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Ru-bda: Unique Molecular Water-Oxidation Catalysts with Distortion Induced Open Site and Negatively Charged Ligands
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.ORCID iD: 0000-0002-4093-1251
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry.ORCID iD: 0000-0002-4521-2870
2019 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 141, no 14, p. 5565-5580Article, review/survey (Refereed) Published
Abstract [en]

A water-oxidation catalyst with high intrinsic activity is the foundation for developing any type of water-splitting device. To celebrate its 10 years anniversary, in this Perspective we focus on the state-of-the-art molecular water-oxidation catalysts (MWOCs), the Ru-bda series (bda = 2,2'-bipyridine-6,6'-dicarboxylate), to offer strategies for the design and synthesis of more advanced MWOCs. The O-O bond formation mechanisms, derivatives, applications, and reasons behind the outstanding catalytic activities of Ru-bda catalysts are summarized and discussed. The excellent performance of the Ru-bda catalyst is owing to its unique structural features: the distortion induced 7-coordination and the carboxylate ligands with coordination flexibility, proton transfer function as well as small steric hindrance. Inspired by the Ru-bda catalysts, we emphasize that the introduction of negatively charged groups, such as the carboxylate group, into ligands is an effective strategy to lower the onset potential of MWOCs. Moreover, distortion of the regular configuration of a transition metal complex by ligand design to generate a wide open site as the catalytic site for binding the substrate as an extra-coordination is proposed as a new concept for the design of efficient molecular catalysts. These inspirations can be expected to play a great role in not only water oxidation catalysis but also other small molecule activation and conversion reactions involving artificial photosynthesis, such as CO2 reduction and N-2 fixation reactions.

Place, publisher, year, edition, pages
AMER CHEMICAL SOC , 2019. Vol. 141, no 14, p. 5565-5580
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Chemical Sciences
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URN: urn:nbn:se:kth:diva-251494DOI: 10.1021/jacs.8b12862ISI: 000464769000001PubMedID: 30889353Scopus ID: 2-s2.0-85064226482OAI: oai:DiVA.org:kth-251494DiVA, id: diva2:1316223
Note

QC 20190516

Available from: 2019-05-16 Created: 2019-05-16 Last updated: 2019-05-16Bibliographically approved

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Zhang, BiaobiaoSun, Licheng

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