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. 2009 Jul 20;15(29):7203-14.
doi: 10.1002/chem.200900230.

Multicomponent supramolecular systems: self-organization in coordination-driven self-assembly

Yao-Rong Zheng  1 , Hai-Bo Yang, Koushik Ghosh, Liang Zhao, Peter J Stang
Affiliations

Multicomponent supramolecular systems: self-organization in coordination-driven self-assembly

Yao-Rong Zheng et al. Chemistry. .

Abstract

The self-organization of multicomponent supramolecular systems involving a variety of two-dimensional (2 D) polygons and three-dimensional (3 D) cages is presented. Nine self-organizing systems, SS(1)-SS(9), have been studied. Each involves the simultaneous mixing of organoplatinum acceptors and pyridyl donors of varying geometry and their selective self-assembly into three to four specific 2 D (rectangular, triangular, and rhomboid) and/or 3 D (triangular prism and distorted and nondistorted trigonal bipyramidal) supramolecules. The formation of these discrete structures is characterized using NMR spectroscopy and electrospray ionization mass spectrometry (ESI-MS). In all cases, the self-organization process is directed by: 1) the geometric information encoded within the molecular subunits and 2) a thermodynamically driven dynamic self-correction process. The result is the selective self-assembly of multiple discrete products from a randomly formed complex. The influence of key experimental variables--temperature and solvent--on the self-correction process and the fidelity of the resulting self-organization systems is also described.

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Figures

Scheme 1
Scheme 1
Graphical representation of self-organization systems SS1–SS4 involving diverse coordination-driven self-assembly: small rectangle (RS), large rectangle (RL), small distorted triangular prism (DTPS), large distorted triangular prism (DTPL), and nondistorted triangular prism (NTP).
Scheme 2
Scheme 2
Graphical representation of the self-organization process in SS1 regulating randomly formed and disordered oligomeric structures into an ordered multicomponent supramolecular system of RS, RL, and DTPS.
Scheme 3
Scheme 3
Graphical representation of self-organization systems SS5–SS7 involving diverse coordination-driven self-assembly: small rhomboid (RhS), large rhomboid (RhL), small triangle (TS), large triangle (TL), and triangular bipyramid (TBP).
Scheme 4
Scheme 4
Graphical representation of self-organization systems SS8 and SS9 involving diverse coordination-driven self-assembly: small rectangle (RS), large rectangle (RL), large distorted triangular prism (DTPL), small triangle (TS), large triangle (TL), and triangular bipyramid (TBP).
Figure 1
Figure 1
31P{1H} NMR spectra (Acetone-d6/D2O 1:1) recorded at 1 h, 6 h and 24 h time intervals during the formation of supramolecular rectangles RS and RL and distorted triangular prism DTPS.
Figure 2
Figure 2
1H NMR spectra (Acetone-d6/D2O 1:1) recorded at 1 h, 6 h and 24 h time intervals during the formation of supramolecular rectangles RS and RL and distorted triangular prism DTPS.
Figure 3
Figure 3
Full ESI mass spectrum (Acetone-d6/D2O 1:1) recorded after 1 h and 24 h during the self-organization of supramolecular rectangles RS and RL and distorted triangular prism DTPS.
Figure 4
Figure 4
Equilibrated 31P{1H} NMR spectra (Acetone-d6/D2O 1:1) recorded for self-organization systems (a) SS2 (RS, DTPS, and DTPL), (b) SS3 (RS, RL, and NTP), and (c) SS4 (RS, DTPS, and NTP).
Figure 5
Figure 5
Partial 1H NMR spectra (Acetone-d6/D2O 1:1) recorded for equilibrated self-organization systems (a) SS2 (RS, DTPS, and DTPL), (b) SS3 (RS, RL, and NTP), and (c) SS4 (RS, DTPS, and NTP).
Figure 6
Figure 6
Full ESI mass spectrum (Acetone-d6/D2O 1:1) of equilibrated self-organizing systems (a) SS2 (RS, DTPS, and DTPL), (b) SS3 (RS, RL, and NTP), and (c) SS4 (RS, DTPS, and NTP).
Figure 7
Figure 7
Equilibrated 31P{1H} NMR spectra (Acetone-d6/D2O 1:1) recorded for self-organizing systems (a) SS5 (TS, RhS, and TBP), (b) SS6 (TS, RhS, and RhL), and (c) SS7 (TS, TL, and RhS).
Figure 8
Figure 8
Partial 1H NMR spectra (Acetone-d6/D2O 1:1) recorded for equilibrated self-organizing systems (a) SS5 (TS, RhS, and TBP), (b) SS6 (TS, RhS, and RhL), and (c) SS7 (TS, TL, and RhS).
Figure 9
Figure 9
Full ESI mass spectrum (Acetone-d6/D2O 1:1) of equilibrated self-organizing systems (a) SS5 (TS, RhS, and TBP), (b) SS6 (TS, RhS, and RhL), and (c) SS7 (TS, TL, and RhS).
Figure 10
Figure 10
31P{1H} (a) and Partial 1H (b) NMR spectra (Acetone-d6/D2O 1:1) recorded for equilibrated self-organizing system SS8 (RS, RL, TS, and TL).
Figure 11
Figure 11
31P{1H} (a) and Partial 1H (b) NMR spectra (Acetone-d6/D2O 1:1) recorded for equilibrated self-organizing system SS9 (RS, TS, DTPL, and TBP).
Figure 12
Figure 12
31P{1H} NMR spectra (Acetone-d6/D2O 1:1) recorded for mixtures of SS1 (RS, RL, and DTPS) heated at (a) 65–70 °C for 1 h, (b) 65–70 °C for 24 h, (c) 45–50 °C for 120 h, and (d) 25–30 °C for 20 d.
Figure 13
Figure 13
31P{1H} NMR spectra of SS1 in various solvents: (a) Acetone-d6/D2O (1:1), (b) CD2Cl2, (c) Acetone-d6/D2O (20:1), (d) Acetone-d6/D2O (1:1) after removal of CD2Cl2, and (e) Acetone-d6/D2O (1:1) after removal of Acetone-d6/D2O (20:1).
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