Tailored design of ruthenium molecular catalysts with 2,2′-bypyridine-6,6′-dicarboxylate and pyrazole based ligands for water oxidation

2016 ◽  
Vol 45 (37) ◽  
pp. 14689-14696 ◽  
Author(s):  
Quentin Daniel ◽  
Lei Wang ◽  
Lele Duan ◽  
Fusheng Li ◽  
Licheng Sun

A series of tailor-designed Ruthenium based water oxidation catalysts have been synthesized. By fine tuning of the catalyst structure, the turnover frequency was increased up to 500 s−1and the stability over 6000 turnovers.

Molecules ◽  
2019 ◽  
Vol 25 (1) ◽  
pp. 157 ◽  
Author(s):  
Dandan Gao ◽  
Ivan Trentin ◽  
Ludwig Schwiedrzik ◽  
Leticia González ◽  
Carsten Streb

This review describes major advances in the use of functionalized molecular metal oxides (polyoxometalates, POMs) as water oxidation catalysts under electrochemical conditions. The fundamentals of POM-based water oxidation are described, together with a brief overview of general approaches to designing POM water oxidation catalysts. Next, the use of POMs for homogeneous, solution-phase water oxidation is described together with a summary of theoretical studies shedding light on the POM-WOC mechanism. This is followed by a discussion of heterogenization of POMs on electrically conductive substrates for technologically more relevant application studies. The stability of POM water oxidation catalysts is discussed, using select examples where detailed data is already available. The review finishes with an outlook on future perspectives and emerging themes in electrocatalytic polyoxometalate-based water oxidation research.


2012 ◽  
Vol 65 (6) ◽  
pp. 638 ◽  
Author(s):  
Alex Izgorodin ◽  
Orawan Winther-Jensen ◽  
Douglas R. MacFarlane

Future requirements for water splitting technologies need highly efficient water oxidation catalysts that are sufficiently stable for operation over many years. Recent research has achieved significant progress in improving the electro-catalytic activities of these catalysts. However, there has not been a strong research focus on their long-term mechanical and chemical stability, yet this is critical for commercial application. In this paper we discuss some of the chemical and thermodynamic challenges confronting this goal, as well as some of the strategies that are available to overcome them. The challenge becomes even greater in the area of photo-active electromaterials; fortunately some of the same strategies may allow progress in this area also.


2021 ◽  
Author(s):  
Yuta Tsubonouchi ◽  
Eman A. Mohamed ◽  
Zaki N. Zahran ◽  
Masayuki Yagi

Polypyridyl ruthenium(II) complexes have been widely researched as promising functional molecules. We have found unique photoisomerization reactions of polypyridyl ruthenium(II) aquo complexes. Recently we have attempted to provide insight into the mechanism of the photoisomerization of the complexes and distinguish between the distal−/proximal-isomers in their physicochemical properties and functions. Moreover, polypyridyl ruthenium(II) aquo complexes have been intensively studied as active water oxidation catalysts (WOCs) which are indispensable for artificial photosynthesis. The catalytic aspect and mechanism of water oxidation by the distal-/proximal-isomers of polypyridyl ruthenium(II) aquo complexes have been investigated to provide the guided thought to develop more efficient molecular catalysts for water oxidation. The recent progress on the photoisomerization and water oxidation of polypyridyl ruthenium(II) aquo complexes in our group are reviewed to understand the properties and functions of ruthenium complexes.


2020 ◽  
Vol 49 (39) ◽  
pp. 13753-13759
Author(s):  
Timofey Liseev ◽  
Andrew Howe ◽  
Md Asmaul Hoque ◽  
Carolina Gimbert-Suriñach ◽  
Antoni Llobet ◽  
...  

Incorporating molecular catalysts into metal–organic frameworks (MOFs) is a promising strategy for improving their catalytic longevity and recyclability.


ACS Catalysis ◽  
2017 ◽  
Vol 7 (9) ◽  
pp. 6235-6244 ◽  
Author(s):  
Jann Odrobina ◽  
Julius Scholz ◽  
Marcel Risch ◽  
Sebastian Dechert ◽  
Christian Jooss ◽  
...  

2015 ◽  
Vol 51 (37) ◽  
pp. 7883-7886 ◽  
Author(s):  
Lei Wang ◽  
Ke Fan ◽  
Quentin Daniel ◽  
Lele Duan ◽  
Fusheng Li ◽  
...  

A molecular water-oxidation catalyst polymerized on a graphite electrode has shown a high initial turnover frequency (TOF) of 10.47 s−1 at ∼700 mV overpotential, and a high turnover number (TON) of 31 600 in 1 h electrolysis.


2020 ◽  
Author(s):  
Laurent Sévery ◽  
Jacek Szczerbiński ◽  
Mert Taskin ◽  
Isik Tuncay ◽  
Fernanda Brandalise Nunes ◽  
...  

The strategy of anchoring molecular catalysts on electrode surfaces combines the high selectivity and activity of molecular systems with the practicality of heterogeneous systems. The stability of molecular catalysts is, however, far less than that of traditional heterogeneous electrocatalysts, and therefore a method to easily replace anchored molecular catalysts that have degraded could make such electrosynthetic systems more attractive. Here, we apply a non-covalent “click” chemistry approach to reversibly bind molecular electrocatalysts to electrode surfaces via host-guest complexation with surface-anchored cyclodextrins. The host-guest interaction is remarkably strong and allows the flow of electrons between the electrode and the guest catalyst. Electrosynthesis in both organic and aqueous media was demonstrated on metal oxide electrodes, with stability on the order of hours. The catalytic surfaces can be recycled by controlled release of the guest from the host cavities and readsorption of fresh guest. This strategy represents a new approach to practical molecular-based catalytic systems.


2021 ◽  
Vol 7 (13) ◽  
pp. eabf3989
Author(s):  
Jiong Wang ◽  
Shuo Dou ◽  
Xin Wang

Heterogeneous molecular catalysts based on transition metal complexes have received increasing attention for their potential application in electrochemical energy conversion. The structural tuning of first and second coordination spheres of complexes provides versatile strategies for optimizing the activities of heterogeneous molecular catalysts and appropriate model systems for investigating the mechanism of structural variations on the activity. In this review, we first discuss the variation of first spheres by tuning ligated atoms; afterward, the structural tuning of second spheres by appending adjacent metal centers, pendant groups, electron withdrawing/donating, and conjugating moieties on the ligands is elaborated. Overall, these structural tuning resulted in different impacts on the geometric and electronic configurations of complexes, and the improved activity is achieved through tuning the stability of chemisorbed reactants and the redox behaviors of immobilized complexes.


2021 ◽  
Vol 60 (3) ◽  
pp. 1806-1813
Author(s):  
Husain N. Kagalwala ◽  
Mahesh S. Deshmukh ◽  
Elamparuthi Ramasamy ◽  
Neelima Nair ◽  
Rongwei Zhou ◽  
...  

Solar RRL ◽  
2021 ◽  
Author(s):  
Matthew V. Sheridan ◽  
Benjamin D. Sherman ◽  
Yi Xie ◽  
Ying Wang

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