SCIENCE OF THE TOTAL ENVIRONMENT
·
2024
·
IF 8.2
Lining Su,Guizhen Wang,Linlin Zhao,Yuan Deng,Yujing Guo,Yong Xiao,Huanwen Wang,Chuan Dong,Lifang Fan
Due to the urgent need for detecting trace amounts of 3,3′,4,4′-tetrachlorobiphenyl (PCB77) in the environment, we have developed an efficient and visible-driven photoelectrochemical (PEC) sensing platform based on carbon quantum dots (CQDs) modified titanium dioxide nanorods (TiO 2 NRs), coupling with exonuclease I (Exo I) assisted in target recycling for significant signal amplification. CQDs/TiO 2 NRs with high visible-light absorption ability and electron-hole separation efficiency is used as photoactive substrate for anchoring anti-PCB77 aptamer and its complementary DNA (cDNA). With the addition of PCB77, the specific interaction between PCB77 and its aptamer forces aptamer to separate from the electrode surface, resulting in an increase in photocurrent density. Adding Exo I in the test system, a self-catalytic target cycle was motivated, which significantly increased the PEC signal by more than twice, achieving signal amplification. The relationship between the photocurrent density changes and the concentrations of PCB77 are utilized to achieve quantitative detection of PCB77. The designed PEC sensing platform has good analytical performance with a detection limit as low as 0.33 pg L −1 , high selectivity and stability. Moreover, the PEC sensor is successfully used to evaluate the content of PBC77 in the environment samples. The established sensing platform provides a simple and efficient method for detecting trace amounts of PCB77 in the environment.
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INORGANICA CHIMICA ACTA
·
2022
·
IF 3.118
Jing-Wen Zhang,Ling-Xiao Wang,Xun Cheng,Lin-Lin Hou,Jing-Zhe Li,Chun-Feng Wang,Xiao-Wei Yan,Kuan-Guan Liu
To prepare new series of mixed-valence polynuclear Cu(I/II) clusters, chloride ions are introduced to construct two mixed-valence polynuclear Cu(I/II) clusters for evaluating their photothermal conversion performance. X-ray single-crystal structural analysis reveals their molecular formula are {Cu II [Cu I (Cy 3 P)] 4 (BTA) 4 Cl 2 }·5DMF (I·5DMF, Cy 3 P = triscyclohexylphosphine, BTA = benzotriazole, DMF = N, N -Dimethylformamide) and {(Cu II ) 3 [Cu I (PPh 2 Py)] 6 (BTA) 8 Cl 4 }·6DMF (II· 6 DMF, Ph 2 PyP = diphenyl-2-pyridylphosphine), respectively. X-ray Photoelectron Spectroscopy (XPS) and Electrospray Ionization Mass Spectrometry (ESI-MS) confirm their chemical composition and charge state. The reported two mixed-valence Cu I /Cu II clusters have different nucleus (penta-nucleus for I and nano-nucleus for II) and different proportion of valence state (1/4 for I vs 1/2 for II). The thermogravimetric analysis (TGA) reveals the thermal stability of both clusters is less than our previously reported penta-nucleus mixed-valence Cu I /Cu II clusters. Contrastively studies of their optical absorption properties by the solid-state ultraviolet diffuse reflection spectra indicate high-nucleus mixed-valence Cu I /Cu II cluster with higher proportion of Cu II is superior to those penta-nucleus mixed-valent Cu(I/II) clusters. With the introduction of chloride ions to the structures of mixed-valence Cu I /Cu II clusters have not remarkably changed their photothermal conversion performance. This study provides a practicable way to construct new mixed-valence Cu I /Cu II clusters with different photothermal conversion performance.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Linjie Wang,Xuechao Xu,Peng Liu,Mengzhu Wang,Xiangheng Niu,Jianming Pan
