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学者姓名:郑彦臻

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Effect of ligand substitution on the SMM properties of three isostructural families of double-cubane Mn(4)Ln(2) coordination clusters EI SCIE Scopus
期刊论文 | 2018 , 47 (10) , 3485-3495 | DALTON TRANSACTIONS
WoS CC Cited Count: 1
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Abstract :

Three isostructural lanthanide series with a core of Mn(2)(III)Mn(2)(II)Ln(2) are reported. These three families have the formulae of [Mn(2)(III)Mn(2)(II)Ln(2)(mu(4)-O)(2)(H(2)edte)(2)(piv)(6)(NO3)(2)] {no crystallization solvent, Ln = La, Ce, Pr, Nd, Eu (1-4, 6); solv = 3MeCN, Ln = Sm, Gd, Tb, Dy, Ho, Er, Tm, Yb, Y (5, 7-13)}, where H(2)edte = N, N, N', N'-tetrakis(2-hydroxyethyl) ethylenediamine and piv = pivalate; [Mn(2)(III)Mn(2)(II)Ln(2)(mu(4)-O)(2)(H(2)edte)(2)(benz)(6)(NO3)(2)], where benz = benzoate, or [Mn(2)(III)Mn(2)(II)Ln(2)(mu(4)-O)(2)(edteH(2))(2)(benz)(6)(NO3)(2)]center dot 2MeCN {Ln = Gd, Tb, Dy (14-16); and [Mn(2)(III)Mn(2)(II)Ln(2)(mu(4)-O)(2)(edteH(2))(2)(piv)(8)]center dot solv {solv = 4MeCN, Ln = La (17); solv = 2MeCN center dot tol center dot H2O, Ln = Pr, Nd, Sm, Tb (18-20, 22); solv = 2MeCN center dot H2O, Ln = Gd (21). These compounds crystallize in two different systems, namely, monoclinic in the space groups P2(1)/n for 1-4, 6, and 14-16 and C2/c for 5, 7-13, 18-20, and 22 and triclinic in the space group P (1) over bar for 17 and 21. The crystal structures of these compounds display a face-fused dicubane structure connected by different types of bridged oxygen atoms. Solid-state dc magnetic susceptibility characterization was carried out for 1-22, and fitting showed that Mn-III. . .Mn-III is antiferromagnetically (AF) coupled and Mn-II. . . Mn-III, Mn-II. . .Ln and Mn-III. . .Ln are weakly ferromagnetically coupled. In addition, ac measurements were carried out and showed that only 7, 15, and 22 for Tb, 8 and 16 for Dy, and 20 for Sm exhibited slow magnetization relaxation. In the case of 15, it was possible to determine the energy barrier of the slow-relaxation behavior by fitting peak temperatures to the Arrhenius law, which gave a value of U-eff = 21.2 K and a pre-exponential factor of tau(0) = 4.0 x 10(-9) s.

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GB/T 7714 Akhtar, Muhammad Nadeem , Lan, Yanhua , AlDamen, Murad A. et al. Effect of ligand substitution on the SMM properties of three isostructural families of double-cubane Mn(4)Ln(2) coordination clusters [J]. | DALTON TRANSACTIONS , 2018 , 47 (10) : 3485-3495 .
MLA Akhtar, Muhammad Nadeem et al. "Effect of ligand substitution on the SMM properties of three isostructural families of double-cubane Mn(4)Ln(2) coordination clusters" . | DALTON TRANSACTIONS 47 . 10 (2018) : 3485-3495 .
APA Akhtar, Muhammad Nadeem , Lan, Yanhua , AlDamen, Murad A. , Zheng, Yan-Zhen , Anson, Christopher E. , Powell, Annie K. . Effect of ligand substitution on the SMM properties of three isostructural families of double-cubane Mn(4)Ln(2) coordination clusters . | DALTON TRANSACTIONS , 2018 , 47 (10) , 3485-3495 .
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Redox-Active Cobalt(II/III) Metal-Organic Framework for Selective Oxidation of Cyclohexene EI SCIE PubMed Scopus
期刊论文 | 2018 , 10 (18) , 15786-15792 | ACS APPLIED MATERIALS & INTERFACES
WoS CC Cited Count: 1
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Abstract :

