Clustered countercurrent-flow micro-channel reactors (C-CFMCR) with varying magnification times were applied for the preparation of Ni-doped manganese dioxide (Ni-MnO2) via co-precipitation processes. Effects of the feeding flow rate of reactants and the concentration of the doping agent on the doping processes were investigated. The C-CFMCR, which is of intensified micromixing efficiency as compared with conventional stirred reactors (STR), played a crucial role in facilitating the uniform nucleation and growth of MnO2 crystals and then the doping of Ni. As a result, the prepared Ni-MnO2 had a decreased particle size and a more uniform microporous structure. EDS analysis showed an even distribution of Ni2+ within the nanocomposites and thus enhanced electrochemical performance of the MnO2 composite materials as supercapacitor electrodes was achieved. The 1.0 at% Ni-MnO2 nanocomposites prepared under optimal conditions exhibited the highest specific capacitance of ~ 389.6 F g−1 at a current density of 1 A g−1 and showed excellent cycling stability with 79.3% retention of the initial capacitance after 5000 charge/discharge cycles in 2 M KOH aqueous solution. The as-assembled Ni-MnO2//activated carbon (AC) asymmetric supercapacitor displayed a wide operating voltage (0–1.6 V), high energy and power densities (13.3 W h kg−1 and 187.52 W kg−1 at 0.25 A g−1, respectively), and a stable cycling behavior (83.8% capacitance retention after 1000 cycles at 1 A g−1). In addition, only a weak scaling-up effect of C-CFMCR on the co-precipitation process was observed, suggesting that C-CFMCR is a prospective technique for the continuous and large-scale production of nanoparticles.
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