Abnormal levels of halide ions in drinking water have enormous threats to human health, and thus designing reliable and sensitive methods to quantify and distinguish these ions becomes extremely crucial. Herein, we develop a single-nanozyme colorimetric array based on target-induced differential surface passivation for the quantification and discrimination of Cl − , Br − and I − ions. Silver citrate (Ag 3 Cit) is designed as an oxidase mimic to efficiently catalyze the 3,3′,5,5′-tetramethylbenzidine (TMB) chromogenic reaction. When halide ions (Cl − , Br − and I − ) are present, due to their different precipitation interactions with the Ag(Ⅰ) entity in Ag 3 Cit, they can passivate the active surface of the nanozyme to various degrees, resulting in the inhibited TMB chromogenic reaction differentially. According to this principle, simple and efficient quantitative detection of Cl − , Br − and I − ions was achieved, with all the detection limits down to the nM level. By employing Ag 3 Cit as a single sensing element, a nanozyme catalysis-based colorimetric array was further established, and both individual and mixed ions were successfully distinguished by integrating the array with principal component analysis . Accurate identification of unknown samples was also verified via a double-blind protocol, indicating potential applications of the array in practice.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Zeyan Yu,Shiyue Zhang,Jiyang Liu,Xiaofeng Dong
A homogeneous electrochemical aptasensor was developed for sensitive detection of aflatoxin B1 (AFB1) by integrating ultrasmall silica nanochannel film (SNF)-modified electrode, two-dimensional (2D) nanoprobes, and DNase I-assisted target recycling. The 2D nanoprobes (Ru(NH 3 ) 6 3+ /AFB1 Apt@GO) were prepared by co-loading cationic electrochemical probe Ru(NH 3 ) 6 3+ and AFB1 specific aptamers (AFB1 Apt) onto graphene oxide (GO) via π–π stacking and electrostatic interaction. SNF was rapidly formed on indium tin oxide (ITO) electrodes within 10 s. The resulting structure provided 2–3 nm nanochannels, which enabled the electrostatic enrichment of Ru(NH 3 ) 6 3+ . In addition, the 2D nanoprobes were unable to enter the ultrasmall nanochannels of the SNF due to size exclusion and thus could not access the underlying electrode surface. In the presence of AFB1, aptamer–target binding caused conformational changes and aptamer detachment, releasing Ru(NH 3 ) 6 3+ . The detached aptamer was digested by DNase I, triggering further Ru(NH 3 ) 6 3+ release as AFB1 participated in additional recognition cycles. The released Ru(NH 3 ) 6 3+ was electrostatically enriched at the electrode surface, amplifying the ECL signal. DNase I-assisted recycling enhanced the ECL response by 3-fold compared to the non-enzymatic system. Under optimized conditions, the aptasensor exhibited a linear detection range for AFB1 detection from 3.12 × 10 −4 to 312 ng/mL and a limit of detection of 302 fg/mL. The method was successfully applied to detect AFB1 in corn and peanut samples, offering a simple, rapid, and highly sensitive strategy for electrochemical toxin detection in food safety analysis.
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JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2014
·
IF 2.302
Xuezhu Wang,Yongyong Wang,Jing Zhang,Xiaoli Zhao,Ye Liu
A series of ionic Au(I)-complexes ligated by the phosphine-functionalized ionic liquids were synthesized and characterized, which are composed of the Au(I)-complex cation and the counteranion of OTf − , AuCl 4 − , or PF 6 − , respectively. The single crystal X-ray diffraction analyses show that the Au(I)-centered vector in 1A , 1B , 2A , 3A , and 4A all possess the slightly twisted linear geometry, and in each individual the Au(I)-center is coordinated by one chlorine and one imidazolium-based phosphine. The aggregation of 1B in acetone can lead to the formation of the trinuclear Au(I)-complex of 1C due to the aurophilic Au(I)–Au(I) interaction, the electrostatic attraction, and the steric preference. When these ionic Au-complexes were employed as precatalysts for hydration of phenylacetylene in aqueous-methanol media, the reaction proceeded selectively according to Markovnikov's rule with moderate to high yields of acetophenone . The highest activities were achieved over 2A with hydrophobic PF 6 − as the counteranion and the trinuclear 1C under mild conditions (75 °C, 2 h), in conjunction with the additive of proton acid H 2 SO 4 . The ion-pair effect on the catalytic performance of the corresponding Au(I)-complexes, coming from the phosphine-ligated cations and the counteranions, were investigated.