We report herein a new cobalt(II/III) mixed-valence metal-organic framework formulated as [(CoCo2III)-Co-II(mu(3)-O)(bdc)(3) (tpt)].guest 1, where bdc = benzene-1,4-dicarboxylate and tpt = 2,4,6-tri(4-pyridinyl)-1,3,5-triazine, which can be used as a redox-active heterogeneous catalyst for selective oxidation of cyclohexene on the allylic position without destroying the adjacent double bond. Two oxidants were chosen to demonstrate this result. For using tert-butyl hydroperoxide, the conversion rate is 63% and only allylic oxidation products (tert-butyl-2-cyclohexenyl-1-peroxide, 86%; 2-cydohexen-l-one, 14%) are found, whereas if using O-2 as oxidant, a total conversion of 38% is achieved and also only the allylic oxidation products (cyclohexenyl hydroperoxide, 72%; 2-cyclohexen-l-one, 20%; and cyclohex-2-en-l-ol, 8%) are found. The absence of any adduct on the double bond may be due to the unique radical chain mechanism triggered by the mixed-valent [(CoCo2III)-Co-II(mu(3)-O)] centers.

Keyword :

oxidation metal-organic framework cyclohexene catalysis cobalt

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GB/T 7714 Zhang, Tao , Hu, Yue-Qiao , Han, Tian et al. Redox-Active Cobalt(II/III) Metal-Organic Framework for Selective Oxidation of Cyclohexene [J]. | ACS APPLIED MATERIALS & INTERFACES , 2018 , 10 (18) : 15786-15792 .
MLA Zhang, Tao et al. "Redox-Active Cobalt(II/III) Metal-Organic Framework for Selective Oxidation of Cyclohexene" . | ACS APPLIED MATERIALS & INTERFACES 10 . 18 (2018) : 15786-15792 .
APA Zhang, Tao , Hu, Yue-Qiao , Han, Tian , Zhai, Yuan-Qi , Zheng, Yan-Zhen . Redox-Active Cobalt(II/III) Metal-Organic Framework for Selective Oxidation of Cyclohexene . | ACS APPLIED MATERIALS & INTERFACES , 2018 , 10 (18) , 15786-15792 .
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Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet SCIE PubMed Scopus
期刊论文 | 2018 , 9 | NATURE COMMUNICATIONS
WoS CC Cited Count: 1
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Understanding quantum tunnelling of the magnetisation (QTM) in single-molecule magnets (SMMs) is crucial for improving performance and achieving molecule-based information storage above liquid nitrogen temperatures. Here, through a field-and temperature-dependent study of the magnetisation dynamics of [Dy((BuO)-Bu-t)Cl(THF)(5)][BPh4]center dot 2THF, we elucidate the different relaxation processes: field-independent Orbach and Raman mechanisms dominate at high temperatures, a single-phonon direct process dominates at low temperatures and fields > 1 kOe, and a field- and temperature-dependent QTM process operates near zero field. Accounting for the exponential temperature dependence of the phonon collision rate in the QTM process, we model the magnetisation dynamics over 11 orders of magnitude and find a QTM tunnelling gap on the order of 10(-4) to 10(-5) cm(-1). We show that removal of Dy nuclear spins does not suppress QTM, and argue that while internal dipolar fields and hyperfine coupling support QTM, it is the dynamic crystal field that drives efficient QTM.

