Graphene has initiated intensive research efforts on 2D crystalline materials due to its extraordinary set of properties and the resulting host of possible applications. Here the authors report on the controllable large-scale synthesis of C N, a 2D crystalline, hole-free extension of graphene, its structural characterization, and some of its unique properties. C N is fabricated by polymerization of 2,3-diaminophenazine. It consists of a 2D honeycomb lattice with a homogeneous distribution of nitrogen atoms, where both N and C atoms show a D -symmetry. C N is a semiconductor with an indirect bandgap of 0.39 eV that can be tuned to cover the entire visible range by fabrication of quantum dots with different diameters. Back-gated field-effect transistors made of single-layer C N display an on-off current ratio reaching 5.5 × 10 . Surprisingly, C N exhibits a ferromagnetic order at low temperatures (<96 K) when doped with hydrogen. This new member of the graphene family opens the door for both fundamental basic research and possible future applications.

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Lithium metal batteries are a promising candidate for future high-energy-density energy storage.

Electrode design strategies that aim to increase the electrochemical performance of Li‐ion batteries (LIBs) play a key role in tapping into the power of the energy transformations involved. Metal‐organic frameworks (MOFs) have attracted scientific interest as electrode materials for LIBs, while the utilization of pristine MOFs is hindered by limited conductivity and stability, partly due to their lack of hierarchically structured pores. Herein a hydrothermal‐mechanical synthesis is reported by combining the one‐pot chemical fabrication of Ni3(2,3,6,7,10,11‐hexaiminotriphenylene)2 sheets and particles, and the mechanical assembly of these building blocks to improve electrical conductivity is also described. The as‐prepared ensemble (denoted as NHM) exhibits a Tostadas‐shaped structure with enriched ultramicropores and micropores. The charge‐discharge profile of NHM gives a superior reversible capacity of 1280 mA h g−1 after 100 cycles at the rate of 0.1 A g−1, surpassing the state‐of‐art pristine MOFs‐based anodes. Moreover, NHM is capable of maintaining 392 mA h g−1 at 1 A g−1 after 1000 cycles, the completion of a stability test in coin cell‐powered light emitting diodes further visualizes the remitted capacity fading of NHM. This work breaks through the limitation of capacity for pristine MOFs, providing a new pathway for achieving better energy conversion and storage.

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Page 6: Figure S3. Rationalization for the noncompressed BCHMX case to explain why transfer of the H to the O of an NO 2 group leads to release of a nearby NO 2 molecule rather than the expected HONO release; whereas for the compressed case the HONO is released rather than the nearby NO 2 . The HONO entity is indicated by the red ellipse, while the NO 2 is indicated with a blue ellipse. The free space available for NO 2 releasing reaction in the non-compressed simulation is indicated by the green arc, while the free space available for HONO release in the compressed simulation is indicated by the green arc. Page 7: Figure S4. Species analysis for decomposition of non-compressed BCHMX heated from 300 to 2200 K. The first decomposition reaction for BCHMX occurs at ~ 1770 K (11 ps), releasing one NO 2 molecule. The 2 nd reaction occurs at 1970 K (12.3 ps) releasing one NO 2 from the other BCHMX molecular. The 3 rd reaction occurs at 2000 K releasing one more NO 2 from the decomposed BCHMX fragment. *

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