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POLYHEDRON
·
2014
·
IF 2.047
Xue-Jie Tan,Hai-Zhen Liu,Chong-Zhao Ye,Jian-Fang Lou,Yun Liu,Dian-Xiang Xing,Sen-Peng Li,Shu-Lian Liu,Lai-Zhou Song
Two new ethylenediamine Schiff bases of 2-acetylthiazole and 2-acetylpyrazine (abbreviated as Th-Th and Py-Py respectively), as well as their silver(I) complexes [Ag(Th-Th)] 2 ·2(NO 3 ) and [Ag(Py-Py)] 2 ·2(NO 3 ) , have been prepared and characterized by a variety of physico-chemical techniques including elemental analyses, m.p., 1 H NMR, 13 C NMR, ESI-QTOF-MS, FT/IR, UV–Vis and theoretical calculations including density functional theory (DFT) and time dependent density functional theory (TD-DFT) methods. All structures were solved from single crystal X-ray diffraction (SXRD) data, except [Ag(Py-Py)] 2 ·2(NO 3 ) , whose crystal is not good enough for SXRD. Hence, conventional powder X-ray diffraction (PXRD) has to be used. As a first step, the stoichiometric formula of [Ag(Py-Py)] 2 ·2(NO 3 ) was ascertained by elemental analyses and ESI-QTOF-MS. IR and UV–Vis indicated the existence of coordinated Py-Py and charge-balancing NO 3 - . On the basis of symmetry character proved by NMR, three possible symmetrical Ag(I) coordination structures were designed and optimized by DFT method. Then, relative binding free energies were calculated to find the most appropriate molecule structure. DFT results suggest that four imine-N and four ortho-ring-N atoms from two Py-Py ligands are coordinated to two Ag(I) ions, resulting in a similar dimer structure as that of [Ag(Th-Th)] 2 ·2(NO 3 ) . The molecule structure was further confirmed by PXRD based crystal structure, which was solved following direct space method and refined by the Rietveld method. The antitumor activities of the Schiff bases and their silver(I) complexes have been evaluated against human lung cancer cell line A549. Both silver(I) complexes were found to display cytotoxicity (IC 50 = 3.15 ± 0.5 and 9.73 ± 1.1 μM) that is similar to or better than that of cisplatin, while metal-free Schiff bases show very low activity.
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MOLECULES
·
2018
·Vol. 23
·期 3
·543
·
IF 3.098
Zhi-Feng Li,Meng-Ying Zhou,Ting Tan,Chen-Cong Zhong,Qi Wang,Shi-Lin Yang,Yu-Lin Feng,Hui Ouyang
Ziyuglycoside I (ZGS1) is a promising drug candidate for the treatment of leucopenia. Currently, information on ZGS1 and its in vivo metabolite ziyuglycoside II (ZGS2) is limited. The objective of this study was to investigate the pharmacokinetics, tissue distribution, and excretion of ziyuglycoside I (ZGS1) and its metabolite ziyuglycoside II (ZGS2) in rats. In our study, a simple and sensitive high-performance liquid chromatography-mass spectrometry (HPLC-MS/MS) method was established for simultaneous determination of ZGS1 and its metabolite for Sprague-Dawley rat pharmacokinetics studies. The method was validated following internationally-approved guidelines. The results presented in this study indicated that subcutaneous administration of ZGS1 prolonged its extension time and increased the area under the curve (AUC0–t) of ZGS2 during 0 to t minutes. In summary, in this study, the pharmacokinetic characteristics of ZGS1 and its metabolite ZGS2 were defined and its tissue distribution, and excretion in rats were described. Our finding may be beneficial for leucopenia drug that focus on ZGS1.Keywords:ziyuglycoside I (ZGS1);ziyuglycoside II (ZGS2);LC-MS/MS;pharmacokinetics;tissue distribution;excretion