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GB/T 7714 Ding, You-Song , Yu, Ke-Xin , Reta, Daniel et al. Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet [J]. | NATURE COMMUNICATIONS , 2018 , 9 .
MLA Ding, You-Song et al. "Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet" . | NATURE COMMUNICATIONS 9 (2018) .
APA Ding, You-Song , Yu, Ke-Xin , Reta, Daniel , Ortu, Fabrizio , Winpenny, Richard E. P. , Zheng, Yan-Zhen et al. Field- and temperature-dependent quantum tunnelling of the magnetisation in a large barrier single-molecule magnet . | NATURE COMMUNICATIONS , 2018 , 9 .
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A Multifunctional Lanthanide Carbonate Cluster Based Metal-Organic Framework Exhibits High Proton Transport and Magnetic Entropy Change SCIE PubMed Scopus
期刊论文 | 2018 , 57 (15) , 9020-9027 | INORGANIC CHEMISTRY
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A novel multifunctional, three-dimensional (3D) lanthanide carbonate cluster based metal organic framework (MOF) with the general formula {[Gd-2(CO3)(ox)(2)(H2O)(2)]3H(2)O}(n) (1) has been synthesized via self-assembly of gadolinium (Gd) carbonate and oxalate under hydrothermal conditions. Single-crystal X-ray diffraction reveals that the compound 1 consists of the Gd carbonate cluster with oxalic acid ligands, which form a 3D framework structure with an ordered one-dimensional (1D) pore channel along the a-axis. The coordination water molecules of Gd3+ ions point to the interior of the pore and form a 1D hydrogen bond pathway with oxygen atoms in adjacent oxalic acid that is stable at high temperature (up to 150 degrees C). The compound 1 features multiple hydrogen-bonding walls and good thermal stabilities, and shows the highest proton conductivity of 1.98 x 10(-3) S cm(-1) at T = 150 degrees C and in room air without additional humidity. Magnetic investigations of compound 1 demonstrate that weak antiferromagnetic couplings between adjacent Gd3+ ions bring about large cryogenic magnetocaloric effects. Remarkably, the maximum entropy change (-Delta S-m) of compound 1 reaches 58.5 J kg(-1) K-1 at 2 K for a moderate field change (Delta H = 7 T). Moreover, the isomorphous MOFs: {[Ln(2)(CO3)(ox)(2)(H2O)(2)]3H(2)O}(n) (Ln(3+) = Ce3+(2), Pr3+(3), Nd3+(4), Tb3+(5)) also are structurally and functionally characterized, and compounds 2-5 exhibit proton conductivity above 10(-3) S cm(-1) in room air and without additional humidity.

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GB/T 7714 Tang, Qun , Yang, Yan-Li , Zhang, Ning et al. A Multifunctional Lanthanide Carbonate Cluster Based Metal-Organic Framework Exhibits High Proton Transport and Magnetic Entropy Change [J]. | INORGANIC CHEMISTRY , 2018 , 57 (15) : 9020-9027 .
MLA Tang, Qun et al. "A Multifunctional Lanthanide Carbonate Cluster Based Metal-Organic Framework Exhibits High Proton Transport and Magnetic Entropy Change" . | INORGANIC CHEMISTRY 57 . 15 (2018) : 9020-9027 .
APA Tang, Qun , Yang, Yan-Li , Zhang, Ning , Liu, Zheng , Zhang, Shu-Hua , Tang, Fu-Shun et al. A Multifunctional Lanthanide Carbonate Cluster Based Metal-Organic Framework Exhibits High Proton Transport and Magnetic Entropy Change . | INORGANIC CHEMISTRY , 2018 , 57 (15) , 9020-9027 .
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Pseudotetrahedral cobalt(II) complexes with PNP-ligands showing uniaxial magnetic anisotropy EI SCIE PubMed
期刊论文 | 2018 , 47 (27) , 8874-8878 | DALTON TRANSACTIONS
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Two mononuclear pseudotetrahedral cobalt(II) complexes with the formula Co(PNP)X-2, where X = Cl (1) or X = SCN (2) and PNP = bis(2-(diphenylphosphaneyl)-4-methylphenyl)amine, have been synthesised. Magnetic and high-frequency/field electron paramagnetic resonance (HF-EPR) spectroscopy and ab initio calculation studies reveal that both complexes show uniaxial magnetic anisotropy.

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GB/T 7714 Zhai, Yuan-Qi , Deng, Yi-Fei , Zheng, Yan-Zhen . Pseudotetrahedral cobalt(II) complexes with PNP-ligands showing uniaxial magnetic anisotropy [J]. | DALTON TRANSACTIONS , 2018 , 47 (27) : 8874-8878 .
MLA Zhai, Yuan-Qi et al. "Pseudotetrahedral cobalt(II) complexes with PNP-ligands showing uniaxial magnetic anisotropy" . | DALTON TRANSACTIONS 47 . 27 (2018) : 8874-8878 .
APA Zhai, Yuan-Qi , Deng, Yi-Fei , Zheng, Yan-Zhen . Pseudotetrahedral cobalt(II) complexes with PNP-ligands showing uniaxial magnetic anisotropy . | DALTON TRANSACTIONS , 2018 , 47 (27) , 8874-8878 .
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"Merged-chelating" approach for constructing high-spin Mn aggregate: A [Mn-2(III)] dimer and a 2-D honeycomb network based on star-shaped [Mn-II Mn-3(III)] tetramer SCIE Scopus
期刊论文 | 2018 , 148 , 44-48 | POLYHEDRON
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Pyridin-2-ylmethanols (hmp) and 1, 3-propanediols have been proven to be successful ligands for constructing high-spin manganese clusters. In this work, both ligands are merged into one framework, resulting in a new tridentate ligand 4-chloro-2-(hydroxy(pyridin-2-yl)methyl)phenol. Its initial attempt in Mn coordination chemistry harvested a Mn-III dimer [Mn-2(III)(L)(2)(AcAc)(2)] and a 2-D honeycomb network based on star-shaped [(MnMn3III)-Mn-II] tetramer {[(MnMn3III)-Mn-II(Na)(1.5)(L)(6)](OH)(0.)(5)center dot(MeOH)(1.5)}(n). The two clusters were characterized by single crystal X-ray diffraction, IR spectra, elemental analysis, and magnetic measurements. Magnetic studies revealed dominant ferromagnetic interactions within the Mn-III dimer and star-shaped [(MnMn3III)-Mn-II] tetramer unit. (C) 2018 Elsevier Ltd. All rights reserved.

