2017
DOI: 10.1039/c6cp06679h
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Tris-bipyridine based dinuclear ruthenium(ii)–osmium(iii) complex dyads grafted onto TiO2 nanoparticles for mimicking the artificial photosynthetic Z-scheme

Abstract: The Z-Scheme function within molecular systems has been rarely reported for solar energy conversion although it offers the possibility to achieve higher efficiency than single photon absorber photosystems due to the use of a wider range of visible light. In this study, we synthesized and investigated the electrochemical and spectroscopic properties of two new dyads based on ruthenium and osmium tris-bipyridine complexes covalently linked via a butane bridge to explore their ability to realize the Z-scheme func… Show more

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Cited by 9 publications
(4 citation statements)
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“…Tpy-metal ion complexes exhibit unique electronic, [3][4][5] chemical, [6][7][8] optical, 3,8,9 photovoltaic, 10 and catalytic 6 properties and have been extensively used in medicinal chemistry, 11 materials science 12 and as catalysts. 6 Specifically, tpy-metal complexes are a vivid field of study with wide range of applications such as i) DNA intercalators, 13,14 ii) catalysts in artificial photosynthesis, 5 in Pulsed electron-electron double resonance spectroscopy PELDOR (pulsed electron-electron double resonance or synonymously double electron-electron resonance, DEER) is a pulse EPR technique commonly performed at cryogenic temperatures that allows measurement of distances between unpaired electrons with angstrom resolution. 26,27 In a nutshell, during a PELDOR experiment a set of unpaired electrons (from here on A spins) is observed using microwave pulses at a frequency ωA, while a second set of unpaired electrons (from here on B spins) is selectively inverted by a microwave pulse at a different frequency, ωB (Fig.…”
Section: Introduction (Bio)macromolecular Assembliesmentioning
confidence: 99%
“…Tpy-metal ion complexes exhibit unique electronic, [3][4][5] chemical, [6][7][8] optical, 3,8,9 photovoltaic, 10 and catalytic 6 properties and have been extensively used in medicinal chemistry, 11 materials science 12 and as catalysts. 6 Specifically, tpy-metal complexes are a vivid field of study with wide range of applications such as i) DNA intercalators, 13,14 ii) catalysts in artificial photosynthesis, 5 in Pulsed electron-electron double resonance spectroscopy PELDOR (pulsed electron-electron double resonance or synonymously double electron-electron resonance, DEER) is a pulse EPR technique commonly performed at cryogenic temperatures that allows measurement of distances between unpaired electrons with angstrom resolution. 26,27 In a nutshell, during a PELDOR experiment a set of unpaired electrons (from here on A spins) is observed using microwave pulses at a frequency ωA, while a second set of unpaired electrons (from here on B spins) is selectively inverted by a microwave pulse at a different frequency, ωB (Fig.…”
Section: Introduction (Bio)macromolecular Assembliesmentioning
confidence: 99%
“…In this state, a negative charge density has been transferred from the ruthenium to the osmium acceptor ion. The positive feature at ∼20 000 cm –1 is rather distinctive, and it is present in several IVCT states of related supramolecular bimetallic {Ru–Os} systems. The IVCT state decays to the GS within 3 ps, matching those lifetimes observed for directly excited IVCT states in cyanide-bridged or alkynyl-bridged , mixed-valent bimetallic complexes. The 1.2 ps process that leads from hot- 3 MLCT to IVCT is an ultrafast electron transfer, enabled thanks to the large metal–metal electronic communication promoted by the cyanide bridge. , Additionally, the metallic dπ orbitals involved in both states extend along the z -axis and have matching (“parallel”) wave-function symmetries, which ensures strong excited-state coupling.…”
mentioning
confidence: 66%
“…Its differential spectrum is strikingly similar to that obtained upon subtracting the differential spectrum corresponding to the {Ru­(tpy)} oxidation process, minus the differential spectrum corresponding to the {M­(CN) 6 } oxidation (Figure ). , Therefore, it is assigned as the {(tpy)­Ru III –NC-Os II } IVCT state, that is, the same excited state that can be populated directly via GSIVCT absorption. In this state, a negative charge density has been transferred from the ruthenium to the osmium acceptor ion.…”
mentioning
confidence: 99%
“…Osmium is predominately used as an alloy with other metals for high wear applications. Osmium nanoparticles have been synthesized by various methods [77,[82][83][84][85][86][87]; however, to date no antimicrobial studies have been conducted on these constructs. Osmium tetroxide (OsO 4 ) injections for the application of synovectomy is used in arthritic patients in Scandinavia and is the only known clinical use of osmium.…”
Section: Osmiummentioning
confidence: 99%