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Facet-dependent electrochemical properties of Co3O4 nanocrystals toward heavy metal ions.

ABSTRACT: We revealed an interesting facet-dependent electrochemical behavior toward heavy metal ions (HMIs) based on their adsorption behaviors. The (111) facet of Co3O4 nanoplates has better electrochemical sensing performance than that of the (001) facet of Co3O4 nanocubes. Adsorption measurements and density-functional theory (DFT) calculations reveals that adsorption of HMIs is responsible for the difference of electrochemical properties. Our combined experimental and theoretical studies provide a solid hint to explain the mechanism of electrochemical detection of HMIs using nanoscale metal oxides. Furthermore, this study not only suggests a promising new strategy for designing high performance electrochemical sensing interface through the selective synthesis of nanoscale materials exposed with different well-defined facets, but also provides a deep understanding for a more sensitive and selective electroanalysis at nanomaterials modified electrodes.

SUBMITTER: Yu XY

PROVIDER: S-EPMC3791446 | biostudies-literature | 2013 Oct

REPOSITORIES: biostudies-literature

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Facet-dependent electrochemical properties of Co3O4 nanocrystals toward heavy metal ions.

Yu Xin-Yao XY Meng Qiang-Qiang QQ Luo Tao T Jia Yong Y Sun Bai B Li Qun-Xiang QX Liu Jin-Huai JH Huang Xing-Jiu XJ

Scientific reports 20131007

We revealed an interesting facet-dependent electrochemical behavior toward heavy metal ions (HMIs) based on their adsorption behaviors. The (111) facet of Co3O4 nanoplates has better electrochemical sensing performance than that of the (001) facet of Co3O4 nanocubes. Adsorption measurements and density-functional theory (DFT) calculations reveals that adsorption of HMIs is responsible for the difference of electrochemical properties. Our combined experimental and theoretical studies provide a so ...[more]

PMID: 24097175

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Project description:The facet-dependent redox reactions of diruthenium metal-string complexes by gold nanoparticles (AuNPs) are explored by using the surface-enhanced Raman scattering (SERS) technique. Gold nano-rhombic dodecahedrons (AuRDs), gold nanocubes (AuNCs), and gold octahedrons (AuOhs) with exclusive facets {110}, {100}, and {111}, respectively, were synthesized. These AuNPs linked face-to-face by metal-string complexes Ru2M(dpa)4Cl2 (dpa = dipyridyl amino, M = Ni, Cu) with chloride axial ligands serve as both SERS substrates and reducing agents in the reactions. We employ the diruthenium core in these complexes with multiple redox states to study the reduction ability of varied AuNP facets upon plasmonic excitation. In Ru2Ni(dpa)4Cl2, the Ru-Ru stretching mode νRu-Ru str. lies at 327 cm-1 on the SERS substrate AuOh, but this band shifts to 313 cm-1 on the AuRD and AuNC. The diruthenium moiety was reduced to [Ru2]4+ by the AuRD facet {110} and the AuNC {100}. The gold nanorods in the solution prepared with metal-string complexes bridging head-to-head on {111} facets were used for the SERS substrate. The SERS curves of the complexes in these self-assembled head-to-head rods display νRu-Ru str. at 327 cm-1, which is assigned to having an [Ru2]5+ core. Hence, facets {110} and {100} have a reduction reactivity greater than that of {111}. In Ru2Cu(dpa)4Cl2, the νRu-Ru str. is observed to lie at 312 cm-1 on AuRD, but shifts to 320 cm-1 on the AuNC and AuOh. In the latter cases, the diruthenium moiety was reduced to having a charge of 4+ with electronic configuration π*2δ*2, whereas the former case band at 312 cm-1 with a weaker Ru-Ru bonding is also attributed to [Ru2]4+ but with electron configuration π*4. π*4 lies at an energy greater than π*2δ*2. The electrochemical SERS spectra of diruthenium complexes were recorded to verify their oxidation states. Conclusively, these results yield the reduction reactivity of the following facet: {110} > {100} > {111}. According to the results of the redox reactions, the valence states of the diruthenium metal-string complexes are verified. In the [Ru2] n+ core, n = 4 π*4, 4 π*2δ*2, 5 π*2δ*, and 6 π*δ*, and the νRu-Ru str. is 312, 320, 327, and 337 cm-1, respectively.

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Facet-dependent electrochemical properties of Co3O4 nanocrystals toward heavy metal ions.

Publications

Facet-dependent electrochemical properties of Co3O4 nanocrystals toward heavy metal ions.

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