Keyword :

High spin molecules Mn clusters Magnetism Ligand design Coordination network

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GB/T 7714 Bai, Jiaquan , Yang, Chao , Li, Guanghua et al. "Merged-chelating" approach for constructing high-spin Mn aggregate: A [Mn-2(III)] dimer and a 2-D honeycomb network based on star-shaped [Mn-II Mn-3(III)] tetramer [J]. | POLYHEDRON , 2018 , 148 : 44-48 .
MLA Bai, Jiaquan et al. ""Merged-chelating" approach for constructing high-spin Mn aggregate: A [Mn-2(III)] dimer and a 2-D honeycomb network based on star-shaped [Mn-II Mn-3(III)] tetramer" . | POLYHEDRON 148 (2018) : 44-48 .
APA Bai, Jiaquan , Yang, Chao , Li, Guanghua , Bi, Yanfeng , Li, Xiaolei , Tang, Jinkui et al. "Merged-chelating" approach for constructing high-spin Mn aggregate: A [Mn-2(III)] dimer and a 2-D honeycomb network based on star-shaped [Mn-II Mn-3(III)] tetramer . | POLYHEDRON , 2018 , 148 , 44-48 .
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Quantum Monte Carlo simulations of a giant {Ni21Gd20} cage with a S=91 spin ground state SCIE PubMed Scopus
期刊论文 | 2018 , 9 | NATURE COMMUNICATIONS
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The detailed analysis of magnetic interactions in a giant molecule is difficult both because the synthesis of such compounds is challenging and the number of energy levels increases exponentially with the magnitude and number of spins. Here, we isolated a {Ni21Gd20} nanocage with a large number of energy levels (approximate to 5 x 10(30)) and used quantum Monte Carlo (QMC) simulations to perform a detailed analysis of magnetic interactions. Based on magnetization measurements above 2 K, the QMC simulations predicted very weak ferromagnetic interactions that would give a record S = 91 spin ground state. Low-temperature measurements confirm the spin ground state but suggest a more complex picture due to the single ion anisotropy; this has also been modeled using the QMC approach. The high spin and large number of low-lying states lead to a large low-field magnetic entropy (14.1 J kg(-1) K-1 for Delta H = 1 T at 1.1 K) for this material.

