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Spontaneous resolution and absolute chiral induction of 3d-4f heterometal-organic frameworks from achiral precursors

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Science China Chemistry 2021年第10期64卷 1698-1702页

作者： Manting Chen Zuochang Chen Huijun Chen Lu Xu Xiangjian Kong Lasheng Long Lansun Zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid SurfacesDepartment of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

The asymmetric assembly and spontaneous resolution of chiral heterometal-organic frameworks from achiral precursors remain a great challenge. Herein, we report the formation and spontaneous resolution of three-dimensional(3 D) chiral 3 d-4 f heterometal-organic frameworks from achiral ligands in the presence of lactic acid enantiomers as chiral inducers. In the absence of a chiral inducer, the reactants randomly generated both enantiopure crystals in equal measure. However, enantiopure lactic acid induced asymmetric resolution to achieve single chiral crystallization. DFT theoretical calculations showed that the absolute chiral resolution of the enantiomers is due to the difference in the interactions between the two enantiomeric Λ/Δ-[Fe L_(3)]^(3-)units and the chiral inducer.

关键词： chirality spontaneous resolution chirality induction heterometal-organic framework achiral precursors

Lanthanide-oxo clusters for efficient catalytic reduction of carboxamides

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Science China Chemistry 2023年第2期66卷 443-448页

作者： Zhen-Zhang Weng Chao-Long Chen Long-Wu Ye La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

The reduction of carboxamides into high value-added amines is a very interesting but great challenging *** we demonstrate that polynuclear lanthanide-oxo clusters Ln16(Ln=Eu and Gd)can be used as efficient catalyst to reduce primary and secondary carboxamides to amines with excellent yield of 71%-98%and broad substrates *** methodology can extend to the gram-scale synthesis of phenethylamine drug with 93%*** on the isolation and characterization of catalytic intermediates,a catalytic mechanism involving multipath reaction is *** work provides efficient lanthanide cluster catalysts for the reduction of carboxamides to amines.

关键词： lanthanide clusters amide reduction metal-hydride BH3 catalytic mechanism

Integration of bio-inspired lanthanide-transition metal cluster and P-doped carbon nitride for efficient photocatalytic overall water splitting

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National Science Review 2021年第9期8卷 41-49页

作者： Rong Chen Gui-Lin Zhuang Zhi-Ye Wang Yi-Jing Gao Zhe Li Cheng Wang Yang Zhou Ming-Hao Du Suyuan Zeng La-Sheng Long Xiang-Jian Kong Lan-Sun Zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University College of Chemical Engineering Zhejiang University of Technology College of Chemistry and Chemical Engineering Liaocheng University

Photosynthesis in nature uses the Mn4CaO5cluster as the oxygen-evolving center to catalyze the water oxidation efficiently in photosystem II. Herein, we demonstrate bio-inspired heterometallic Ln Co3(Ln=Nd, Eu and Ce) clusters, which can be viewed as synthetic analogs of the Ca *** Ln Co3on phosphorus-doped graphitic carbon nitrides (PCN) shows efficient overall water splitting without any sacrificial reagents. The Nd Co3/PCN-c photocatalyst exhibits excellent water splitting activity and a quantum efficiency of 2.0%at 350 nm. Ultrafast transient absorption spectroscopy revealed the transfer of a photoexcited electron and hole into the PCN and Ln Co3for hydrogen and oxygen evolution reactions, respectively. A density functional theory (DFT) calculation showed the cooperative water activation on lanthanide and O-O bond formation on transition metal for water oxidation. This work not only prepares a synthetic model of a bio-inspired oxygen-evolving center but also provides an effective strategy to realize light-driven overall water splitting.

关键词： bio-inspired lanthanide-transition metal cluster photocatalytic overall water splitting synergistic effects oxygen-evolving center

Synthesis,structures and photoluminescence of uranyl polyoxometalate clusters based on trilacunary[TeW_(9)O_(33)]^(8-)

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Tungsten 2023年第2期5卷 254-260页

作者： Hai-Ying Wang Xiu-Ying Zheng La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Henan Key Laboratory of Polyoxometalate Chemistry College of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004China Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China

