JOURNAL OF CHROMATOGRAPHY A
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2024
·
IF 3.8
Zilong Zhang,Jiahuan Chen,Lixiang Chen,Kaihua Long,Lejing Qu,Silin Huang,Xinyi Yuan,Xu Ji,Qian Li,Xinfeng Zhao
Functional protein immobilization forms the basis for bio-detections. A series of one-point, site-specific immobilization methods have been developed, however, it still remains as a challenge how to avoid the proteins to move in all directions as well as conveniently regenerate the bio-devices. Herein, we have developed a bivalent affinity binding-inspired method for PPARγ immobilization using DNA aptamer and nickel-nitrilotriacetic acid (Ni 2+ -NTA) chelation. The specific DNA aptamer ( Apt 2 ) was selected by an on-column systematic evolution of ligands by exponential enrichment (SELEX) method with affinity of (1.57 ± 0.15) × 10 5 M −1 , determined by isothermal titration calorimetry (ITC). Apt 2 and nickel-nitrilotriacetic acid (Ni 2+ -NTA) were modified on macroporous silica gels via L-α-allylglycine as a linker. They respectively interacted with PPARγ and 6×His tag via bivalent affinity binding for the receptor immobilization. After comprehensive surface characterization, PPARγ was proved to be successful immobilized. Chromatographic studies revealed that the immobilized PPARγ has conformation selectivity, which discriminated agonist and antagonist of the receptor. Ligand-binding parameters (affinity and rate constant) of four agonists (rosiglitazone, pioglitazone, troglitazone, and magnolol) with PPARγ were determined. Troglitazone showed the lowest dissociation rate constant. The binding affinities (3.28 × 10 7 , 1.91 × 10 6 , 2.25 × 10 7 , and 2.43 × 10 7 M −1 ) were highly consistent with the data obtained using purified receptor in solution (2.16 × 10 7 , 4.52 × 10 6 , 1.20 × 10 7 , and 1.56 × 10 7 M −1 ), offering reliable bio-detection method for PPARγ and its ligands. Due to the biocompatibility of nuclear receptor with DNA, it is conceivable that the bivalent affinity-based method will be a general method for the immobilization of other nuclear receptors, which may provide selective conformation and improved ligand-binding activity for the receptors.
研究领域:
生物化学
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分子生物学
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生物技术
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分析化学
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DOI
PubMed
高影响因子
ANALYST
·
2019
·Vol. 144
·期 12
·3826-3835
·
IF 4.019
Xinglin Wang,Xiaoyi Gao,Jiale He,Xiaochen Hu,Yunchao Li,Xiaohong Li,Louzhen Fan,Hua-Zhong Yu
Graphene oxide (GO)-based aptasensors are currently one of the most popular sensing platforms for the simple and rapid detection of various targets. Unfortunately, the GO-based aptasensors with long aptamer strands typically show unsatisfactory performance resulting from insignificant structural transformations upon target binding. We report herein the utilization of an aptamer-truncating strategy to combat such a challenge. Taking a pre-selected anti-aflatoxin B1 (AFB1) aptamer (P-AFB1-50) as a trial system, we sequentially remove the extraneous nucleotides within the aptamer by means of circular dichroism (CD) spectroscopy and binding affinity analysis. Particularly, the ratio of the quenching constants between the GO sheets and the truncated aptamers (labelled with fluorophores) in the absence and presence of the target was determined for each of the truncated aptamers to evaluate the optimal sequence. As a result, the truncated aptamer comprising 40 nucleotides was confirmed to show the highest FL output and the best detection limit upon conjugation with GO sheets. More importantly, we demonstrated that this truncating strategy is versatile, i.e., it can be easily extended to other aptamer systems (anti-ochratoxin A (OTA) aptamer, P-OTA-61, as an example) for extraneous nucleotide identification. Impressively, the two optimal truncated aptamers can work together on GO sheets to achieve a simultaneous detection of two different mycotoxins (i.e., AFB1 and OTA) in one single test. Essentially, this research opens a new avenue for the design and testing of aptamer-/GO-based-sensing platforms for rapid, low-cost and multiplex quantification of analytical targets of interest.
