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JOURNAL OF MOLECULAR STRUCTURE · 2021 · IF 3.196

Slow magnetic relaxation in mixed-valence coordination polymer, containing Co(III) cluster and Co(II) nodes

Jingyan Zhu,Baolin Liu,Weibing Zhang,Jun Jiang,Xinhua Li

Single-molecule magnets in cobalt clusters is much less well known than it is in manganese(II)/(III)/(IV) clusters. To explore new types of cobalt clusters and their potential applications, a new mixed valence coordination polymer ([Co(III) 3 Co(II) 2 (mba) 6 (Hdtba) (H 2 O) 4 ] n , H 2 dtba=2,2’-dithiodibenzoic acid, H 2 mba=2-mercaptobenzoic acid) ( 1 ) is constructed by employing cobalt chloride hexahydrate and H 2 mba as starting reactants under hydrothermal conditions. Single-crystal XRD studies indicate that 1 consists of a trinuclear cobalt(III)-sulfur cluster moiety and two discrete cobalt(II) nodes, which result in the formation of a covalent three-dimensional complex network. Similarly, the cobalt(III) cluster moiety acts as a building unit in this infinite coordination polymer 1 instead of the discrete and tiara-like clusters previously reported in the literature. Magnetic studies show its slow magnetic relaxation in the absence of an applied dc field, which is characteristic behavior of single-ion magnets, caused by the individual Co(II) ions.

CAS / MDL: 7791-13-1
研究领域: 无机化学 · 材料科学
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POLYHEDRON · 2021 · IF 3.052

A novel Dy4 cluster constructed by an 8‑hydroxyquinoline Schiff base showing remarkable single molecule magnet behavior

Hai-Tang Wang,Jin-Rong Pu,Xin Li,Yue Zhang,Ying Zhang,Li Li,Ming Fang

The construction of polynuclear Ln(III)-based clusters toward interesting topological structures and outstanding magnetic properties is a critical challenge for chemists. Herein, by using a flexible Schiff base ligand H 2 L, a novel Dy 4 cluster with the formula {Dy 4 (acac) 4 L 4 }·solvent ( 1 ) (Hacac =  acetylacetone , and H 2 L = pyridine-2-carboxylic acid (8-hydroxy-quinolin-2-ylmethylene)-hydrazide), has been synthesized, structurally and magnetically studied. The X-ray structural analysis suggests cluster 1 is a tetranuclear dysprosium compound, and the four central Dy(III) ions are connected by eight bridging N atoms of four H 2 L forming a quadrilateral Dy 4 core. It is interesting that more than one magnetic relaxation processes were clearly observed in the 1-Dy 4 cluster under H dc  = 0 Oe field.

研究领域: 无机化学 · 磁性材料科学
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ANALYTICA CHIMICA ACTA · 2022 · IF 6.911

CRISPR/Cas13a assisted amplification of magnetic relaxation switching sensing for accurate detection of miRNA-21 in human serum

Xin Guo,Tian Tian,Xinchun Deng,Yang Song,Xiaoming Zhou,Erqun Song

Development of rapid and accurate detection of miRNAs in complex samples is of great significance for potential early diagnosis of disease. Herein, we report a magnetic relaxation switching (MRS)-based strategy for direct detection of miRNAs in complex samples via the assistance of signal amplification system of CRISPR/Cas13a which has the ability to specifically recognize target RNA. In the designed strategy, 30 nm-magnetic nanoparticles (MB 30 ) and 1000 nm-magnetic particles (MM 1000 ) linked by single-strand RNA 1 complexes (MB 30 -RNA 1 - MM 1000 ) were employed as signal probe. After the target miRNAs (taking miR-21 as model) recognition by CRISPR/Cas13a system, the resulted trans -cleavage degrades the MB 30 -RNA 1 -MM 1000 , releasing MB 30 which caused transverse relaxation time (T 2 ) signal change. The combination of CRISPR/Cas13a assisted signal amplification and the MRS assay achieved direct detection of miR-21 in the serum sample without extracting within 60min, with a detection limit of 0.22 pM. Moreover, the detection accuracy is confirmed by performing the detection of miR-21 using qRT-PCR. The CRISPR/Cas13a system assisted MRS assay successfully achieved accurate, simple, and rapid detection of miRNAs in complex samples, showing great potential for detection miRNAs in potential clinical applications.