Synthesis of uranyl polyoxometalate clusters attract more attention but remain great ***,two uranyl polyoxometalate inorganic clusters of{Na_(6)(NH_(4))_(19)[(TeW_(9)O_(33))_(4)[TeO_(2)(OH)](UO_(2))4(H_(2)O)_(2)]·50H_(2)O}n(1,Te-U_(4))and(NH_(4))18{Na@[(TeW_(9)O_(32)OH)(TeW_(9)O_(33))_(2)[TeO(OH)][W_(3)O_(12)(μ_(3)-OH)](UO_(2))_(6)(μ_(2)-OH)_(2)H_(2)O]}·75H_(2)O(2,Te-U6)were prepared using trilacunary[α-B-TeW_(9)O_(33)]8-as inorganic *** analysis showed that compound 1 is a one-dimensional chain structure formed by tetrameric aggregates of[(α-B-TeW_(9)O_(33))_(4)(TeO_(2)(OH))(UO_(2))_(4)(H_(2)O)2]25-as nodes and Na+ions as *** anionic tetrameric aggregates in 1 is made of two sandwich-type dimers of[(TeW_(9)O_(33))_(2)(UO_(2))_(2)H_(2)O]12-bridged by a[TeO_(2)(OH)]-*** 2 is a triangular trimeric architecture templated by Na+*** solid-state luminescence emission spectra of compounds 1 and 2 show the characteristic peaks of uranyl *** 1 with one-dimensional chain structure exhibited a higher photoluminescence quantum yields(PLQY)than that of 2,due to the more rigidity of 1 reducing the nonradiative transitions.

关键词： Uranyl Polyoxometalate Cluster Lacunary Luminescence

Anchoring heterometallic cluster on P-doped carbon nitride for efficient photocatalytic nitrogen fixation in water and air ambient

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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： Chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng Xiang-Jian Kong Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

Encapsulating a Ni（Ⅱ） molecular catalyst in photoactive metal–organic framework for highly efficient photoreduction of CO2

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Science Bulletin 2019年第14期64卷 976-985页

作者： Zhi-Hao Yan Bo Ma Shu-Rong Li Junxue Liu Rong Chen Ming-Hao Du Shengye Jin Gui-Lin Zhuang La-Sheng Long Xiang-Jian Kong Lan-Sun Zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surface and Department of Chemistry College of Chemistry and Chemical Engineering Xiamen University Xiamen 361005 China State Key Laboratory of Molecular Reaction Dynamics and Collaborative Innovation Center of Chemistry for Energy Materials Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China College of Chemical Engineering Zhejiang University of Technology Hangzhou 310032 China

Photocatalytic reduction of CO2 to CO is a promising strategy for reducing atmospheric CO2 levels and storing solar radiation as chemical ***,we demonstrate that a molecular catalyst[NiⅡ(bpet)(H2O)2]successfully encapsulated into a highly robust and visible-light responsive metal–organic framework(Ru-UiO-67)to fabricate composite catalysts for photocatalytic CO2 *** composite Ni@Ru-UiO-67 photocatalysts show efficient visible-light-driven CO2 reduction to CO with a TON of 581 and a selectivity of 99% after 20-h illumination,because of the facile electron transfer from Ru-photosensitizer to Ni(Ⅱ)active sites in Ni@Ru-UiO-67 *** mechanistic insights into photoreduction of CO2 have been studied based on thermodynamical,electrochemical,and spectroscopic investigation,together with density functional theory(DFT)*** work shows that encapsulating molecular catalyst into photoactive MOF highlights opportunities for designing efficient,stable and recyclable photocatalysts.

关键词： Metal-organic frameworks CO2 reduction Transient absorption Photocatalysis DFT calculations

Enhanced proton conductivity of Mo_(154)-based porous inorganic framework

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Science China Chemistry 2021年第6期64卷 959-963页

作者： Hai-Ying Wang Shu-Rong Li Xing Wang La-Sheng Long Xiang-Jian Kong Lan-Sun Zheng Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid SurfacesDepartment of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

The construction of inorganic porous frameworks from discrete polyoxometalate(POM)units is a major research ***,a three-dimensional(3D)all-inorganic porous structure{Mo_(154)}_n that consists of classic Mo_(154)rings connected by Mo–O–Mo covalent bonds was ***,the proton conductivity of the 3D-{Mo_(154)}_n framework is 1.1×10^(-2)S cm^(-1)at 22℃and 100%relative humidity(RH),which is one of the highest proton conductivities reported thus far for POM-based conductive *** to the discrete{Mo_(154)}cluster and 1D-{Mo_(154)}_n,the enhanced conductivity of 3D-{Mo_(154)}_n suggests that assembling POM-based all-inorganic porous frameworks is a promising method for designing proton-conductive materials.

