▎ 摘　　要

Defect-engineering of few-layer graphene, by modulating local electronic structure and forming highlyactive reaction sites, benefits the charge storage and electrochemical reactions. To control defect morphology of graphene, herein, we devise a CH4- chemical vapor deposition (CVD) approach to directly synthesize graphene film with extremely high defect density of 5.9 x 10(11) cm(-2) and relatively high crystallinity at a low temperature of 700 degrees C. The C atoms involved in Cu bulk are induced to segregate onto the Cu surface to establish synergetic C-Cu complex catalyst. Theoretical evidence verifies that the interaction between the Cu and C atoms in form of C cluster atop the Cu plane lowers energy barriers for stepwise decomposition of CH4. The (CH4)-C-13 isotope data demonstrate that the C clusters are integrated sequentially into the graphene lattice, unraveling the dual roles of carbon impurities. The defective graphene film exhibits a specific capacitance of 10.6 mu F/cm(2) and excellent electro-catalytic performance. Such a self-induced synergetic catalyst can innovate the methodology of catalysis engineering for controllable synthesis of graphene and other 2D materials. (C) 2019 Elsevier Ltd. All rights reserved.