期刊
DALTON TRANSACTIONS
卷 41, 期 5, 页码 1475-1480出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c1dt10734h
关键词
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资金
- University of Bath
- EPSRC
- Ministerio de Ciencia e Innovacion in Spain
- EPSRC [EP/H046305/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/H046305/1] Funding Source: researchfish
Metal-organic framework (MOF) materials based on zinc(II) and aluminium(III) dicarboxylate frameworks with covalently attached ferrocene functional redox groups were synthesised by post-synthetic modification and investigated by voltammetry in aqueous and non-aqueous media. In the voltammetry experiments, ferrocene oxidation occurs in all cases, but chemically reversible and stable ferrocene oxidation without decay of the voltammetric response requires a mild dichloroethane solvent environment. The voltammetric response in this case is identified as surface-confined with fast surface-hopping of electrons and without affecting the bulk of MOF microcrystals. In aqueous media a more complex pH-dependent multi-stage redox process is observed associated with chemically irreversible bulk oxidation and disintegration of the MOF framework. A characteristic 30 mV per pH unit dependence of redox potentials is observed attributed to a framework effect: the hydroxide-driven MOF framework dissolution.
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