研究领域:
分析化学
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生物传感器
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毒理学
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产品关联
DOI
PubMed
高影响因子
Nano Research
·
2020
·Vol. 14
·期 5
·1523-1532
·
IF 8.183
Zhang Liang,Wang Jing,Wang Huiting,Zhang Wentao,Zhu Wenxin,Du Ting,Ni Yongsheng,Xie Xianghong,Sun Jing,Wang Jianlong
The increasing accumulation of toxic mercury species in water environment has posed a serious health threat worldwide, making it inevitable to develop the versatile materials to achieve efficient prevention and remediation of mercury pollution. Guided by the solvent-assisted ligand exchange (SALE) approach, this work rationally constructed a mixed-ligand NH 2 -UiO-66-SH (NSU66) with hierarchical-pore structure by incorporating the thiol-rich ligands (H 2 DMBD) into the water-stable NH 2 -UiO-66 (NU66) precursor to act as a smart adsorbent equipped with sensitive detector for simultaneous sensing and removal of Hg 2+ . Unlike the traditional adsorbents, the as-prepared NSU66 not only exhibits a remarkable removal ability with fast capture rate (within 60.0 min), large uptake capacity (265.29 mg/g), and qualified selectivity, but also possesses satisfactory sensing capability, accompanied by low detection limit (3.50 × 10 −2 µM), wide linear range (1.00–99.7 µM), high specificity, and strong anti-interference capability. The detection function plays a vital role in indicating the removal behavior and the pre-enrichment effect of adsorption process correspondingly improves the sensitivity of indicator. Notably, the sensing and trapping capabilities of NSU66 are significantly improved compared to the NU66, which stems from the delicate design of the mixed-ligand and hierarchical-pore structure. Furthermore, proven excellent stability and recyclability emphasize the feasibility of NSU66 in practical applications. These results suggest that the smart NSU66 adsorbent can serve as a favorable platform for early warning and guided removal of toxic Hg 2+ in water.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
ChemNanoMat
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2018
·Vol. 5
·期 3
·318-322
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IF 3.173
Li Zhang,Qiong Zhang,Xiangyu Xing,Yuanzhi Jiang,Tingwei He,Yanmin Huang,Zhiwei Ma,Jien Yang,Mingjian Yuan
Graphical Efficient green light-emitting diodes were fabricated by using CsPbBr 3 nanocrystals with excellent carrier transportation properties, owing to the introduction of conjugated alkyl-amine through two-step surface ligand engineering. LEDs exhibit a high luminance of 26,475 cd m −2 , a high CE of 23.53 cd A −1 by incorporation conjugation molecular ligand into the all-inorganic perovskite nanocrystals. Long alkyl-chain capped ligands are prerequisites for preserving high photoluminescence quantum yield (PLQY) in perovskite nanocrystals (NCs). Unfortunately, the insulating feature of surface ligands potentially hinders carrier transport in light-emitting diode (LED) devices, which will degenerate the LED performance. To overcome this shortcoming, we introduce a conjugated molecule, 3-phenyl-2-propen-1-amine (PPA), into CsPbBr 3 NCs through a two-step surface ligand engineering process. Owing to excellent electrical conductivity of PPA, PPA-capped CsPbBr 3 NCs LEDs exhibit a maximum current efficiency of 23.53 cd A −1 , and a maximum luminance of 26,475 cd m −2 at the wavelength of 517 nm. This work offers a new strategy to improve the quality of CsPbBr 3 NCs and LEDs by introducing conjugation molecular ligands into the all-inorganic perovskite nanocrystals.
