Optimal surface/diffusion-controlled kinetics of bimetallic selenide nanotubes for hybrid supercapacitors

Nickel chalcogenides, as electrode materials, often have low rate capability and poor cycling stability because of their sluggish diffusion-controlled electrochemical kinetics in aqueous alkaline electrolytes. In this study, Co ions serving as both morphological and electronic modulators were introduced to synthesize NixCo1-xSe2 nanotubes. The chemical composition of these nanotubes can be designed purpose-fully. Moreover, their electrochemical kinetics and pseudocapacitive behavior can be controlled using a typical two-step hydrothermal strategy by tuning the feed amount of Co2+. The optimized Ni0.67Co0.33Se2 electrode provided a distinguished specific capacity (1157F g(-1) at 1 A g(-1)), cycling stability (91% after 2000 cycles), and excellent rate capability (600F g(-1) at 20 A g(-1)). Through calculations, we explain that the obtained Ni0.67Co0.33Se2 electrode has both battery and capacitance behavior and a synergistic effect that combines the complementary advantages of metal Ni and Co ions, thus addressing a massive boost in the specific capacity and cycle performance. Density functional theory (DFT) was used to verify the benefit of substituting Co ions for partial Ni ions in nickel selenides in enhancing charge transfer and accelerating OH- adsorption and deprotonation/protonation reactions. (c) 2022 Elsevier Inc. All rights reserved.