JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Ziyu Gao,Huidong Wang,Yuchen Hu,Jianmin Sun
Multi-functional MOF catalyst with oxidative- and acid- centers showed potential in olefins oxidative carboxylation to cyclic carbonates directly. In this work, a series of bimetallic MnZn-MOF-74 with different molar ratios of Mn and Zn were synthesized successfully through a one-pot facile method. Thoroughly characterization indicated that the existence of Zn regulated the valance state distribution of Mn in the obtained MnZn-MOF-74. Mn 99.3 Zn 0.7 -MOF-74 with the highest ratio of Mn III (61.3 %) performed the most efficient activity for olefin direct tandem oxidative carboxylation reaction using aqueous tert -butyl hydroperoxide oxidant under solvent-free condition of 90 °C, 1.0 MPa CO 2 and 4 h. Mn 99.3 Zn 0.7 -MOF-74 also showed satisfactory versatility and recyclability. Based on the experiments, a feasible mechanism was presented. Thanks to the high ratio of active Mn III as main oxidative center, the coordination unsaturated bimetal Mn and Zn as Lewis-acid sites, O 2– of metal − O as Lewis-base sites and combined effect with Bu 4 NBr cocatalyst, Mn 99.3 Zn 0.7 -MOF-74 presented efficient performance for the direct synthesis of cyclic carbonates from olefins. The metal Zn in MOF can regulate the valance state distribution of Mn and result in efficient catalytic property, presenting a potential avenue for direct oxidative carboxylation reaction of olefins to cyclic carbonates synthesis.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COORDINATION CHEMISTRY
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2015
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IF 2.012
Qiong Wu,Qing Pu,Yongmei Wu,Hongjuan Shi,Yanfang He,Jun Li,Quanshui Fan
The reaction between manganese nitrate and N,Nʹ-(±)-ethylene-bis(salicylicyclohexanediaminate) ((±)-salcy) in dilute lacunary polyoxoanion [PW9O34]9− solution led to isolation of a new Mn-dimer, [Mn((±)-salcy)(N3)]2 (1). Structural analysis indicates that 1 represents the first salcy-based Mn-dimer complex. Magnetic susceptibility studies reveal that 1 shows single-molecule magnet (SMM) behavior from 2 to 5 K.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaohui Zhan,Junyan Liu,Yue Zhao,Yanping Sun,Rui Gao,He Wang,Huixiang Shi
In this study, we designed and synthesized Mn III with tunable spin state in g-C 3 N 4 through one-step calcination of Mn-MOF. The Mn atoms were induced into the six-fold cavity of the g-C 3 N 4 lattice and formed Mn-N 6 coordination. Mn-MOF served as the source of Mn. The collapse of Mn-MOF effectively promoted the stripping of stacked layers in g-C 3 N 4 and increased the atomic loading. The Mn-N coordination induced impurity energy levels which effectively regulated Mnx-CN's bandgap structure and accelerated the migration and separation of carriers. The O 2 − was activated to 1 O 2 by the energy released from the high-spin Mn III transferred ground state. The H 2 production of Mn 10 -CN (13479.19 µmol·g −1 ·h −1 ) is ∼32.2 times that of CN under visible light irradiation and with a remarkable apparent quantum yield (AQY) of 12.23% at 420 nm. The rates of TC degradation and Cr (VI) reduction achieved 0.059 and 0.18 min −1 , respectively. In addition, the practical application conditions and catalytic mechanism of Mnx-CN were explored. This work demonstrates the connection of the spin state of metal with the photocatalytic activity, providing an efficient photocatalytic system that can be used for solar-chemical energy conversion and pollution remediation, and presenting a new approach for modifying the g-C 3 N 4 -based catalysts.
研究领域:
材料科学
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光催化
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环境科学
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能源转换
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF MEDICINAL CHEMISTRY
·
2025
·
IF 6.8
Fei Cai,Jinrong Dong,Peng Xie,Hanlong He,Huiyi Yao,Junxian Guo,Zhibo Yan,Li Ma,Tianfeng Chen
Developing structurally well-defined targeted drugs is an effective way to enhance the chemotherapy efficacy. Herein, a target mitochondrial complex I (complex I) inhibitor was developed for the key methylation site ARG-85 in the key subunit NDUFS2. Based on the unique :NH═C– group of guanidyl and the surrounding environment of ARG-85, the macrocyclic and bulky manganese porphyrin complex [MnIII(TTPPC2–)]+ was selected to insert into the gap of NDUFS2. Experimental and computational analyses revealed that the planar π system of the TTPPC2– ligand and the rotatable benzene ring stably bind between the :NH═C– group of ARG-85 and the manganese metal center, a medium-strong Lewis acid. The Mn-specific recognition of guanidine drives the selective inhibition of complex I activity. Further, MnIII(TTPPC2–)]+ was modified into targeted nanoformulation Mn NPs. In vitro and in vivo experiments confirmed the efficient and mechanism inhibition of complex I activity, offering a novel strategy for targeted drug development.
研究领域:
生物化学
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药物化学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
Crystals
·
2019
·Vol. 9
·期 12
·657
·
IF 2.061
Jian-Chang Xiao,Qiong Wu,Yuan Lei,Jin-Rong Sun,Fang Jiang,Yan Xu,Xin-Di Xu,Tianyu Li
The design and synthesis of magnets with low dimensionality is currently an attractive research topic. The reaction of a Schiff base metal complex with simple molybdate has led to the formation of a new {MnIII-Schiff-base}-decorated molybdate heterometallic cluster, [{Mn(salpn)(H2O)}3MoO4](CH3COO)·2H2O (1) (salpn =N,N’-(1,3-propylene)bis(salicylideneiminate)). The hybrid aggregate was characterized using a range of methods including elemental analysis, single crystal x-ray diffraction, Infrared spectra (IR) spectroscopy, and x-ray structural analysis. The crystals of1are hexagonal:P63/m, a = 14.027(5) Å, c = 17.487(5) Å,V= 1142.6(3) Å3. Structural analyses indicate that we report on the preparation of the first triple metallic-oligomer held by orthomolybdate. Density functional theoretical calculation (DFT) studies have been performed to calculate electronic structure and potential energy landscapes. Additionally, the magnetic property of1indicates an antiferromagnetic coupling between the metal centers in the complex.Keywords:Schiff base;heterometallic cluster;density functional theory;magnetic behavior
研究领域:
无机化学
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材料科学
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理论化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）