CAS / MDL: 288-32-4 51805-45-9
研究领域: 分子生物学 · 医学诊断 · 生物技术
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JOURNAL OF HAZARDOUS MATERIALS · 2024 · IF 12.2

Pd/Cu-TCPP(Fe)-polydopamine mediated magnetic relaxation switching immunosensor for sensitive detection of chlorpyrifos

Yongzhen Dong,Jiawei Liu,Liqin Kong,Dongyang Deng,Long Wu,Yiping Chen

This study presents the development of a magnetic relaxation switching (MRS) immunosensor for the sensitive detection of chlorpyrifos (CPF) with a signal amplification strategy using Pd/Cu-TCPP(Fe) hybrid nanosheets and polydopamine (PDA). Pd/Cu-TCPP(Fe) nanosheets, which exhibit high peroxidase-like activity and excellent storage stability, making them suitable replacements for natural enzymes in biosensors, are further functionalized with goat anti-mouse IgG (Ab 2 ) to construct an immunosensor. The mechanism relies on the competition between free CPF and the immobilized bovine serum albumin-CPF conjugates for antibody binding, which modulates the aggregation of magnetic nanoparticles (MNPs) that are related to the transverse relaxation time. The optimized immunosensor shows a linear detection range from 0.5 ng/mL to 100 ng/mL and a limit of detection (LOD) of 0.24 ng/mL, outperforming traditional enzyme-linked immunosorbent assay (ELISA) methods by achieving an LOD that is about 9 times lower. Real sample analysis demonstrates the applicability of the Pd/Cu-TCPP(Fe)-PDA-MRS immunosensor for detecting CPF residues in tomato and water samples, with results well consistent with those obtained using gas chromatography. This work highlights the potential of nanomaterials in enhancing the performance of MRS immunosensors for pesticide residue analysis in environmental and food safety monitoring.

研究领域: 分析化学 · 环境科学 · 食品安全
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Science China-Materials · 2021 ·Vol. 65 ·期 2 ·477-485 · IF 8.273

Glassy magnetic ground state in layered compound MnSb2Te4

Li Hao,Li Yaoxin,Lian Yukun,Xie Weiwei,Chen Ling,Zhang Jinsong,Wu Yang,Fan Shoushan

As a sister compound of MnBi 2 Te 4 , the high-quality MnSb 2 Te 4 single crystals are grown via solid-state reaction where prolonged annealing and narrow temperature window play critical roles on account of its thermal metastability. Single-crystal X-ray diffraction (SCXRD) analysis on MnSb 2 Te 4 illustrates a crystal model that is isostructural to MnBi 2 Te 4 , consisting of Te-Sb-Te-Mn-Te-Sb-Te septuple layers (SLs) stacking in an ABC sequence. However, MnSb 2 Te 4 reveals a more pronounced cation intermixing in comparison with MnBi 2 Te 4 , comprising 28.9(7)% Sb antisite defects on the Mn (3a) site and 19.3(6)% Mn antisite defects on the Sb (6c) site, which may give rise to novel magnetic properties in emerging layered MnBi 2 Te 4 -family materials. Unlike the antiferromagnetic (AFM) nature in MnBi 2 Te 4 , MnSb 2 Te 4 exhibits a glassy magnetic ground state below 24 K and can be easily tuned to a ferromagnetic state under a weak applied magnetic field. Its magnetic hysteresis, anisotropy, and relaxation process are investigated in detail via static and dynamic magnetization measurements. Moreover, anomalous Hall effect as a p-type conductor is demonstrated with transport measurements. This work grants MnSb 2 Te 4 a possible access to the future exploration of exotic quantum physics by removing the odd/even layer number restraint in realizing quantum transport phenomena in intrinsic AFM MnBi 2 Te 4 -family materials, as a result of the crossover between its magnetism and potential topology arising from the Sb-Te layer.

