Redox-active cerium-based metal-organic layers coordinated on carbon nanotubes as materials for supercapacitors

In this work, the redox-active, two-dimensional (2D), and highly dispersible metal-organic layers (MOLs) constructed from hexa-cerium(IV) clusters, CeBTB (BTB = 1,3,5-benzenetribenzoate), were directly coordinated onto the surface of carboxylic acid-functionalized multi-walled carbon nanotubes (CNTs) by utilizing a post-synthetically grafting approach. Nanocomposites with various MOL-to-CNT ratios can be synthesized. Crystallinity, porosity, morphology, electrical conductivity, and electrochemical behaviors of CeBTB and all nanocomposites as well as the chemical interaction between CeBTB and CNT in the composite are investigated. Thin films of materials with the same mass loading are then fabricated for measuring their capacitive performances in neutral aqueous solutions of Na2SO4. With the electrical conductivity provided by carbon nanotubes and the redox activity of CeBTB between Ce(IV) and Ce(III), the optimal CeBTB-CNT nanocomposite can show a better capacitive performance compared to the pristine CeBTB, pristine CNT, and the physical mixture of both of them with the same MOL-to-CNT ratio. With such a simple post-synthetically grafting approach that can precisely control the ratio between the 2D MOLs and CNTs, the findings here open opportunities for designing numerous composites composed of MOLs and nanocarbons with tunable conductivity, redox activity, and functionality, which are potential candidates for a range of applications.