研究领域:
材料科学
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光电技术
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纳米科技
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产品关联
DOI
高影响因子
Chemical Science
·
2024
·Vol. 15
·期 33
·13359-13368
·
IF 7.6
Sicong Ma,Yanwei Cao,Yun-Fei Shi,Cheng Shang,Lin He,Zhi-Pan Liu
The design of highly active catalysts is a main theme in organic chemistry, but it still relies heavily on expert experience. Herein, powered by machine-learning global structure exploration, we forge a Metal–Phosphine Catalyst Database (MPCD) with a meticulously designed ligand replacement energy metric, a key descriptor to describe the metal–ligand interactions. It pushes the rational design of organometallic catalysts to a quantitative era, where a ±10 kJ mol−1 window of relative ligand binding strength, a so-called active ligand space (ALS), is identified for highly effective catalyst screening. We highlight the chemistry interpretability and effectiveness of ALS for various C–N, C–C and C–S cross-coupling reactions via a Sabatier-principle-based volcano plot and demonstrate its predictive power in discovering low-cost ligands in catalyzing Suzuki cross-coupling involving aryl chloride. The advent of the MPCD provides a data-driven new route for speeding up organometallic catalysis and other applications.
研究领域:
有机化学
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催化科学
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数据科学
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DOI
高影响因子
INORGANICA CHIMICA ACTA
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2024
·
IF 2.7
Jie Cao,Gang Xiong,Zhixiong Luo,Qiuyan Huang,Wenyan Zhou,Ileana Dragutan,Valerian Dragutan,Yaguang Sun,Fu Ding
An amide functionlized bidentate NHC-Pd complex was successfully prepared by a facile solvothermal methodology from a bridged bis-benzimidazolium chloride and K 2 PdCl 4. The new bidentate NHC-Pd complex has been effectively applied as catalyst in Suzuki-Miyaura cross-coupling reactions of aryl halides with arylboronic acids in distilled water (yields up to 99.0%). The bridged bis-benzimidazolium ligand from the Pd complex, bearing the amide functional groups on the nitrogen atom, showed to distinctly influence the electronic and steric effects on the catalytic process. The potential of application of the new NHC-Pd catalyst in diverse C C bond forming processes, working under environmentally friendly conditions, is further outlined.
研究领域:
有机化学
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催化化学
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绿色化学
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DOI
高影响因子
Toxins
·
2019
·Vol. 11
·期 8
·447
·
IF 3.895
Li Liu,Zafar Iqbal Tanveer,Keqiu Jiang,Qingwen Huang,Jinghui Zhang,Yongjiang Wu,Zheng Han
With the widespread contamination of ochratoxin A (OTA), it is of significant importance for detecting OTA in foods and traditional Chinese medicine (TCM). In this study, a novel label-free fluorescent aptasensor utilizing the interaction between OTA-triggered antiparallel G-quadruplex and (N-methyl-4-pyridy) porphyrin (TMPyP) for the rapid and sensitive determination of OTA was established. The fluorescence of CdTe quantum dots (QDs) could be quenched by TMPyP. In the presence of analyte (OTA), the aptamer could recognize OTA and transform from a random coil to the antiparallel G-quadruplex. The interaction between G-quadruplex and TMPyP could release CdTe QDs from TMPyP, and thus recover the fluorescence of CdTe QDs. Under optimized conditions, the detection limit of the designed aptasensor was 0.16 ng mL−1, with a linear range of 0.2 to 20 ng mL−1. Furthermore, this aptasensor showed high selectivity toward OTA against other structural analogs and other mycotoxins, and was successfully applied inAstragalus membranaceussamples. The presented aptasensor for OTA detection could be a promising tool for the field monitoring of food and TCM.Keywords:ochratoxin A;porphyrin;quantum dots;G-quadruplex aptamerKey Contribution:A label-free fluorescent aptasensor for the sensitive determination of ochratoxin A utilizing the interaction between OTA-triggered G-quadruplex and TMPyP is reported.
