Stepwise Assembly of Pd6(RuL3)8 Nanoscale Rhombododecahedral Metal–Organic Cages via Metalloligand Strategy for Guest Trapping and Protection

Li, Kang; Zhang, Luyin; Cheng, Yan; Wei, Shichao; Pan, Mei; Zhang, Li; Su, Cheng‐Yong

doi:10.1021/ja410044r

Cited by 312 publications

(196 citation statements)

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“…1) can be readily obtained from an one-pot reaction of the predesigned redox- and photoactive RuL 3 metalloligands (L=2-(pyridin-3-yl)-1H-imidazo[4,5-f][1,10]-phenanthroline) and Pd 2+ ions as previously reported (Supplementary Note 1)3839, showing the shape of octahedron with six Pd 2+ atoms on the vertices and eight Ru 2+ atoms on the facets. The ligand L consists of a phenanthroline (Phen) part and an benzimidazole-pyridine (BIm–Py) part, playing the dual role of bridging and peripheral ligands in normal one-component bimetallic PMDs.…”

Section: Resultsmentioning

confidence: 79%

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A metal-organic cage incorporating multiple light harvesting and catalytic centres for photochemical hydrogen production

Chen¹,

et al. 2016

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Photocatalytic water splitting is a natural but challenging chemical way of harnessing renewable solar power to generate clean hydrogen energy. Here we report a potential hydrogen-evolving photochemical molecular device based on a self-assembled ruthenium–palladium heterometallic coordination cage, incorporating multiple photo- and catalytic metal centres. The photophysical properties are investigated by absorption/emission spectroscopy, electrochemical measurements and preliminary DFT calculations and the stepwise electron transfer processes from ruthenium-photocentres to catalytic palladium-centres is probed by ultrafast transient absorption spectroscopy. The photocatalytic hydrogen production assessments reveal an initial reaction rate of 380 μmol h−1 and a turnover number of 635 after 48 h. The efficient hydrogen production may derive from the directional electron transfers through multiple channels owing to proper organization of the photo- and catalytic multi-units within the octahedral cage, which may open a new door to design photochemical molecular devices with well-organized metallosupramolecules for homogenous photocatalytic applications.

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Section: Resultsmentioning

confidence: 79%

“…Herein we present a PMD model based on a self-assembled Ru 8 –Pd 6 MOC3839, in which eight Ru 2+ -photocentres and six catalytically active Pd 2+ -centres are organized in a highly ordered octahedral manner to provide multiple but independent energy transfer and electron collection pathways (Fig. 1).…”

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confidence: 99%

A metal-organic cage incorporating multiple light harvesting and catalytic centres for photochemical hydrogen production

Chen¹,

et al. 2016

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“…The P5O groups of the eight ligands point inward to the center of the cage, which provides a hydrophilic environment inside the cavity (Figure 14a,b) (Figure 14c,d) (Figure 15a). [48] This metallocage has a rhombododecahedral shape and contains a 5350 Å 3 cavity and twelve open windows, facilitating effective trapping of guest molecules (Figure 15b). Both nonpolar phen and polar DMPA molecules could be encapsulated in the cavity (Figure 15c), and the protection of photosensitive guests against UV radiation was also studied.…”

Section: P E R S O N a L A C C O U N T T H E C H E M I C A L R E C O R Dmentioning

confidence: 99%

“…[51] As shown in Figure 19a, The maximum phen guest uptake inside and in the doorway of the cage. [48] Copyright V C 2014, American Chemical Society. (Figure 19b).…”

Section: Construction Of M 6 L 4 Metallocages Based On Flexible Tripomentioning

confidence: 99%

Controllable Coordination Self‐Assembly Based on Flexible Tripodal Ligands: From Finite Metallocages to Infinite Polycatenanes Step by Step

Chen

Jiang

et al. 2015

The Chemical Record

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This article describes the developments in coordination self-assembly based on flexible tripodal ligands with different metal species. Various finite metallocages such as M3 L2 , M6 L8 , M6 L4 , M4 L4 and different catenanes based on discrete metallocages constructed from flexible tripodal ligands with suitable metal species are presented here. Many M3 L2 metallocages based on ligands L(1) -L(12) and different two-coordinated metal species have been prepared, in which various Ag(I) salts and other metal species that have been protected by suitable groups, such as Zn(OAc)2 , ZnBr2 , and PdBr2 , have been used as effective acceptors. All of the M6 L8 -type metallocages are constructed from ligands L(2) or L(12) -L(20) and different four-coordinated metal species, such as various palladium(II) salts or NiCl2 , and have similar topological structures. Only a few discrete M6 L4 -type metallocages, based on ligands L(21) -L(24) , have been reported, using different strategies such as protecting groups and steric hindrance. All of the M4 L4 -type cages have similar topological structures and are constructed from ligands L(25) -L(29) with multiple donor sites. More intriguing interlocking ensembles constructed from discrete metallocages are also described here in detail, namely, three [2]catenanes based on ligands L(30) -L(32) and four polycatenanes based on ligands L(33) -L(34) .

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“…Most of these polyhedra are highly symmetric and achiral202122232425, and chiral molecular polyhedra with lower symmetry have attracted more and more attention because they increase the complexity of motifs and may bring more sophisticated functions262728293031. Generally, the construction of chiral molecular polyhedra follows two strategies: to use predetermined 3D chiral building blocks as the edges3032, vertices3334 or faces3536 of polyhedra to transfer 3D chirality of the components to the 3D chirality of the chiral structures, or to use achiral components to generate chiral metal-organic polyhedra373839404142 during a self-assembly process.…”

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confidence: 99%

Assembled molecular face-rotating polyhedra to transfer chirality from two to three dimensions

Wang

Yang

et al. 2016

Nat Commun

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In nature, protein subunits on the capsids of many icosahedral viruses form rotational patterns, and mathematicians also incorporate asymmetric patterns into faces of polyhedra. Chemists have constructed molecular polyhedra with vacant or highly symmetric faces, but very little is known about constructing polyhedra with asymmetric faces. Here we report a strategy to embellish a C3h truxene unit with rotational patterns into the faces of an octahedron, forming chiral octahedra that exhibit the largest molar ellipticity ever reported, to the best of our knowledge. The directionalities of the facial rotations can be controlled by vertices to achieve identical rotational directionality on each face, resembling the homo-directionality of virus capsids. Investigations of the kinetics and mechanism reveal that non-covalent interaction among the faces is essential to the facial homo-directionality.

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Stepwise Assembly of Pd₆(RuL₃)₈ Nanoscale Rhombododecahedral Metal–Organic Cages via Metalloligand Strategy for Guest Trapping and Protection

Cited by 312 publications

References 46 publications

A metal-organic cage incorporating multiple light harvesting and catalytic centres for photochemical hydrogen production

A metal-organic cage incorporating multiple light harvesting and catalytic centres for photochemical hydrogen production

Controllable Coordination Self‐Assembly Based on Flexible Tripodal Ligands: From Finite Metallocages to Infinite Polycatenanes Step by Step

Assembled molecular face-rotating polyhedra to transfer chirality from two to three dimensions

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