Host-Guest Chemistry in Discrete Polyoxo-12-Palladate(II) Cubes [MO8Pd12L8]n- (M = ScIII, CoII, CuII, L = AsO43 -; M = CdII, HgII, L = PhAsO32-): Structure, Magnetism, and Catalytic Hydrogenation.
Host-Guest Chemistry in Discrete Polyoxo-12-Palladate(II) Cubes [MO8Pd12L8]n- (M = ScIII, CoII, CuII, L = AsO43 -; M = CdII, HgII, L = PhAsO32-): Structure, Magnetism, and Catalytic Hydrogenation.
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DOI：
10.1021/acs.inorgchem.2c02751
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发表时间：
2022-11
影响因子：
4.6
通讯作者：
Peng Yang;M. E. Mahmoud;Yixian Xiang;Zhengguo Lin;Xiang Ma;J. Christian;J. K. Bindra;Jared S Kinyon-Ja
中科院分区：
文献类型：
--
作者：
Peng Yang;M. E. Mahmoud;Yixian Xiang;Zhengguo Lin;Xiang Ma;J. Christian;J. K. Bindra;Jared S Kinyon-Ja
在长方体12-钯-氧代笼[MO 8 Pd 12 L 8]n-内包含不同金属离子的五个主-客体组装体的家族，（Mpd12L8，M = ScIII，CoII，CuII，L = AsO 43-; M = Cd Ⅱ，Hg Ⅱ，L = PhAsO_（32-），并通过单晶X射线衍射（XRD），傅里叶变换红外光谱（FT-IR），和热重分析，并通过多核NMR光谱和电喷雾电离质谱（ESI-MS）验证了它们的溶液和气相稳定性。多钯酸盐（POP）ScPd 12 As 8、CoPd 12 As 8和CuPd 12 As 8代表了Mpd 12 As 8原型的前三个例子。{MO 8}独特的立方配体场允许使用45 Sc和113 Cd NMR技术收集溶液中持久性有机污染物的形态分布。详细的磁和电子顺磁共振（EPR）的研究进行了CuPd 12 As 8。对SBA-15负载的MPd_（12）As_8（M = Cu Ⅱ和Co Ⅱ）的催化研究揭示了客体金属依赖的结构-功能关系，CuPd_（12）As_8是固定床反应器中邻二甲苯加氢转化的更有效的预催化剂。
A family of five host-guest assemblies comprising different metal ions inside a cuboid 12-palladium-oxo cage, [MO8Pd12L8]n- (MPd12L8, M = ScIII, CoII, CuII, L = AsO43-; M = CdII, HgII, L = PhAsO32-), was synthesized and structurally characterized in the solid state by single-crystal X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and thermogravimetric analysis, and their solution and gas-phase stability were validated by multinuclear NMR spectroscopy and electrospray-ionization mass spectrometry (ESI-MS). The polyoxopalladates (POPs) ScPd12As8, CoPd12As8, and CuPd12As8 represent the first three examples of the MPd12As8 archetype. The unique cubic ligand field of {MO8} allows for collecting the speciation profiles of the POPs in solution using 45Sc and 113Cd NMR techniques. Detailed magnetic and electron paramagnetic resonance (EPR) studies were performed on CuPd12As8. Catalytic studies on MPd12As8 (M = CuII and CoII) supported on SBA-15 unveiled a guest metal-dependent structure-function relationship, with CuPd12As8 being the more efficient precatalyst for the hydroconversion of o-xylene in a fixed-bed reactor.