研究领域:
食品安全
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分析化学
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生物技术
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DOI
PubMed
高影响因子
Catalysts
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2022
·Vol. 12
·期 6
·671
·
IF 4.501
Chenhui Qi,Shuaipeng Han,Jialiang Lin,Jianhua Cheng,Kesi Du,Yongyou Hu,Yuancai Chen
Photoelectro-Fenton (PEF) process can continuously promote the occurrence of Fenton reaction and the generation of active species, which is an advanced oxidation technology for pollutant degradation. However, the lack of bifunctional catalysts restricts the development of PEF technology. In this study, the electronic rearrangement MOF-525 modified by metalloporphyrin (named MOF-525-Fe/Zr) was prepared, to load on the carbon felt as a novel cathode catalyst, which is used in PEF process. A series of characterization and photoelectric chemical properties tests combined with DFT calculation showed that the modification of MOF-525 could not only have the large specific surface area and multistage pore structure but also co-stimulate the metal-to-ligand charge transfer (MLCT) and ligand-to-cluster charge transfer (LCCT) by photoelectric synergy. These charge transitions provide periodic electron donor-acceptor conduction paths in MOF-525-Fe/Zr, which can improve the active species formation and transfer efficiency. Owing to their favorable pore and electronic structure as well as stability, MOF-525-Fe/Zr shows great promise for the application in the catalytic process of PEF. Sulfamethoxazole (SMX) degradation was enhanced by MOF-525-Fe/Zr with the TOC removal rate above 75% both in river water and tap water. Finally, the reasonable pathway of PEF catalytic degradation of SMX was proposed by HPLC-MS analysis. In conclusion, this study provides a new idea for reconstructing the electronic structure of MOFs catalyst and broadening the practical application of PEF technology.Keywords:photoelectro-Fenton;MOF-525;metal-to-ligand charge transfer;ligand-to-cluster charge transfer;sulfamethoxazole
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Small
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2024
·
IF 13
Hongyuan Cui,Tianfang Zheng,Nana Qian,Xueqi Fu,Aijun Li,Shu Xing,Xiao-Feng Wang
Exosomes are nanovesicles secreted by cells, which play a crucial role in various pathological processes. Exosomes have shown great promise as tumor biomarkers because of the abundant secretion during tumor formation. The development of a convenient, efficient, and cost-effective method for simultaneously enriching and detecting exosomes is of utmost importance for both basic research and clinical applications. In this study, an aptamer-functionalized magnetic Ti 3 C 2 composite material (Fe 3 O 4 @Ti 3 C 2 @PEI@DSP@aptamer@FAM-ssDNA) is prepared for the simultaneous enrichment and detection of exosomes. CD63 aptamers are utilized to recognize and capture the exosomes, followed by magnetic separation. The exosomes are then released by cleaving the disulfide bonds of DSP. Compared to traditional methods, Fe 3 O 4 @Ti 3 C 2 @PEI@DSP@aptamer@FAM-ssDNA exhibited superior efficiency in enriching exosomes while preserving their structural and functional integrity. Detection of exosome concentration is achieved through the fluorescence quenching of Ti 3 C 2 and the competitive binding between the exosomes and a fluorescently labeled probe. This method exhibited a low detection limit of 4.21 × 10 4 particles mL −1 , a number that is comparable to the state-of-the-art method in the detection of exosomes. The present study demonstrates a method of simultaneous enrichment and detection of exosomes with a high sensitivity, accuracy, specificity, and cost-effectiveness providing significant potential for clinical research and diagnosis.
