Discovery of a Neutral 40-PdII-Oxo Molecular Disk, [Pd40O24(OH)16{(CH3)2AsO2}16]: Synthesis, Structural Characterization, and Catalytic Studies

Bhattacharya, Saurav; Ma, Xiang; Mougharbel, Ali S.; Haouas, Mohamed; Su, Pei; Espenship, Michael F.; Taffa, Dereje H.; Jaensch, Helge; Bons, Anton‐Jan; Stuerzer, Tobias; Wark, Michael; Laskin, Julia; Cadot, Emmanuel; Kortz, Ulrich

doi:10.1021/acs.inorgchem.1c02749

Cited by 17 publications

(9 citation statements)

References 83 publications

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“…The catalytic activity of 1 supported on modified SBA-15 ( 1-apts-SBA15 ) was investigated for the hydrogenation of o -xylene yielding cis -1,2-dimethylcyclohexane and trans -1,2-dimethylcyclohexane using a PID-Effi fixed-bed reactor, where SBA-15 is a highly robust mesoporous silica having uniform hexagonal pores with tunable pore sizes . The detailed procedures for the preparation of the supported precatalyst 1-apts-SBA15 and the catalyst bed are described in the Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

Discovery of Polythioplatinate(II) [Pt₃S₂(SO₃)₆]^10– and Study of Its Solution and Catalytic Properties

et al. 2022

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We have discovered the first polythioplatinate(II), [PtII 3S2(SO3)6]10– (1), which was synthesized in aqueous basic medium (pH 11) by hydrothermal heating at 150 °C. Polyanion 1 comprises a discrete, triangular assembly of three Pt2+ ions linked by two μ3-sulfido ligands, and their square-planar coordination geometry is completed by two terminal S-bound sulfito ligands. Polyanion 1 was isolated as a hydrated sodium salt, Na10[PtII 3(μ3-S)2(SO3)6]·22H2O (Na-1), which was characterized in the solid state by single-crystal X-ray diffraction, Fourier-transform infrared spectroscopy, thermogravimetric analysis, X-ray photoelectron spectra, and elemental analysis, in solution by 195Pt NMR and atomic absorption spectroscopy, and in the gas phase by electrospray ionization mass spectrometry. Density functional theory calculations were performed, and the 195Pt NMR chemical shifts of 1 were computed theoretically and shown to match well with the experimental data. Furthermore, the discrete title polyanion 1 was immobilized on mesoporous SBA-15 support and used as a precatalyst for the hydrogenation of o-xylene.

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Section: Resultsmentioning

confidence: 99%

Discovery of Polythioplatinate(II) [Pt₃S₂(SO₃)₆]^10– and Study of Its Solution and Catalytic Properties

et al. 2022

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“…The first polyoxopalladate(II) (POPd), [H 6 Pd II 13 O 8 (AsO 4 ) 8 ] 8– , and the first polyoxoaurate(III) (POAu), [Au III 4 O 4 (AsO 4 ) 4 ] 8– , were discovered by Kortz and co-workers in 2008 and 2010, respectively, which eventually led to the discovery of a large family of POPds with different shapes, sizes, and compositions . Recently, the first neutral palladium(II)-oxo clusters (POCs) were reported by Kortz and co-workers, such as the disk-shaped [Pd 16 O 8 (OH) 8 ((CH 3 ) 2 AsO 2 ) 8 ] (Pd 16 ) and its chloro-derivative [Pd 16 O 8 (OH) 5 Cl 3 ((CH 3 ) 2 AsO 2 ) 8 ] (Pd 16 Cl), the larger, bicapped derivative [Pd 24 O 12 (OH) 8 ((CH 3 ) 2 AsO 2 ) 16 ] (Pd 24 ), and the even larger [Pd 40 O 24 (OH) 16 ((CH 3 ) 2 AsO 2 ) 16 ] (Pd 40 ) . Even more recently, Kortz and co-workers discovered the first two examples of cationic POCs containing f -metal ions, [Pd II 6 O 12 M 8 {(CH 3 ) 2 AsO 2 } 16 (H 2 O) 8 ] 4+ (M = Ce IV , Th IV ) .…”

Section: Introductionmentioning

confidence: 99%

Pt^IV-Containing Hexaplatinate(II) [Pt^IVPt^II₆O₆(AsO₂(CH₃)₂)₆]^2– and Hexapalladate(II) [Pt^IVPd^II₆O₆(AsO₂(CH₃)₂)₆]^2–

Zhang,

Bhattacharya,

Khsara

et al. 2023

Inorg. Chem.