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GB/T 7714 Chen, Wei-Peng , Singleton, Jared , Qin, Lei et al. Quantum Monte Carlo simulations of a giant {Ni21Gd20} cage with a S=91 spin ground state [J]. | NATURE COMMUNICATIONS , 2018 , 9 .
MLA Chen, Wei-Peng et al. "Quantum Monte Carlo simulations of a giant {Ni21Gd20} cage with a S=91 spin ground state" . | NATURE COMMUNICATIONS 9 (2018) .
APA Chen, Wei-Peng , Singleton, Jared , Qin, Lei , Camon, Agustin , Engelhardt, Larry , Luis, Fernando et al. Quantum Monte Carlo simulations of a giant {Ni21Gd20} cage with a S=91 spin ground state . | NATURE COMMUNICATIONS , 2018 , 9 .
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Large-scale synthesis of ultrathin lanthanide carbonate hydroxides nanowires for potential biomedical applications CPCI-S SCIE
会议论文 | 2018 , 255 | 255th National Meeting and Exposition of the American-Chemical-Society (ACS) - Nexus of Food, Energy, and Water
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GB/T 7714 Zhang, Xinyu , Li, Yannan , Ge, Juan et al. Large-scale synthesis of ultrathin lanthanide carbonate hydroxides nanowires for potential biomedical applications [C] . 2018 .
MLA Zhang, Xinyu et al. "Large-scale synthesis of ultrathin lanthanide carbonate hydroxides nanowires for potential biomedical applications" . (2018) .
APA Zhang, Xinyu , Li, Yannan , Ge, Juan , Qin, Lei , Zheng, Yanzhen , Lei, Bo et al. Large-scale synthesis of ultrathin lanthanide carbonate hydroxides nanowires for potential biomedical applications . (2018) .
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Lanthanide Clusters Toward Single-Molecule Magnets SCIE Scopus
期刊论文 | 2017 , 173 , 209-314 | RECENT DEVELOPMENT IN CLUSTERS OF RARE EARTHS AND ACTINIDES: CHEMISTRY AND MATERIALS | IF: 2.721
WoS CC Cited Count: 4
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Single-molecule magnets (SMMs) have attracted increasing attention for their potential applications in high-density information storage and quantum computing. Thereinto, polynuclear 4f complexes are excellent candidates to create high-performance SMMs for the advantages of significant single-ion magnetic anisotropy arising from 4f ions and manipulable magnetic exchange couplings via tunable arrangement of the metal ions, which promotes the rapid development of this area in the last decade. In this chapter we present a comprehensive review focusing on cluster-based lanthanide SMMs and their correlations between the molecular structures and magnetic behaviors and further highlight some novel strategies for enhancing SMMs.

Keyword :

Magnetic relaxation Polynuclear 4f complexes Lanthanide Single-molecule magnets

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GB/T 7714 Han, Tian , Ding, You-Song , Zheng, Yan-Zhen . Lanthanide Clusters Toward Single-Molecule Magnets [J]. | RECENT DEVELOPMENT IN CLUSTERS OF RARE EARTHS AND ACTINIDES: CHEMISTRY AND MATERIALS , 2017 , 173 : 209-314 .
MLA Han, Tian et al. "Lanthanide Clusters Toward Single-Molecule Magnets" . | RECENT DEVELOPMENT IN CLUSTERS OF RARE EARTHS AND ACTINIDES: CHEMISTRY AND MATERIALS 173 (2017) : 209-314 .
APA Han, Tian , Ding, You-Song , Zheng, Yan-Zhen . Lanthanide Clusters Toward Single-Molecule Magnets . | RECENT DEVELOPMENT IN CLUSTERS OF RARE EARTHS AND ACTINIDES: CHEMISTRY AND MATERIALS , 2017 , 173 , 209-314 .
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Quantum Monte Carlo Simulations and High-Field Magnetization Studies of Antiferromagnetic Interactions in a Giant Hetero-Spin Ring EI SCIE PubMed Scopus
期刊论文 | 2017 , 56 (52) , 16571-16574 | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | IF: 12.102
WoS CC Cited Count: 7
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Chromium lanthanide heterometallic wheel complexes {Cr(8)Ln(8)} (Ln = Gd, Dy and Y) with alternating metal centres are presented. Quantum Monte Carlo simulations reveal antiferromagnetic exchange-coupling constants with an average of 2.1 K within the {Cr8Gd8} wheel, which leads to a large ground spin state (S-T-16) that is confirmed by magnetization studies up to 20 Tesla. The {Cr8Dy8} wheel is a single-molecule magnet.

Keyword :

exchange coupling cyclic coordination clusters chromium lanthanides single-molecule magnets

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GB/T 7714 Qin, Lei , Singleton, Jared , Chen, Wei-Peng et al. Quantum Monte Carlo Simulations and High-Field Magnetization Studies of Antiferromagnetic Interactions in a Giant Hetero-Spin Ring [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2017 , 56 (52) : 16571-16574 .
MLA Qin, Lei et al. "Quantum Monte Carlo Simulations and High-Field Magnetization Studies of Antiferromagnetic Interactions in a Giant Hetero-Spin Ring" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 56 . 52 (2017) : 16571-16574 .
APA Qin, Lei , Singleton, Jared , Chen, Wei-Peng , Nojiri, Hiroyuki , Engelhardt, Larry , Winpenny, Richard E. P. et al. Quantum Monte Carlo Simulations and High-Field Magnetization Studies of Antiferromagnetic Interactions in a Giant Hetero-Spin Ring . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2017 , 56 (52) , 16571-16574 .
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