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Dynamic dimer copper coordination redox shuttles
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DOI：10.1016/j.chempr.2021.10.017.png)
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摘要
En 中文
Conventional redox mediators based on metal coordination complexes undergo electron transfer through the change in oxidation state of the metal center. However, electron transfer kinetics are offset toward preferred oxidation states when preorganized ligands constrain the reorganization of the coordination sphere. In contrast, we report here on dimeric copper(II/I) redox couples, wherein the extent of oxidation/reduction of two metal centers dictates the dynamic formation of dimer and monomer complexes: the dimeric (Cu(I))2 transitions to monomers of Cu(II). The bis(thiazole/ pyrrole)-bipyridine tetradentate ligands stabilize both oxidation states of the unique redox systems. The dynamic dimer redox mediators offer a viable two-electron redox mechanism to develop efficient hybrid solar cells through inhibited recombination and rapid charge transport. Density functional theory calculations reveal inner reorganization energies for single-electron transfer as low as 0.27 eV, marking the dimeric complexes superior redox systems over single complexes as liquid and potentially solid-state electrolytes.
Keyword:
SENSITIZED SOLAR-CELLS
ELECTRON-TRANSFER
MASS-TRANSPORT
SOLID-STATE
COMPLEXES
MEDIATORS
REGENERATION
COBALT
RAMAN
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期刊
IF:
19.6
论文数:
2.8K
被引数:
3.0W
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引用论文
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