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Dynamics with Explicit Solvation Reveals Formation of the Prereactive Dimer as Sole Determining Factor for the Efficiency of Ru(bda)L-2 Catalysts
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Theoretical Chemistry and Biology.ORCID iD: 0000-0002-1553-4027
2018 (English)In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 8, no 9, p. 8642-8648Article in journal (Refereed) Published
Abstract [en]

This report describes all key steps in the O-O bond formation from two separated [Ru-V=O(bda)L-2](+) cations to form the dinuclear [(bda)L2RuIV-O-Ru-IV(bda)L-2](2+) in explicit solvent. The three steps involve the diffusion of the catalysts in the water phase, formation of the prereactive dimer, and the bond formation between the two catalysts. On the basis of the calculated parameters, we compute the rate constant of two catalysts with different L-ligands, isoquinoline and picoline, and the computed values are in excellent agreement with the experimental ones. The interaction of the axial ligands is key to the improved rates of the larger ligand, mainly by facilitating the formation of the prereactive dimer from the solvated monomer. By comparing the binding free energy of hydrophilic Ru-IV-OH and hydrophobic Ru-V=O, the hydrophobic driving force of Ru-V=O in this system has been estimated to 1 kcal mol(-1).

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2018. Vol. 8, no 9, p. 8642-8648
Keywords [en]
water oxidation, binding free energy, diffusion rate, O-O bond formation, rate constant, molecular dynamics, empirical valence bond
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-235594DOI: 10.1021/acscatal.8b02519ISI: 000444364800095Scopus ID: 2-s2.0-85052393349OAI: oai:DiVA.org:kth-235594DiVA, id: diva2:1252191
Note

QC 20181001

Available from: 2018-10-01 Created: 2018-10-01 Last updated: 2018-10-01Bibliographically approved

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Zhan, ShaoqiZou, RongfengAhlquist, Mårten S. G.

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