Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule

Kopilevich S, Müller A, Weinstock IA (2015)
Journal of the American Chemical Society 137(40): 12740-12743.

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Abstract
Using the hydrolysis of epoxides in water as a model reaction, the effect of multiple active sites on Michaelis-Menten compliant rate accelerations in a porous capsule is demonstrated. The capsule is a water-soluble 4-symmetry Keplerate-type complex of the form, [{(Mo6O21)-O-VI(H2O)(612){(Mo2O4)-O-V(L)}(30)](42-), in which 12 pentagonal "ligands," {(Mo-VI)(Mo5O2)-O-VI, (H2O)(6)}(6-), are coordinated to 30 dimolybdenum sites, {(Mo2O4L)-O-V}(1+) (L = an endohedrally coordinated 772-bound carboxylate anion), resulting in 20 MO9O9 pores. When "up-regulated" by removal of ca. one-third of the blocking ligands, L, an equal number of dimolybdenum sites are activated, and the newly freed-up space allows for encapsulation of nearly twice as many substrate guests, leading to a larger effective molarity (amplification), and an increase in the rate acceleration (k(cat)/L-uncat) from 16,000 to an enzyme-like value of 182,800.
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Kopilevich S, Müller A, Weinstock IA. Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule. Journal of the American Chemical Society. 2015;137(40):12740-12743.
Kopilevich, S., Müller, A., & Weinstock, I. A. (2015). Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule. Journal of the American Chemical Society, 137(40), 12740-12743.
Kopilevich, S., Müller, A., and Weinstock, I. A. (2015). Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule. Journal of the American Chemical Society 137, 12740-12743.
Kopilevich, S., Müller, A., & Weinstock, I.A., 2015. Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule. Journal of the American Chemical Society, 137(40), p 12740-12743.
S. Kopilevich, A. Müller, and I.A. Weinstock, “Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule”, Journal of the American Chemical Society, vol. 137, 2015, pp. 12740-12743.
Kopilevich, S., Müller, A., Weinstock, I.A.: Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule. Journal of the American Chemical Society. 137, 12740-12743 (2015).
Kopilevich, Sivii, Müller, Achim, and Weinstock, Ira A. “Amplified Rate Acceleration by Simultaneous Up-Regulation of Multiple Active Sites in an Endo-Functionalized Porous Capsule”. Journal of the American Chemical Society 137.40 (2015): 12740-12743.
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PMID: 26354143
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