Supercapacitors have attracted great interest because of their fast, reversible operation and sustainability. However, their energy densities remain lower than those of batteries. In the last decade, supercapacitors with an energy content of ∼110 W h L-1 at a power of ∼1 kW L-1 were developed by leveraging the open framework structure of graphene-related architectures. Here, we report that the reaction of fluorographene with azide anions enables the preparation of a material combining graphene-type sp2 layers with tetrahedral carbon-carbon bonds and nitrogen (pyridinic and pyrrolic) superdoping (16%). Theoretical investigations showed that the C-C bonds develop between carbon-centered radicals, which emerge in the vicinity of the nitrogen dopants. This material, with diamond-like bonds and an ultra-high mass density of 2.8 g cm-3, is an excellent host for the ions, delivering unprecedented energy densities of 200 W h L-1 at a power of 2.6 kW L-1 and 143 W h L-1 at 52 kW L-1. These findings open a route to materials whose properties may enable a transformative improvement in the performance of supercapacitor components.

Department of Experimental Physics Faculty of Science Palacký University Olomouc 17 listopadu 1192 12 Olomouc 77900 Czech Republic

Department of Physical Chemistry Faculty of Science Palacký University 17 listopadu 1192 12 779 00 Olomouc Czech Republic

IT4Innovations VŠB Technical University of Ostrava 17 listopadu 2172 15 708 00 Ostrava Poruba Czech Republic

Nanotechnology Centre Centre of Energy and Environmental Technologies VŠB Technical University of Ostrava 17 listopadu 2172 15 Poruba 708 00 Ostrava Czech Republic

Regional Centre of Advanced Technologies and Materials Czech Advanced Technology and Research Institute Palacký University Šlechtitelů 27 783 71 Olomouc Czech Republic

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