The Kirkendall effect is a consequence of the different diffusivities of atoms in a diffusion couple causing a supersaturation of lattice vacancies. This supersaturation may lead to a condensation of extra vacancies in the form of so-called “Kirkendall voids” close to the interface. On the macroscopic and micrometer scale these Kirkendall voids are generally considered as a nuisance because they deteriorate the properties of the interface. In contrast, in the nanoworld the Kirkendall effect has been positively used as a new fabrication route to designed hollow nano-objects. In this Review we summarize and discuss the demonstrated examples of hollow nanoparticles and nanotubes induced by the Kirkendall effect. Merits of this route are compared with other general methods for nanotube fabrication. Theories of the kinetics and thermodynamics are also reviewed and evaluated in terms of their relevance to experiments. Moreover, nanotube fabrication by solid-state reactions and non-Kirkendall type diffusion processes are covered.

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Formation of nanotubes and hollow nanoparticles based on Kirkendall and diffusion processes: a review.

There is a deep interest in methods to fabricate hollow nanocrystals for potential application as high-efficiency catalysts or drug-delivery agents. Tubular one-dimensional nanocrystals have been prepared for a wide variety of materials, including semiconductors1,2, metals3,4, ferroelectrics5,6 and magnetite7. They can be produced by rolling up layered materials or via an axial growth in a rolled-up form8,9,10, coating pores in templates11 or by eliminating the core of a core-shell nanowire1,7. The Kirkendall effect, a classical phenomenon in metallurgy12, was recently applied to explain the formation of hollow spherical nanocrystals13,14,15,16,17. Although the experimental demonstration and theoretical treatment mainly concern binary compounds and planar interfaces or nanoscale spherical interfaces, the fabrication route provided by the Kirkendall effect should be generic, and should also work for high-aspect-ratio hollow cylinders (that is, nanotubes) or even more complex superstructures. In this letter, we report, for the first time, on ultra-long single-crystal ZnAl2O4 spinel nanotubes (total diameter: ∼40 nm, wall thickness: ∼10 nm) fabricated through a spinel-forming interfacial solid-state reaction of core-shell ZnO–Al2O3 nanowires involving the Kirkendall effect. Our results simultaneously represent an extension of applying the Kirkendall effect in fabricating hollow nano-objects from zero-dimensional to multidimensional, and from binary to ternary systems.

Monocrystalline spinel nanotube fabrication based on the Kirkendall effect

Ionic liquids (ILs), 1-butyl-3-methylimidazolium tetrafluoroborate (bmimBF4), were substituted for polar water and formed nonaqueous microemulsions with toluene by the aid of nonionic surfactant TX-100. The phase behavior of the ternary system was investigated, and microregions of bmimBF4-in-toluene (IL/O), bicontinuous, and toluene-in-bmimBF4 (O/IL) were identified by traditional electrical conductivity measurements. Dynamic light scattering (DLS) revealed the formation of the IL microemulsions. The micropolarities of the IL/O microemulsions were investigated by the UV−vis spectroscopy using the methyl orange (MO) and methylene blue (MB) as absorption probes. The results indicated that the polarity of the IL/O microemulsion increased only before the IL pools were formed, whereas a relatively fixed polar microenvironment was obtained in the IL pools of the microemulsions. Moreover, UV−vis spectroscopy has also shown that ionic salt compounds such as Ni(NO3)2, CoCl2, CuCl2, and biochemical reagent riboflav...

Studies on the micropolarities of bmimBF4/TX-100/toluene ionic liquid microemulsions and their behaviors characterized by UV-visible spectroscopy.

The controlled synthesis of SrCO3 nanostructures with different morphologies, such as rodlike, whiskerlike, ellipsoidlike, and spherelike, were successfully achieved by the cationic surfactant-CTAB-microemulsion-mediated solvothermal method. Various comparison experiments showed that fundamental experimental parameters, such as the molar ratio of H2O to CTAB and the concentration of reactants, played important roles in the morphological control of SrCO3 nanostructures. A lower molar ratio of H2O to CTAB favors rodlike products, whereas a higher molar ratio generally leads to the formation of spherical products. A rational mechanism based on fusion, aggregate, and coalescence of microemulsion droplets is proposed for the selective formation of various morphologies. X-ray powder diffraction (XRD), transmission electron microscopy (TEM), selected area electron diffraction (SAED), and field-emission scanning electron microscope (FE-SEM) were used to characterize the products.

Microemulsion-mediated solvothermal synthesis of SrCO3 nanostructures.

Generally, a microemulsion consists of oil, water, surfactant, and sometimes cosurfactant. Herein, we report a surfactant-free microemulsion (denoted as SFME), consisting of oleic acid (oil phase), water, and n-propanol without the amphiphilic molecular structure of a traditional surfactant. The phase behavior of the ternary system was investigated, showing that there were a single-phase microemulsion region and a multiphase region in the ternary phase diagram. The electrical conductivity measurement was employed to investigate the microregions of the single-phase microemulsion region, and three different microregions, that is, water-in-oleic acid (W/O), a bicontinuous (B.C.) region, and oleic acid-in-water (O/W), were identified, which were further confirmed by freeze-fracture and cryogenic transmission electron microscopy (FF-TEM and Cryo-TEM) observations. The polarity and the salt solubility of water domains in the W/O SFME were investigated by UV–visible spectroscopy using methyl orange and potassium...

Surfactant-free microemulsion composed of oleic acid, n-propanol, and H2O.

The first titanium phosphate nanotubes with alternating interlayer spacings have been successfully prepared and characterized. The synthesis is accomplished in a reverse microemulsion formed in an amine extraction system. TEM data from samples made after different times of reaction suggest a scrolling-formation mechanism.

Microemulsion-based synthesis of titanium phosphate nanotubes via amine extraction system.

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Microemulsion-based synthesis of titanium phosphate nanotubes via amine extraction system.