Acceleration and deceleration of chirality inversion speeds in a dynamic helical metallocryptand by alkali metal ion binding
We report that the chirality inversion kinetics of a trinickel(II) cryptand can be controlled by guest recognition in the cryptand cavity. When the guest was absent, the nickel(II) cryptand underwent a dynamic interconversion between the P and M forms in solution, preferring the M form, with a half-...
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| Published in | Science advances Vol. 9; no. 44; p. eadj5536 |
|---|---|
| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Association for the Advancement of Science
03.11.2023
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| Abstract | We report that the chirality inversion kinetics of a trinickel(II) cryptand can be controlled by guest recognition in the cryptand cavity. When the guest was absent, the nickel(II) cryptand underwent a dynamic interconversion between the
P
and
M
forms in solution, preferring the
M
form, with a half-life of
t
1/2
= 4.99 min. The
P
/
M
equilibrium is reversed to
P
-favored by binding with an alkali metal ion in the cryptand cavity. The timescale of this
M→P
inversion kinetics was both notably accelerated and decelerated by the guest binding (
t
1/2
= 0.182 min for K
+
complex; 186 min for Cs
+
complex); thus, the equilibration rate constants differed by up to 1000-fold depending on the guest metal ions. This acceleration/deceleration can be explained in terms of the virtual binding constants at the transition state of the
P
/
M
chirality inversion; K
+
binding more stabilizes the transition state rather than the
P
and
M
forms to result in the acceleration.
Chirality inversion of a helical trinickel(II) cryptand was both accelerated and decelerated by alkali metal ion binding. |
|---|---|
| AbstractList | We report that the chirality inversion kinetics of a trinickel(II) cryptand can be controlled by guest recognition in the cryptand cavity. When the guest was absent, the nickel(II) cryptand underwent a dynamic interconversion between the
P
and
M
forms in solution, preferring the
M
form, with a half-life of
t
1/2
= 4.99 min. The
P
/
M
equilibrium is reversed to
P
-favored by binding with an alkali metal ion in the cryptand cavity. The timescale of this
M→P
inversion kinetics was both notably accelerated and decelerated by the guest binding (
t
1/2
= 0.182 min for K
+
complex; 186 min for Cs
+
complex); thus, the equilibration rate constants differed by up to 1000-fold depending on the guest metal ions. This acceleration/deceleration can be explained in terms of the virtual binding constants at the transition state of the
P
/
M
chirality inversion; K
+
binding more stabilizes the transition state rather than the
P
and
M
forms to result in the acceleration.
Chirality inversion of a helical trinickel(II) cryptand was both accelerated and decelerated by alkali metal ion binding. We report that the chirality inversion kinetics of a trinickel(II) cryptand can be controlled by guest recognition in the cryptand cavity. When the guest was absent, the nickel(II) cryptand underwent a dynamic interconversion between the P and M forms in solution, preferring the M form, with a half-life of t1/2 = 4.99 min. The P/M equilibrium is reversed to P-favored by binding with an alkali metal ion in the cryptand cavity. The timescale of this M→P inversion kinetics was both notably accelerated and decelerated by the guest binding (t1/2 = 0.182 min for K+ complex; 186 min for Cs+ complex); thus, the equilibration rate constants differed by up to 1000-fold depending on the guest metal ions. This acceleration/deceleration can be explained in terms of the virtual binding constants at the transition state of the P/M chirality inversion; K+ binding more stabilizes the transition state rather than the P and M forms to result in the acceleration.We report that the chirality inversion kinetics of a trinickel(II) cryptand can be controlled by guest recognition in the cryptand cavity. When the guest was absent, the nickel(II) cryptand underwent a dynamic interconversion between the P and M forms in solution, preferring the M form, with a half-life of t1/2 = 4.99 min. The P/M equilibrium is reversed to P-favored by binding with an alkali metal ion in the cryptand cavity. The timescale of this M→P inversion kinetics was both notably accelerated and decelerated by the guest binding (t1/2 = 0.182 min for K+ complex; 186 min for Cs+ complex); thus, the equilibration rate constants differed by up to 1000-fold depending on the guest metal ions. This acceleration/deceleration can be explained in terms of the virtual binding constants at the transition state of the P/M chirality inversion; K+ binding more stabilizes the transition state rather than the P and M forms to result in the acceleration. |
| Author | Ikbal, Sk Asif Akine, Shigehisa Ehara, Masahiro Zhao, Pei |
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| Title | Acceleration and deceleration of chirality inversion speeds in a dynamic helical metallocryptand by alkali metal ion binding |
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