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JOURNAL OF SEPARATION SCIENCE
·
2025
·Vol. 48
·期 10
·e70271
·
IF 2.8
Man Yang,Tianyu Liu,Wentao Ma,Alimjan Esmayil,Zihang Yu,Kunze Du,Yanxu Chang
An innovative approach combining electrochemistry with online quadrupole time-of-flight-mass spectrometry (EC-MS/MS) was employed to study the oxidative products and metabolic pathways of three bioactive compounds found in Phellodendri Chinensis Cortex , including phellodendrine, obaculactone, and obacunone. This advanced analytical technique provided detailed insights into their transformation processes. The simulation of phase I metabolism reactions was conducted within an electrochemical microreactor system. The heart of this apparatus was a reliably performing boron-doped diamond electrode. Meanwhile, a defined concentration of glutathione (GSH) was injected into the reaction system to obtain phase II metabolites. The metabolites were collected and concentrated for offline electrochemistry-ultra-high-performance liquid chromatography-quadrupole-time of flight-mass spectrometry analysis (EC-UHPLC-MS/MS). The main converted products and metabolic pathways were further verified through in vitro liver microsome incubation experiments. It was revealed that the simulated metabolic process based on the electrochemical system effectively produced a variety of metabolites from the compounds, which were subsequently compared with those obtained from rat liver microsomal incubations. Without matrix interference, the drug metabolic process could be effectively simulated and analyzed using the electrochemical system. The findings underscore the utility of electrochemistry as a robust tool for preliminary investigations into the metabolism of natural products, offering a reliable and efficient alternative to traditional methods.
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Food Analytical Methods
·
2026
·Vol. 19
·期 12
·388
·
IF 3
Deng Guican,Bao Yonghua,Hong Yanping,Hong Jiaxin,Duan Luying,Du Huaying,Tan Zhimei,Wang Chunrong
As illegal synthetic colorants in food, Sudan dyes possess carcinogenic potential and can severely threaten human health following long-term intake. Rapid and sensitive detection of Sudan dyes in complex food matrices (e.g., chili powder and tomato sauce) remains a critical challenge for food safety supervision. Herein, a facile and sensitive detection strategy targeting Sudan I, II, III, and IV was established by combining magnetic substrates with surface-enhanced Raman spectroscopy (SERS). The influence of Au NPs loading on SERS analytical performance was systematically investigated, and FSA-3 was identified as the optimal substrate. Under optimized conditions, the limits of detection (LODs) for Sudan I–IV in chili powder and tomato sauce were determined to be 0.75–11.5 μg/kg, with satisfactory recoveries ranging from 84.5% to 110%. Compared with previously reported SERS methods and conventional analytical techniques, the proposed method exhibits excellent resistance to matrix interference capability and enables sensitive and efficient detection. This work provides a reliable and efficient alternative for the rapid screening of Sudan dye residues in complex food matrices, holding great promise for practical food safety applications.
