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Construction of d-f heterometallic cluster with Metal-Metal Bonds

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Construction of d-f Heterometallic Cluster with Metal-Metal ...

Synthesis and Crystal Structure of (η5 EtO（O）CC5H4)RuCoMo（μ3-S）(CO)8

中国化学会第十届全国无机化学学术会议

作者： Genfeng Feng Congqing Zhu School of Chemistry and Chemical Engineering Nanjing University

heterometallic clusters are important in catalysis and small molecule activation because of the multimetallic synergistic effects from different metals. However, multimetallic species containing uranium-metal bonds remain very scarce due to the difficulties in their synthesis. Heterobidentate ligands are effective for the synthesis of complexes with supported uranium-metal bonds. Two typical examples are the phosphinoamide ligand(I) with a rigid nitrogen-phosphorus scaffold and the diphenylphosphine-substituted aryloxide ligand(II) with an oxygen-phosphorus scaffold. Significantly, Arnold and co-workers reported a novel synthetic route for a uranium-cobalt bond, which was generated by photolysis of an isocarbonyl species with a heptadentate NP scaffold(III). These ligand scaffolds, however, support only one uranium-metal bond. Recently, we report an efficient synthetic strategy to construct a series of unprecedented multimetallic bridged clusters with four or six uranium-metal bonds, employing a new heptadentate NP scaffold with three rigid nitrogen-phosphorus units(IV). In addition, the first example of f-block metal-metal triple bond(U-Rh triple bond) whose structure has been authenticated by X-ray diffraction was also synthesized and isolated. We expect that these researches may further our understanding of the bonding between uranium and transition metals, which may help to design new d-f heterometallic catalysts with uranium-metal bonds for small molecule activation and to promote the utilization of abundant depleted uranium resource.

关键词： metal-metal bond heterometallic cluster nitrogen-phosphorus ligand triple bond uranium

来源： cnki会议评论

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Chinese Journal of Structural Chemistry 2000年第1期19卷 15-18页

作者： ZHANG Yu Hua a\ WU Shu Lin a\ LI Qing Shan a\ SONG Cui Ping a YIN Yuan Qi a② \ HUANG Xiao Ying b a(State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, the Chinese Academy of Science 中科院兰州化学物理所羰基合成与选择氧化国家重点实验室甘肃兰州 730000 中科院福建物质结构所福建福州 350002

The chiral sulfido cluster ( η 5 EtO(O)CC 5H 4)RuCoMo( μ 3 S)(CO) 8 was synthesized by refluxing a solution of SRuCo 2(CO) 9 and Na〔Mo(CO) 3CpC(O)OEt〕 in tetrahydrofuran. It was characterized by elemental analysis, IR and 1H NMR. Crystal data: C 16 H 9O 10 CoMoRuS, M r =649.24, monoclinic, space group P2 1/n, a = 10.075(1), b = 9.034(2), c = 22.973(7), β= 92.70(1), V = 2088.7(8) 3, Z = 4, D c = 2.064g·cm -3 , μ (Mo Kα ) = 22.07 cm -1 , F(000) = 1256, T = 296K, final R = 0.030, R w = 0.042 for 3686 observed reflections with I>2\^00σ(I) . The crystal structure determination shows that the cluster has a chiral tetrahedral core containing a ethoxycarbonyl attached to the cyclopentadienyl.\;

关键词： synthesis crystal structure tetrahedral framework heterometallic cluster

Structural Characterization of Chiral Sulfido cluster(η~5-C_5H_5) WFeCo(CO)_8 (μ_3-S)

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Chinese Journal of Structural Chemistry 1997年第1期16卷 59-63页

作者： Xu, Feng Sun, Wen-Hua Yang, Shi-Yan Yin, Yuan-Qi Wu, Qiang-Jin State Key Lab. OXO Synthesis/S. O. Lanzhou Inst. of Chemical Physics Chinese Academy of Sciences Lanzhou 730000 China Fujian Inst. Res. Struct. of Matter Chinese Academy of Sciences Fuzhou 350002 China

The chiral sulfido cluster (η5-C5H5)WFeCo(CO)8(μ3--S) was synthesized by refluxing a solution of HFe2Co(CO)9 (μ3,--S) and (η5-C5H5)Fe(CO)3Cl in tetrahydrofuran. It was characterized by elemental analysis, IR and 1H/13C--NMR. Theproposal concerning mechanism was discussed herewith and the structure was reportedas well. Crystallographic data: Mr= 563. 85, monoclinicl P21/n(# 14); a= 8. 009(2), b= 17. 600(5), c=12. 003(4) A; β=95. 91(2)°; V= 1683. 0 (9) A3; Z=4;Dc=2. 22 g. cm-3; F(000) = 1048, μ=89. 27 cm-1 ; final R=0. 039 and Rw=0. 049for 2121 observable reflections with (I≥3. cσ(I) ). The crystal structure determinationshows that S atom coordinates to all three metal (W,Fe,Co) atoms in a μ3,-fashion,thetitle cluster core has the tetrahedral skeleton.

关键词： heterometallic cluster carbonyl sulfido tetrahedral framework

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Odd-membered cyclic hetero-polyoxotitanate nanoclusters with high stability and photocatalytic H_(2) evolution activity

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Chinese Journal of Catalysis 2021年第8期42卷 1332-1337页

作者： Ya-Jie Liu Lin Geng Yao Kang Wei-Hui Fang Jian Zhang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina University of Chinese Academy of Sciences Beijing 100049China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007FujianChina

We investigated the hydrolysis of TiⅣ along with naturally abundant AlⅢ ions and reported the formation of a stable and semiconducting nanocluster. Interestingly, this compound exhibits an unusual odd-membered ring structure and also represents the largest Al-containing polyoxotitanium cluster(PTC) observed thus far. The presence of a shell of organic ligands as well as the incorporation of hetero-AlⅢ ions endowed the nanocluster with high air, thermal, and pH stabilities. The present compound exhibited a record photocatalytic hydrogen evolution of 402.88 μmol g–1 h–1 among PTC materials. This work not only paves the way towards stable PTC materials but also provides new insights into the design of novel photocatalysts.

关键词： Polyoxotitanate heterometallic cluster Nanocluster Water-splitting H2 production

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