TY - JOUR
T1 - Multiple Transformations among Anion-based A2 nL3 nAssemblies
T2 - Bicapped Trigonal Antiprism A8L12, Tetrahedron A4L6, and Triple Helicate A2L3(A = Anion)
AU - Li, Boyang
AU - Zhang, Wenyao
AU - Lu, Shuai
AU - Zheng, Bo
AU - Zhang, Dan
AU - Li, Anyang
AU - Li, Xiaopeng
AU - Yang, Xiao Juan
AU - Wu, Biao
N1 - Publisher Copyright:
©
PY - 2020/12/16
Y1 - 2020/12/16
N2 - The construction of sophisticated, high-nuclearity polyhedral cages is an attractive yet challenging task in supramolecular chemistry. Herein we report the anion-coordination-driven assembly (ACDA) of a series of A2nL3n architectures ("A"denotes anion, L is ligand, n = 1, 2, 4) with a biphenylene-spaced bis-bis(urea) ligand including triple helicate A2L3 (H), tetrahedron A4L6 (T), and the octanuclear, bicapped trigonal antiprism (or parallelepiped) A8L12 (P). Among them, P is held by 96 hydrogen bonds, the largest number ever reported in a discrete polyhedron, and encapsulates multiple guests (three tetramethylammonium cations) in three compartments. Remarkably, multiple reversible transformations of these dynamic assemblies have been realized by alternation of the template guest, solvent, and concentration. Furthermore, a chiral ligand (L2S) with carbon stereocenters at both termini of the bis-bis(urea) backbone was designed and assembled with phosphate to form the enantio-pure triple helicate or tetrahedron. The chiral amplification effect in the tetrahedral complex is significantly larger than that in the triple helicate as a function of the point chirality.
AB - The construction of sophisticated, high-nuclearity polyhedral cages is an attractive yet challenging task in supramolecular chemistry. Herein we report the anion-coordination-driven assembly (ACDA) of a series of A2nL3n architectures ("A"denotes anion, L is ligand, n = 1, 2, 4) with a biphenylene-spaced bis-bis(urea) ligand including triple helicate A2L3 (H), tetrahedron A4L6 (T), and the octanuclear, bicapped trigonal antiprism (or parallelepiped) A8L12 (P). Among them, P is held by 96 hydrogen bonds, the largest number ever reported in a discrete polyhedron, and encapsulates multiple guests (three tetramethylammonium cations) in three compartments. Remarkably, multiple reversible transformations of these dynamic assemblies have been realized by alternation of the template guest, solvent, and concentration. Furthermore, a chiral ligand (L2S) with carbon stereocenters at both termini of the bis-bis(urea) backbone was designed and assembled with phosphate to form the enantio-pure triple helicate or tetrahedron. The chiral amplification effect in the tetrahedral complex is significantly larger than that in the triple helicate as a function of the point chirality.
UR - http://www.scopus.com/inward/record.url?scp=85097758285&partnerID=8YFLogxK
U2 - 10.1021/jacs.0c10346
DO - 10.1021/jacs.0c10346
M3 - Article
C2 - 33272016
AN - SCOPUS:85097758285
SN - 0002-7863
VL - 142
SP - 21160
EP - 21168
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 50
ER -