研究领域:
纳米技术
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生物标志物研究
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癌症诊断
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分子生物学
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产品关联
DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2022
·
IF 16.383
Wenge Zhang,Pei-Chao Zhang,Yin-Lin Li,Hai-Hong Wu,Junliang Zhang
Asymmetric cycloaddition reactions are the most powerful tool to the expeditious construction of enantioenriched cyclic motifs in organic chemistry. In sharp contrast to well-developed cycloaddition reactions via the palladium-trimethylenemethane (Pd-TMM) intermediate, hetero (3 + 2) cycloadditions of the heteroallyl cations remain rare, largely due to their thermally forbidden nature. To the best of our knowledge, there is no example of asymmetric version leading to enantioenriched heterocycles reported so far. Herein we enabled the first example of catalytic asymmetric (3 + 2) cycloaddition of electrophilic palladium-heteroallyl zwitterion intermediate (Pd-OTMM or Pd-NTMM) with cyclic or acyclic 1,3-dienes via a pathway terminated with C–N or C–O bond formation, delivering the highly substituted or fused pyrrolidine and tetrahydrofuran rings in high yields with excellent regio-, diastereo-, and enantioselectivity. Engineering the PC-Phos, one of the chiral sulfinamide phosphine (Sadphos) type ligands, by introducing the di-tert-butyl or/and 3,5-difluorophenyl group is a vital component in achieving excellent catalytic reactivity and enantioselectivity.
研究领域:
有机化学
·
催化化学
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DOI
高影响因子
APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 35
·期 1
·e6045
·
IF 3.14
Zhuming Guo,Jing Jin,Zhiyin Xiao,Naiwen Chen,Xiujuan Jiang,Xiaoming Liu,Lingfeng Wu,Yi He,Shuhua Zhang
Four iron(II) carbonyl complexes, fac -[Fe (CO) 3 X 2 (py)] (X = I − , 1 and Br − , 3 ), fac -[{Fe (CO) 3 X 2 } 2 (bipy)] (X = I − , 2 and Br − , 4 ), were facilely synthesized by reacting cis -[Fe (CO) 4 X 2 ] (X = I − , Br − ) with pyridine (py) and 4,4′-dipyridine (bipy) ligands, respectively, in good yields (70%~85%). These complexes were fully characterized, and the structures of Complexes 2 and 3 were crystallographically analyzed. In dimethyl sulfoxide, they decomposed rapidly to release carbon monoxide (CO), and in methanol, they showed better stability which allowed kinetically analyzing their decomposing behaviors. The self-decomposing in methanol fitted first-order kinetics with a half-time ranging from several minutes to 1 h. Our results suggested that the ligand with great conjugation (bipy) and strong electron-donating capability (iodide) could stabilize the iron(II) carbonyl complexes. The decomposition of the iodo complexes ( 1 and 2 ) involved the production of iodine radicals. MTT (3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl tetrazolium bromide) assessments revealed that the efficacy against human bladder carcinoma cell line (RT112) is in the following trend: 1 > 2 > 3 > 4 . The relatively strong efficacy of Complexes 1 and 2 is mainly contributed to the in situ generated iodine radicals. The combination of the cytotoxicity of the in situ generated radicals with the anticancer activity of CO as reported in literatures may lead to developing novel anticancer drugs with enhanced efficacy.
研究领域:
无机化学
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药物化学
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生物化学
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
·Vol. 12
·期 12
·4007-4018
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IF 6.4
Hong-Juan Lv,Yunhui Zhai,Ying-Ying Xue,Jiao Lei,Wenyu Yuan,Quan-Guo Zhai
Adsorption-based separation techniques are pivotal in the purification of C2H2, leveraging their eco-friendly and energy-efficient attributes. However, the reusability of adsorbents is highly restricted by the trade-off between adsorption capacity and adsorption enthalpy, which is required to be urgently addressed. Herein, we demonstrated that the implantation of distortable ligands with functional groups is efficient in solving the above issue. The functional groups provided binding sites for C2H2 adsorption, while the distortable ligands optimized the pore structures to reduce adsorption enthalpy, thus balancing the trade-off between adsorption capacity and enthalpy. A series of ultra-microporous MOFs was successfully constructed by employing different pyridine ligands. The adsorption capacity of SNNU-504 after optimization was effectively enhanced, while the adsorption enthalpy hardly increased due to the adjustable ligand torsion angle. Breakthrough experiments and GCMC simulations further verified the potential C2H2/CO2 separation applications.
研究领域:
材料科学
·
化学工程
·
吸附技术
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分离科学
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纳米多孔材料
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）