研究领域: 凝聚态物理 · 材料科学 · 磁学 · 量子输运 · 晶体化学
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SENSORS AND ACTUATORS B-CHEMICAL · 2021 · IF 7.46

Magnetic graphene quantum dots facilitate closed-tube one-step detection of SARS-CoV-2 with ultra-low field NMR relaxometry

Yongqiang Li,Peixiang Ma,Quan Tao,Hans-Joachim Krause,Siwei Yang,Guqiao Ding,Hui Dong,Xiaoming Xie

The rapid and sensitive diagnosis of the highly contagious severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) is one of the crucial issues at the outbreak of the ongoing global pandemic that has no valid cure. Here, we propose a SARS-CoV-2 antibody conjugated magnetic graphene quantum dots (GQDs)-based magnetic relaxation switch (MRSw) that specifically recognizes the SARS-CoV-2. The probe of MRSw can be directly mixed with the test sample in a fully sealed vial without sample pretreatment, which largely reduces the testers’ risk of infection during the operation. The closed-tube one-step strategy to detect SARS-CoV-2 is developed with home-made ultra-low field nuclear magnetic resonance (ULF NMR) relaxometry working at 118 μT. The magnetic GQDs-based probe shows ultra-high sensitivity in the detection of SARS-CoV-2 due to its high magnetic relaxivity, and the limit of detection is optimized to 248 Particles mL ‒1 . Meanwhile, the detection time in ULF NMR system is only 2 min, which can significantly improve the efficiency of detection. In short, the magnetic GQDs-based MRSw coupled with ULF NMR can realize a rapid, safe, and sensitive detection of SARS-CoV-2.

CAS / MDL: 19598-90-4 2615-15-8
研究领域: 生物医学工程 · 病毒学 · 分子诊断
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Magnetochemistry · 2025 ·Vol. 11 ·期 12 ·102 · IF 2.5

Dysprosium Complexes Incorporating Halogen-Substituted Anthracene: Piezochromism and Single-Molecule Magnet Properties

Ye-Hui Qin,Qian-Qian Su,Song-Song Bao,Li-Min Zheng

Lanthanide-based single-molecule magnets (Ln-SMMs) showing stimuli-responsive changes in photoluminescence (PL) and magnetic properties are attractive for their potential applications in information storage and molecular devices. In this work, we report two mononuclear complexes, namely, Dy(SCN)2(NO3)(Cl-depma)2(4-hpy)2(Dy-Cl) and Dy(SCN)2(NO3)(Br-depma)2(4-hpy)2(Dy-Br), where X-depma represents 10-X-9-diethylphosphinomethylanthracene (X = Cl, Br) and 4-hpy is 4-hydroxypyridine. Both contain face-to-face π-π-interacted anthracene rings and exhibit yellow-green excimer emission. Unlike the other related Dy–anthracene complexes without a halogen substituent,Dy-ClandDy-Brcannot undergo photocycloaddition reaction under UV-light irradiation. However, they exhibited remarkable grinding-induced changes in luminescence. Magnetic studies revealed thatDy-ClandDy-Brshow SMM behavior under zero dc field with the effective energy barriers (Ueff/kB) of 259 K and 264 K, respectively. We also investigated the effect of pressure on the magnetic properties ofDy-Brand observed a reduction in the magnetization value, narrowing of the butterfly-shaped hysteresis loop, and acceleration of the magnetic relaxation under 1.09 GPa. The results demonstrate that introducing a halogen substituent into an anthracene group may pose significant influences on the photophysical and photochemical properties of the complexes. In addition, pressure may be a promising external stimulus to modulate the PL and SMM behaviors of Dy–anthracene complexes.

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INORGANIC CHEMISTRY · 2023 · IF 4.6

A Combined Synthetic, Magnetic, and Theoretical Study on Enhancing Ligand-Field Axiality for Dy(III) Single-Molecule Magnets Supported by Ferrocene Diamide Ligands

Kexin Yang,Rong Sun,Jingliang Zhao,Chong Deng,Bingwu Wang,Song Gao,Wenliang Huang

