We found a match
Your institution may have rights to this item. Sign in to continue.
- Title
Promoting Proton Transfer and Stabilizing Intermediates in Catalytic Water Oxidation via Hydrophobic Outer Sphere Interactions.
- Authors
Liu, Tianqi; Li, Ge; Shen, Nannan; Wang, Linqin; Timmer, Brian J. J.; Kravchenko, Alexander; Zhou, Shengyang; Gao, Ying; Yang, Yi; Yang, Hao; Xu, Bo; Zhang, Biaobiao; Ahlquist, Mårten S. G.; Sun, Licheng
- Abstract
The outer coordination sphere of metalloenzyme often plays an important role in its high catalytic activity, however, this principle is rarely considered in the design of man‐made molecular catalysts. Herein, four Ru‐bda (bda=2,2′‐bipyridine‐6,6′‐dicarboxylate) based molecular water oxidation catalysts with well‐defined outer spheres are designed and synthesized. Experimental and theoretical studies showed that the hydrophobic environment around the Ru center could lead to thermodynamic stabilization of the high‐valent intermediates and kinetic acceleration of the proton transfer process during catalytic water oxidation. By this outer sphere stabilization, a 6‐fold rate increase for water oxidation catalysis has been achieved.
- Subjects
OXIDATION of water; CATALYTIC oxidation; PROTON transfer reactions; SPHERES; PROTONS; CATALYTIC activity
- Publication
Chemistry - A European Journal, 2022, Vol 28, Issue 24, p1
- ISSN
0947-6539
- Publication type
Article
- DOI
10.1002/chem.202104562