an organic cage was reported as a sensitive fluorescent probe for ·OH and glucose in aqueous solution without serious secondary pollution. The prepared organic cage with good water solubility showed specific redox affinity to ·OH in acidic condition, resulting in two oxidation stages of mild oxidation and subsequent oxidative degradation. Fluorescence around 485 nm enhanced remarkably in the first stage, and benzene ring in organic cage was degraded in the second stage. Based on the significant fluorescence enhancement, a sensitive fluorescence turn-on sensing method for ·OH was established within 90 s with the limit of detection (3 s/k , where s and k are the standard deviation for 10 replicate detections of blank and the slope of calibration function) of 5 nM. The recoveries of spiked ·OH in human serum and water samples ranged from 95.2 % to 102.7 %. After the glucose oxidase enzyme-Fenton reaction was involved, the ·OH detection was also applied to sensitive sensing of glucose with the limit of detection (3 s/k ) of 6 nM. The recoveries of spiked glucose in sugary drinks ranged from 96.2 % to 102.6 %. Furthermore, the proposed method would also be suitable for other hazardous substances and biomarkers which can produce hydrogen peroxide and further form ·OH via Fenton reaction.
研究领域:
分析化学
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生物医学工程
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环境科学
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PubMed
高影响因子
CHIRALITY
·
2024
·Vol. 36
·期 4
·e23665
·
IF 2.8
Luzheng Dong,Jun Wu,Xiashi Zhu
In this paper, the amino acid chiral ionic liquid (AACIL) was prepared with L-phenylalanine and imidazole. It was characterized by CD, FT-IR, 1 H NMR, and 13 C NMR spectrum. The chiral recognition sensor was constructed with AACIL and Cu(II), which exhibited different chiral visual responses (solubility or color difference) to the enantiomers of glutamine (Gln) and phenylalanine (Phe). The effects of solvent, pH, time, temperature, metal ions, and other amino acids on visual chiral recognition were optimized. The minimum concentrations of Gln and Phe for visual chiral recognition were 0.20 mg/ml and 0.28 mg/ml, respectively. The mechanism of chiral recognition was investigated by FT-IR, TEM, SEM, TG, XPS, and CD. The location of the host-guest inclusion or molecular placement has been conformationally searched based on Gaussian 09 software.
研究领域:
化学
·
分析化学
·
材料科学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Detao Li,Zichen Ning,Zhuoshan Gong,Limin Zhou,Li Xu,Feiqiang He,Hamza Shehzad,Heng Jerry,Shichao Du,Jinbo Ouyang
According to in-depth research on cocrystals of polyhydroxylated natural products, we previously summarized the substitution model to elucidate the formation mechanism of cocrystals. However, when refers to salt formation of natural products, the substitution model reveals numerous deficiencies. To compensate for the shortcomings of substitution model in predicting salt formation, this study conducts a comprehensive exploration of natural product salts. By supplementing the energy difference rule to the substitution model, it endows the modified model with broader applicability. Simultaneously, the transfer of protons within salts structures is verified by this modified model. Furthermore, we apply competitive cocrystallization technique to separate flavonoid natural products (quercetin, hesperetin, and naringenin). In view of the characteristics of various natural products as well as their cocrystals/salts, numerous separation processes are developed, and the separation effects of these processes are analyzed in detail. The purity of the products obtained from separation process all reaches above 70%, strongly demonstrating the feasibility of using cocrystallization for the binary separation of flavonoids. This work not only refines the substitution model for predicting cocrystals/salts formation of natural products but also indicates the promising application prospects of cocrystallization in industrial separation of natural products.
研究领域:
有机化学
·
药学
·
分离工程
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DOI
高影响因子
LANGMUIR
·
2025
·
IF 3.9
Huimin Wang,Guangxin Wang,Ruoxi Liu,Jin Yong Lee,Shufeng Liu,Yingqi Tang,Jing Yu
The development of highly efficient chiral recognition systems by simple and cost-effective means is critical to advance the precise application of chiral molecules. Herein, a novel electrochemiluminescence (ECL) enantioselective recognition platform was constructed based on l-histidine-functionalized zeolitic imidazolate frameworks (l-His-ZIF8). Detailed characterization verified the successful preparation of the chiral l-His-ZIF8 material. It was then applied to the chiral discrimination of six amino acids: cysteine (Cys), tryptophan (Trp), phenylalanine (Phe), glutamic acid (Glu), histidine (His), and proline (Pro). Among them, the system employing Ru(bpy)32+ as the luminophore demonstrated the most efficient chiral recognition of d-Cys over l-Cys, as evidenced by a distinct ECL signal ratio (ECLd-Cys/ECLl-Cys) of 3.3 at 1 mM. A detection limit of approximately 0.193 mM was achieved for Cys enantiomers. Conversely, an inverse chiral recognition was observed for the tryptophan (Trp)/sodium tetraphenylborate (TPB) system, resulting in a stronger ECL response for l-Trp over that for d-Trp (ECLl-Trp/ECLd-Trp = 2.4 at 1 mM). Theoretical calculations indicate that the excellent ECL enantioselectivity stems from the preferential binding of the “host” l-His-ZIF8 with specific “guest” enantiomers (d-Cys or l-Trp) via stronger intermolecular interactions. This preferential binding leads to the formation of more stable diastereoisomers that facilitate electrooxidation of more “guests” to generate a stronger luminescent signal than its isomer. This study establishes a novel strategy for electrochemiluminescent enantiomer discrimination using chiral site-engineered metal–organic frameworks (MOFs) and opens new avenues for the future of chiral sensing.
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