Mononuclear ruthenium polypyridine complexes that catalyze water oxidation

Tong, Lianpeng; Thummel, Randolph P.

doi:10.1039/c6sc02766k

Mononuclear ruthenium polypyridine complexes that catalyze water oxidation

Journal Article · Fri Aug 05 00:00:00 EDT 2016 · Chemical Science

DOI:https://doi.org/10.1039/c6sc02766k· OSTI ID:1434583

Tong, Lianpeng ^[1]; Thummel, Randolph P. ^[2]

Univ. of Houston, Houston, TX (United States). Dept. of Chemistry; Friedrich-Alexander Univ. of Erlangen–Nuremberg (FAU), Erlangen (Germany). Dept. of Chemistry and Pharmacy and Inorganic Chemistry; University of Houston
Univ. of Houston, Houston, TX (United States). Dept. of Chemistry

Over the past decade, significant advances have been made in the development of molecular water oxidation catalysts (WOCs) in the context of developing a system that would accomplish artificial photosynthesis. Mononuclear ruthenium complexes with polypyridine ligands have drawn considerable attention in this regard, due to their high catalytic activity and relatively simple structure. In this perspective review, we will discuss mononuclear Ru polypyridine WOCs by organizing them into four groups according to their ligand environments. Each group will be discussed with regard to three fundamental questions: first, how does the catalyst initiate O–O bond formation? Second, which step in the catalytic cycle is rate-determining? Third, how efficient is the catalyst according to the specific descriptors such as turnover frequency? All discussion is based on the high-valent ruthenium intermediates that are proposed in the catalytic cycle according to experimental observation and theoretical simulation. Two fundamental mechanisms are set forth. An acid–base mechanism that involves the attack of a water molecule on the oxo of a high valent Ru=O species to form the O–O bond. Subsequent steps lead to dissociation of O₂ and rehydration of the metal center. A second mechanism involves the formation of a Ru–O˙ radical species, two of which then couple to form a Ru–O–O–Ru species that can release O₂ afterwards. The acid–base mechanism appears to be more common and mechanistic differences could result from variation directly related to polypyridine ligand structures. Thus, understanding how electronic, steric, and conformational properties can effect catalyst performance will lead to the rational design of more effective WOCs with not only ruthenium but also other transition metals.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Houston, Houston, TX (United States)

Sponsoring Organization:: The Welch Foundation, Houston, TX (United States); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: FG02-07ER15888

OSTI ID:: 1434583

Journal Information:: Chemical Science, Journal Name: Chemical Science Journal Issue: 11 Vol. 7; ISSN 2041-6520; ISSN CSHCBM

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Chemical and photochemical water oxidation catalyzed by novel ruthenium complexes comprising a negatively charged NC ^NHC O ligand Su, Wei; Younus, Hussein A.; Zhou, Kui Catalysis Science & Technology, Vol. 7, Issue 2 https://doi.org/10.1039/c6cy02333a	journal	January 2017
Catalyst–solvent interactions in a dinuclear Ru-based water oxidation catalyst Shatskiy, Andrey; Lomoth, Reiner; Abdel-Magied, Ahmed F. Dalton Transactions, Vol. 45, Issue 47 https://doi.org/10.1039/c6dt03789e	journal	January 2016
O–O bond formation in ruthenium-catalyzed water oxidation: single-site nucleophilic attack vs. O–O radical coupling Shaffer, David W.; Xie, Yan; Concepcion, Javier J. Chemical Society Reviews, Vol. 46, Issue 20 https://doi.org/10.1039/c7cs00542c	journal	January 2017
A ruthenium water oxidation catalyst containing a bipyridine glycoluril ligand Mane, Vishwanath S.; Kumbhar, Avinash S.; Thummel, Randolph P. Dalton Transactions, Vol. 46, Issue 38 https://doi.org/10.1039/c7dt02485a	journal	January 2017
Spectroelectrochemical studies of a ruthenium complex containing the pH sensitive 4,4′-dihydroxy-2,2′-bipyridine ligand Viere, Erin J.; Kuhn, Ashley E.; Roeder, Margaret H. Dalton Transactions, Vol. 47, Issue 12 https://doi.org/10.1039/c7dt04554a	journal	January 2018
Synthesis and characterization of [Ru(NC ^NHC O)(bpy)L] ⁺ complexes and their reactivity towards water oxidation Cai, Fanglin; Su, Wei; Younus, Hussein A. New Journal of Chemistry, Vol. 42, Issue 4 https://doi.org/10.1039/c7nj03198j	journal	January 2018
Synthesis, crystal structure and water oxidation activity of [Ru(terpy)(bipy)Cl] ⁺ complexes: influence of ancillary ligands on O ₂ generation Dhiman, Rekha; Singh, Namita; Ugale, Bharat RSC Advances, Vol. 7, Issue 62 https://doi.org/10.1039/c7ra07186h	journal	January 2017
Experimental and computational studies on ruthenium( ii ) bis-diimine complexes of N , N ′-chelate ligands: the origin of changes in absorption spectra upon oxidation and reduction Tan, Siew San; Yanagisawa, Susumu; Inagaki, Kouji Physical Chemistry Chemical Physics, Vol. 21, Issue 15 https://doi.org/10.1039/c8cp05016c	journal	January 2019
Artificial photosynthesis: opportunities and challenges of molecular catalysts Zhang, Biaobiao; Sun, Licheng Chemical Society Reviews, Vol. 48, Issue 7 https://doi.org/10.1039/c8cs00897c	journal	January 2019
Early photophysical events of a ruthenium( ii ) molecular dyad capable of performing photochemical water oxidation and of its model compounds Nastasi, Francesco; Santoro, Antonio; Serroni, Scolastica Photochemical & Photobiological Sciences, Vol. 18, Issue 9 https://doi.org/10.1039/c8pp00530c	journal	January 2019
Structural evolution of the Ru-bms complex to the real water oxidation catalyst of Ru-bda: the bite angle matters Yang, Jing; Liu, Bin; Duan, Lele Dalton Transactions, Vol. 49, Issue 14 https://doi.org/10.1039/c9dt04693c	journal	January 2020
A luminescent on–off probe based calix[4]arene linked through triazole with ruthenium( ii ) polypyridine complexes to sense copper( ii ) and sulfide ions Ramachandran, Mohanraj; Anandan, Sambandam; Ashokkumar, Muthupandian New Journal of Chemistry, Vol. 43, Issue 25 https://doi.org/10.1039/c9nj01632e	journal	January 2019
Redox-active ligand assisted electrocatalytic water oxidation by a mononuclear cobalt complex Biswas, Sachidulal; Bose, Suranjana; Debgupta, Joyashish Dalton Transactions https://doi.org/10.1039/d0dt00838a	journal	January 2020

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