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The first PtIV-containing discrete polyoxoplatinate(II) [PtIVPtII 6O6(AsO2(CH3)2)6]2– (Pt 7 ) and polyoxopalladate(II) [PtIVPdII 6O6(AsO2(CH3)2)6]2– (PtPd 6 ) have been prepared and characterized in the solid state, in solution, and in the gas phase. The molecular structures of the noble metal-oxo clusters Pt 7 and PtPd 6 comprise a central, octahedral PtIVO6 hetero group surrounded by six square-planar MO4 (M = PtII, PdII) units, which are capped by six dimethylarsinate ligands. The polyanions were prepared under simple one-pot aqueous solution conditions by reacting H2Pt(OH)6 with either K2PtCl4 or Pd(NO3)2 in sodium dimethylarsinate buffer (pH 7) at 80 °C. Catalytic studies were performed on Pt 7 supported on SBA15-apts for o-xylene hydrogenation at 300 °C and 90 bar H2 pressure and indicated excellent activity and recyclability with low activation temperature.

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“…This field is currently dominated by platinum − and ruthenium − containing complexes. The polyoxopalladates, discovered and developed by the Kortz group, are also in focus. − Recently, Na 5 [H 3 Pt IV W 6 O 24 ] and Na 3 K 5 [Pt 2 II (W 5 O 18 ) 2 ] were reported to have high hydrogen evolution reaction (HER) performance, and in situ XAS experiments and DFT calculations suggest the Pt–O bond to be the active site . The Pt–O junction facilitates electron–proton coupling and leads to the rapid release of H 2 .…”

Section: Introductionmentioning

confidence: 99%

Coordination of Pt(IV) by {P₈W₄₈} Macrocyclic Inorganic Cavitand: Structural, Solution, and Electrochemical Studies

et al. 2022

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Hydrothermal reaction of a macrocyclic inorganic POM cavitand Li17(NH4)21H2[P8W48O184] with [Pt(H2O)2(OH)4] results in coordination of up to six {Pt(H2O) x (OH)4–x } fragments to the internal surface of the polyoxoanion. The product was isolated as K22(NH4)9H3[{Pt(OH)3(H2O)}6P8W48O184]·79H2O (1) and characterized by multiple techniques in the solid state (SCXRD, XRPD, XPS, FTIR, and TGA) and in solution (NMR, ESI-MS, and HPLC-ICP-AES). Electrochemical properties were studied both in solution and as components of the paste electrode. The complex shows electrocatalytic activity in water oxidation.

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Discovery of a Neutral 40-Pd^II-Oxo Molecular Disk, [Pd₄₀O₂₄(OH)₁₆{(CH₃)₂AsO₂}₁₆]: Synthesis, Structural Characterization, and Catalytic Studies

Cited by 17 publications

References 83 publications

Discovery of Polythioplatinate(II) [Pt₃S₂(SO₃)₆]^10– and Study of Its Solution and Catalytic Properties

Discovery of Polythioplatinate(II) [Pt₃S₂(SO₃)₆]^10– and Study of Its Solution and Catalytic Properties

Pt^IV-Containing Hexaplatinate(II) [Pt^IVPt^II₆O₆(AsO₂(CH₃)₂)₆]^2– and Hexapalladate(II) [Pt^IVPd^II₆O₆(AsO₂(CH₃)₂)₆]^2–

Coordination of Pt(IV) by {P₈W₄₈} Macrocyclic Inorganic Cavitand: Structural, Solution, and Electrochemical Studies

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Discovery of a Neutral 40-PdII-Oxo Molecular Disk, [Pd40O24(OH)16{(CH3)2AsO2}16]: Synthesis, Structural Characterization, and Catalytic Studies

Cited by 17 publications

References 83 publications

Discovery of Polythioplatinate(II) [Pt3S2(SO3)6]10– and Study of Its Solution and Catalytic Properties

Discovery of Polythioplatinate(II) [Pt3S2(SO3)6]10– and Study of Its Solution and Catalytic Properties

PtIV-Containing Hexaplatinate(II) [PtIVPtII6O6(AsO2(CH3)2)6]2– and Hexapalladate(II) [PtIVPdII6O6(AsO2(CH3)2)6]2–

Coordination of Pt(IV) by {P8W48} Macrocyclic Inorganic Cavitand: Structural, Solution, and Electrochemical Studies

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Discovery of a Neutral 40-Pd^II-Oxo Molecular Disk, [Pd₄₀O₂₄(OH)₁₆{(CH₃)₂AsO₂}₁₆]: Synthesis, Structural Characterization, and Catalytic Studies

Discovery of Polythioplatinate(II) [Pt₃S₂(SO₃)₆]^10– and Study of Its Solution and Catalytic Properties

Discovery of Polythioplatinate(II) [Pt₃S₂(SO₃)₆]^10– and Study of Its Solution and Catalytic Properties

Pt^IV-Containing Hexaplatinate(II) [Pt^IVPt^II₆O₆(AsO₂(CH₃)₂)₆]^2– and Hexapalladate(II) [Pt^IVPd^II₆O₆(AsO₂(CH₃)₂)₆]^2–

Coordination of Pt(IV) by {P₈W₄₈} Macrocyclic Inorganic Cavitand: Structural, Solution, and Electrochemical Studies