Unlocking Maximum Synergy: Screen‐Printing Fabrication of Heterostructured Microsupercapacitor Stacks

Abstract A cost‐effective and scalable approach for the fabrication of heterostructured microsupercapacitors (MSCs) employing screen‐printing followed by sequential electrochemical and microspray deposition techniques has been demonstrated. The microsupercapacitor electrode (MSC) that composed of stacked layers of mesoporous carbon, polyaniline (PANI), and MXene hold significant promise for wearable electronics. By adjusting the deposition and spray cycles, the MSC can be readily coated with PANI and MXene. The sequentially stacked two layers of MXene and PANI on the mesoporous carbon spheres (PMPM‐MSC) yielded a specific capacitance of 1003 mF cm −2 at 0.5 mA cm −2 , surpassing the performance of PANI/mesoporous carbon electrode by 1.6 times (771 mF cm −2 ). After 10,000 cycles of charge and discharge, PMPM‐MSCs retained more than 86% of their initial capacitance. In‐situ Raman spectroscopy confirmed the synergistic effects between MXene and PANI within the heterostructured stacked PMPM‐MSC electrodes, including enhanced electronic conductivity and improved electrolyte ion dissociation, which aligned with the electrochemical measurement results, such as fast charge/discharge rates and reduced internal and mass transport resistance. This study demonstrates the potential of screen‐printed heterostructured MSC stacks with maximum electrochemical synergy for portable and wearable energy storage devices.