关键词： polyoxomolybdate proton conductor three-dimensional structure self-assembly cluster

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稀土-钛氧簇合物的研究进展

高等学校化学学报 2020年第12期41卷 2577-2586页

作者：李观俊龙腊生孔祥建郑兰荪厦门大学化学化工学院化学系固体表面物理化学国家重点实验室能源材料化学协同创新中心厦门361005

稀土-钛氧簇合物作为团簇化学的一个新分支,不但结合了稀土和钛离子的特性,而且由于二者的协同效应而表现出优异的光、电、磁和催化性能.本文综合评述了不同配体稀土-钛氧簇合物的合成与结构,介绍了稀土-钛氧簇合物的代表性成果,并对其... 详细信息

稀土-钛氧簇合物作为团簇化学的一个新分支,不但结合了稀土和钛离子的特性,而且由于二者的协同效应而表现出优异的光、电、磁和催化性能.本文综合评述了不同配体稀土-钛氧簇合物的合成与结构,介绍了稀土-钛氧簇合物的代表性成果,并对其合成策略和发展前景进行了总结和展望.

关键词：稀土-钛氧簇合物合成结构荧光光催化

稀土-钛氧簇合物EuTi6,EuTi7和La2Ti14的可控合成

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物理化学学报 2020年第9期36卷 124-129页

作者：杨亚梅伦会洁龙腊生孔祥建郑兰荪厦门大学化学化工学院化学系固体表面物理化学国家重点实验室能源材料化学协同创新中心福建厦门361005

相比于纳米材料,原子精度的金属簇合物具有精确的表面结构和晶体结构,更有利于在原子水平上去理解化学反应的活性与结构的关系。作为团簇的一个有趣的分支,异金属的稀土-钛氧簇合物因其有趣的化学性质引起了人们的广泛关注。但是稀土-... 详细信息

相比于纳米材料,原子精度的金属簇合物具有精确的表面结构和晶体结构,更有利于在原子水平上去理解化学反应的活性与结构的关系。作为团簇的一个有趣的分支,异金属的稀土-钛氧簇合物因其有趣的化学性质引起了人们的广泛关注。但是稀土-钛氧簇合物的精准合成是目前的重要挑战,这阻碍了其性能的进一步研究。因为螯合配体可以降低Ti4+的水解速度,因此选择合适的螯合配体是制备稀土钛氧团簇的有效方法。最近,我们以螯合作用较强的3,5-二叔丁基水杨酸(H2dtbsa)为配体,稀土盐和Ti(OiPr)4为原料,通过溶剂热法成功合成了四个新的稀土-钛氧簇合物[EuTi6(μ3-O)3(OC2H5)8(dtbsa)6(Hdtbsa)]·(C2H5OH)(1),[EuTi7(μ3-O)3(μ2-OH)2(OiPr)9(dtbsa)6(Hdtbsa)Cl]·(HOiPr)3(2),[EuTi7(μ3-O)3(μ2-OH)2(OiPr)8(dtbsa)7(Hdtbsa)]·(HOiPr)2(3)和[LaTi7(μ3-O)3(μ2-OH)2(OC2H5)8(dtbsa)7(Hdtbsa)]2·(C2H5OH)4(4)。单晶分析表明,七核化合物1内核EuTi6具有三角棱柱的结构,其中Eu3+位于六个Ti4+离子形成的棱柱中心。八核化合物2和3的金属内核结构可以看作是化合物1中三棱柱的一侧连接一个Ti4+。化合物4中,Ln2Ti14的金属骨架可看作是EuTi7的二聚体。紫外-可见漫反射光谱估算的带隙值表明,簇合物1、2和3的禁带宽度值分别为2.35、2.07和2.16 eV,明显小于锐钛矿的禁带宽度值。光电响应测试发现这三种簇合物具有明显的光电响应,而且簇合物1和2的电荷分离效应好于簇合物3。为了探索这类簇合物在光催化方面的应用,我们做了在甲醇水溶液中的光催化(300–800 nm)分解水产氢实验。簇合物1、2和3的产氢率分别为112、106和87μmol?h-1?g-1,高于商用P25。粉末X射线衍射(PXRD)和热重分析(TGA)证明了簇合物的光热稳定性。本文不但提供了一种制备稀土钛氧簇合物的螯合配体策略,而且还表明稀土钛氧簇合物具有较低的带隙和光驱动的催化活性。

关键词：稀土-钛氧簇合物精确结构溶剂热法产氢光解水