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Metal-Ligand Cooperation in Single-Site Ruthenium Water Oxidation Catalysts: A Combined Experimental and Quantum Chemical Approach
KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Kemi, Organisk kemi.ORCID-id: 0000-0002-6089-5454
Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Key Lab Mat Chem Energy Convers & Storage, Hubei Key Lab Mat Chem & Serv Failure,Minist Educ, Wuhan 430074, Hubei, Peoples R China..
Stockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, Sweden..
Huazhong Univ Sci & Technol, Sch Chem & Chem Engn, Key Lab Mat Chem Energy Convers & Storage, Hubei Key Lab Mat Chem & Serv Failure,Minist Educ, Wuhan 430074, Hubei, Peoples R China..ORCID-id: 0000-0002-8989-6928
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2018 (Engelska)Ingår i: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 57, nr 17, s. 10881-10895Artikel i tidskrift (Refereegranskat) Published
Abstract [en]

Catalysts for oxidation of water to molecular oxygen are essential in solar-driven water splitting. In order to develop more efficient catalysts for this oxidatively demanding reaction, it is vital to have mechanistic insight in order to understand how the catalysts operate. Herein, we report the mechanistic details associated with the two Ru catalysts 1 and 2. Insight into the mechanistic landscape of water oxidation catalyzed by the two single-site Ru catalysts was revealed by the use of a combination of experimental techniques and quantum chemical calculations. On the basis of the obtained results, detailed mechanisms for oxidation of water by complexes 1 and 2 are proposed. Although the two complexes are structurally related, two deviating mechanistic scenarios are proposed with metal-ligand cooperation being an important feature in both processes. The proposed mechanistic platforms provide insight for the activation of water or related small molecules through nontraditional and previously unexplored routes.

Ort, förlag, år, upplaga, sidor
American Chemical Society (ACS), 2018. Vol. 57, nr 17, s. 10881-10895
Nationell ämneskategori
Kemi
Identifikatorer
URN: urn:nbn:se:kth:diva-235445DOI: 10.1021/acs.inorgchem.8b01527ISI: 000443923700046PubMedID: 30133266Scopus ID: 2-s2.0-85053049783OAI: oai:DiVA.org:kth-235445DiVA, id: diva2:1251534
Forskningsfinansiär
Vetenskapsrådet, 621-2013-4872 621-2012-2404Knut och Alice Wallenbergs Stiftelse
Anmärkning

QC 20180927

Tillgänglig från: 2018-09-27 Skapad: 2018-09-27 Senast uppdaterad: 2018-09-27Bibliografiskt granskad

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Kärkäs, Markus D.Liao, Rong-ZhenÅkermark, Björn
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Inorganic Chemistry
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