Half‐sandwich ruthenium complex with a very low overpotential and excellent activity for water oxidation under acidic conditions

Younus, Hussein A.; Yildiz, Ibrahim; Ahmad, Nazir; Mohamed, Hemdan S.; Khabiri, Gomaa; Zhang, Shiguo; Verpoort, Francis; Liu, Piao; Zhang, Yan

doi:10.1002/aoc.6538

Title: Half‐sandwich ruthenium complex with a very low overpotential and excellent activity for water oxidation under acidic conditions

Journal Article · 10 December 2021 · Applied Organometallic Chemistry

DOI: https://doi.org/10.1002/aoc.6538 · OSTI ID:1996871

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College of Materials Science and Engineering Hunan University Changsha China, Chemistry Department, Faculty of Science Fayoum University Fayoum Egypt
College of Arts and Sciences Khalifa University of Science and Technology Abu Dhabi United Arab Emirates
Department of Chemistry Government College University Lahore Pakistan
Physics Department, Faculty of Science Fayoum University Fayoum Egypt
College of Materials Science and Engineering Hunan University Changsha China
Laboratory of Organometallics, Catalysis and Ordered Materials, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan China
Hunan LEED Electronic Ink Co., Ltd. Zhuzhou China

Abstract Molecular catalysts are acknowledged for the ability to design reaction sites within well‐defined structures to achieve high catalytic activities. However, in many cases, molecular catalysts undergo structural changes to some other form(s), which are finally the real catalysts. Here, we report two half‐sandwich ruthenium complexes; [Ru([9]aneN3)(bpy)Cl] ⁺ 3 and [Ru([9]aneN3)(pic)OH ₂ ] ²⁺ 4 , based on the macrocyclic 1,4,7‐triazacyclononane ([9]aneN3) ligand for water oxidation (WO). The two complexes have similar core but different ancillary ligands, which greatly affected their stability as well as activity for WO. Complex 3 retained high stability and excellent activity (turnover number [TON] = 1250) in chemical WO and first‐order reaction kinetics with respect to [Ce ^IV ] with a calculated rate constant ( k _cat ) of 34.59 s ⁻¹ . Further, the complex demonstrated very low overpotential of ~210 mV in electrochemical WO. At an overpotential of only 400 mV, turnover frequency (TOF) of complex 3 was electrochemically estimated to be 131.2 s ⁻¹ . In contrast, complex 4 underwent picolinate ligand dissociation, as a deactivation pathway, to form the tri‐aqua derivative. Density functional theory (DFT) calculations are used to explain the dissociation mechanism of picolinate ligand in complex 4 , which happens through a stepwise dissociation mechanism.

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Sponsoring Organization:: USDOE

OSTI ID:: 1996871

Journal Information:: Applied Organometallic Chemistry, Journal Name: Applied Organometallic Chemistry Journal Issue: 3 Vol. 36; ISSN 0268-2605

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: United Kingdom

Language:: English

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