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Abstract Framework oxide materials are well-known for exhibiting not only negative thermal expansion (NTE), but also demonstrating thermal expansion that can be controlled using composition as a tuning parameter. In this work, we study the intrinsic thermal expansion properties of Co2V2O7, which has shown bulk linear NTE, and attempt to understand how substituting Ni2+for Co2+will affect the thermal expansion. The isomorphic solid solution is synthesized through solid-state methods and characterized using x-ray diffraction (XRD), diffuse reflectance spectroscopy, and neutron diffraction. The size difference between Ni2+and Co2+as well as the polyhedral volume of each Co2+metal coordination environment in the crystal structure allows Ni2+to partially be directed toward one crystallographic site over the other. Variable temperature synchrotron XRD data are employed to understand intrinsic thermal expansion. Across the solid solution, no intrinsic NTE is observed at the microscopic level, yet a degree of tunability in the thermal expansion coefficient with Ni substitution is demonstrated. The disparities between the intrinsic and bulk thermal expansion properties suggest that a morphological mechanism may have resulted in NTE in the bulk.
