ABSTRACT Surface engineering of triboelectric layers is crucial for enhancing the energy‐harvesting performance of triboelectric nanogenerators (TENGs). Herein, a systematic study on the surface modification of polydimethylsiloxane (PDMS) films using radio‐frequency (RF) plasma treatment in different gaseous atmospheres (Ar, O 2 , CF 4 , and O 2 +CF 4 ) is reported to tune the surface properties for enhanced triboelectric performance. The synergistic effect of the plasma process using a mixed gas atmosphere of O 2 +CF 4 with a ratio of 1:4 led to a surface with enhanced polarity, electronegativity, and charge‐trapping ability by combining oxygen‐containing polar functionalities and fluorinated groups. Such changes enabled a significant rise in surface charge density and effective contact area, which greatly increased the output voltage and current of TENG devices. Also, a dual‐filler system consisting of ZnSnO 3 ‐decorated surface‐modified carbon nanotubes (ZTO–SMC) and BaTiO 3 was embedded in the plasma‐treated PDMS matrix to promote dielectric properties and interfacial polarization synergistically. The optimized TENG device exhibited an extraordinary enhancement of voltage (702.88 V) and current (57.03 µA) compared to untreated PDMS‐based devices. This work highlights the prospects for combining plasma‐assisted surface engineering with systematic materials engineering to realize high‐performance TENGs, providing new insights into the development of self‐sustaining energy systems.
Lee et al. (Tue,) studied this question.