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Energy Storage Materials
·
2024
·
IF 18.9
Kaiqiang Zhang,Yang Ge,Qianchuan Yu,Pengbo Zhang,Yuge Feng,Zuoxiu Tie,Jing Ma,Zhong Jin
Self-stratified liquid electrode batteries are considered as a viable solution for large-scale energy storage applications due to their high safety and low cost. However, achieving long-term operation stability with high efficiency of selective ion migration/separation in multiple liquid phases remains a challenge. Here, we report an aqueous biphasic system based on imidazolium ionic liquids (ILs) for constructing membrane-free self-stratified aqueous biphasic Zn–I and Zn–Br batteries. The limited intersolubility and density difference between the IL-dominated catholyte and the aqueous anolyte create a self-stratified liquid-liquid phase separation structure, promising a reliable battery construction. Molecular dynamics simulations identify the internal association of IL, which forms a 3D H–bond network with the C–H···O interaction being the primary contributor, along with a thermodynamic electron transfer of ≤0.03 e. Additionally, a unique π + –bond effect is found between the positively charged imidazole ring of cation and the anion of IL. The as-constructed self-stratified aqueous biphasic Zn–halogen batteries work stably without the necessity of air isolation and exhibit long-term cycling stability (with a capacity mentation of 81.0 % for Zn–I batteries and 76.8 % for Zn–Br batteries over 1000 cycles), high energy efficiencies (93.5 % for Zn–I batteries and 86.7 % for Zn–Br batteries), inherent fire resistance and good scalability, demonstrating great potential for large-scale energy storage applications.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2024
·Vol. 416
·期 10
·2541-2551
·
IF 3.8
Niu Yanyan,Chen Yuxue,Zhou Juan,Sun Wei
In this study, an online electrochemistry coupling high-performance liquid chromatography-mass spectrometry (EC-HPLC-MS) technology has been developed for simulating metabolic reactions and rapid analysis of metabolites of flavone, quercetin, and rutin, which are not only widely present compounds with pharmacological activity in nature, but also have structural similarity and variability. The simulated metabolic processes of the substrates (phase I and phase II metabolism) were implemented on the surface of glassy carbon electrode (GCE) by using different electrochemical methods. After online chromatographic separation, the products were transmitted to a mass spectrometer for detection, in order to speculate relevant reaction pathways and structural information of the reaction product. The main metabolites, including methylation, hydroxylation, hydrolysis, and conjugation reaction products, had been successfully identified through the designed in situ hyphenated technique. Furthermore, compared with metabolites produced by in vitro incubation of rat liver microsomes, it was found that the products of electrochemical simulated metabolism were more abundant with diverse metabolic pathways. The results indicated that the proposed method exhibited advantages in the sample pretreatment process and detection cycle without compromising the reliability and accuracy of the results. Graphical
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 33
·44984-45002
·
IF 7.8
Wang Shuaihang,Ji Zhonghao,Shen Ding,Liu Siyu,Hao Jingbin,Cheng Qi,Jia Bao,Guo Liang,Shang Jie,Chen Kai,Han Meng
Currently, the repair of bone defects faces multiple challenges, including insufficient angiogenesis and limited osteogenic differentiation capacity, which pose significant obstacles to treatment. In this study, a ternary composite scaffold composed of PCL-nHA-nMgO (PHM) was fabricated using 3D printing technology. After surface modification with a photothermal polydopamine (PDA) coating, a PHM@PDA composite scaffold was obtained. Metformin (Met) and PDA were loaded into GelMA hydrogels to produce GPM hydrogels. The GPM hydrogels were then packed into the PHM@PDA composite scaffolds, resulting in near-infrared region-I (NIR-I)-responsive PHM@PDA/GPM composite scaffolds. The outer GPM layer serves as a three-dimensional in vivo-like microenvironment, providing physical transport channels for cellular nutrient exchange. Upon stimulation by NIR-I, the scaffold enables the dynamic release of Mg 2+ and Met, upregulates the expression of the VEGF and KDR, accelerates vascular network reconstruction, and creates a mild microenvironment conducive to cell proliferation. Furthermore, by activating the PI3K/AKT signaling pathway, it promotes the expression of osteogenesis-related factors (such as transcription factor Sp7, alkaline phosphatase, and osteocalcin), thereby accelerating the osteogenic differentiation process. In vivo animal experiments, micro-CT and tissue staining confirmed that, under near-infrared light (NIR-I) stimulation, this scaffold significantly increased bone mineral density, trabecular bone thickness, and trabecular bone count and demonstrated excellent angiogenic effects. In summary, this NIR-I-responsive composite scaffold can meet the dual requirements of reconstructing the vascular network and promoting osteogenic differentiation, enabling personalized precision therapy and offering a promising new treatment strategy for complex bone defects where vascular regeneration and osteogenic differentiation are challenging.
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