Molecular design is crucial for improving the performance of single-molecule magnets (SMMs). For dysprosium(III) SMMs, enhancing ligand-field axiality is a well-suited strategy to achieve high-performance SMMs. We synthesized a series of dysprosium(III) complexes, (NNTIPS)DyBr(THF)2 (1, NNTIPS = fc(NSiiPr3)2; fc = 1,1′-ferrocenediyl, THF = tetrahydrofuran), [(NNTIPS)Dy(THF)3][BPh4] (2), (NNTIPS)DyI(THF)2 (3), and [(NNTBS)Dy(THF)3][BPh4] (4, NNTBS = fc(NSitBuMe2)2), supported by ferrocene diamide ligands. X-ray crystallography shows that the rigid ferrocene backbone enforces a nearly axial ligand field with weakly coordinating equatorial ligands. Dysprosium(III) complexes 1–4 all exhibit slow magnetic relaxation under zero fields and possess high effective barriers (Ueff) around 1000 K, comparable to previously reported (NNTBS)DyI(THF)2 (5). We probed the influences of structural variations on SMM behaviors by theoretical calculations and found that the distribution of negative charges defined by rq, i.e., the ratio of the charges on the axial ligands to the charges on the equatorial ligands, plays a decisive role. Moreover, theoretical calculations on a series of model complexes 1′–5′ without equatorial ligands unveil that the axial crystal-field parameters B20 are directly proportional to the N–Dy–N angles and support the hypothesis that enhancing the ligand-field axiality could improve SMM performance.

研究领域: 无机化学 · 配位化学 · 分子磁性 · 材料科学 · 理论化学
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

A magnetic relaxation switching and visual dual-mode sensor for selective detection of Hg2+ based on aptamers modified Au@Fe3O4 nanoparticles

Yuanyuan Liu,Zhaoxia Cai,Long Sheng,Meihu Ma,Xiaoyun Wang

The solvated mercuric ion (Hg 2+ ) from industrial pollutants are highly toxic to the ecological environment and human health. Driven by urgent need for the selective and sensitive detection of Hg 2+ , a magnetic relaxation switching (MRS) based on Fe 3 O 4 nanoparticles (NPs) was designed. Practically, the concentrations of Hg 2+ in industrial pollutant is usually much higher than the detection range. Thus, gold nanoparticles (AuNPs) were synthesized on the surface of Fe 3 O 4 NPs to enable the visual detection of [email protected] 3 O 4 NPs. The presence of Hg 2+ in sample can specifically cause the aggregation of [email protected] 3 O 4 -aptamers NPs through T-Hg 2+ -T base pairs, leading to the change in transverse relaxation time T 2 value of detection solution. The MRS sensor showed excellent response for Hg 2+ ions in the range of 10 nM-100 nM and 100 nM to 5 μM. A highly sensitive and selective measurement of Hg 2+ was obtained with a limit of detection of 2.7 nM. Noticeably, the visual detection can qualitatively analyze the Hg 2+ beyond 5 μM by naked eye without advanced instrumentation and skilled operators.

CAS / MDL: 7439-97-6
研究领域: 环境科学 · 分析化学 · 纳米技术 · 毒理学
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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

Graphene quantum dots-based magnetic relaxation switch involving magnetic separation for enhanced performances of endoglin detection using ultra-low-field nuclear magnetic resonance relaxometry

Yongqiang Li,Zhifeng Shi,Liuyang Shang,Quan Tao,Qisheng Tang,Hans-Joachim Krause,Siwei Yang,Guqiao Ding,Hui Dong

Magnetic relaxation switches (MRS) based on target-induced state changes of magnetic nanoparticles are vital approaches for biomolecule detection in in vitro diagnosis. Recently, magnetic graphene quantum dots have been employed as magnetic probes instead of iron oxide nanoparticles and showed high sensitivity. Introducing magnetic separation into an MRS assay before the relaxometry measurements can enhance the sensitivity, elevate accuracy, and expand the linear region. In this work, magnetic separation-assisted MRS was developed to detect endoglin utilizing iron oxide as the magnetic carrier and magnetic graphene quantum dots as the magnetic probe. The assay possesses a broad linear region from 5 ng/mL to 50 μg/mL and a sensitive limit of detection of 1.3 ng/mL, which is two orders of magnitude lower than that of MRS without magnetic separation. The high accuracy and consistency have been proved for endoglin (CD105) detection in real samples. This graphene quantum dot-based MRS involving magnetic separation provides a new route for enhancing the sensitivity and accuracy of biomolecule detection.

研究领域: 生物分子检测 · 纳米技术 · 磁共振 · 体外诊断
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