Current energy and environmental challenges demand the development and design of multifunctional porous materials with tunable properties for catalysis, water purification, and energy conversion and storage. Because of their amenability to de novo reticular chemistry, metal-organic frameworks (MOFs) have become key materials in this area. However, their usefulness is often limited by low chemical stability, conductivity and inappropriate pore sizes. Conductive two-dimensional (2D) materials with robust structural skeletons and/or functionalized surfaces can form stabilizing interactions with MOF components, enabling the fabrication of MOF nanocomposites with tunable pore characteristics. Graphene and its functional derivatives are the largest class of 2D materials and possess remarkable compositional versatility, structural diversity, and controllable surface chemistry. Here, we critically review current knowledge concerning the growth, structure, and properties of graphene derivatives, MOFs, and their graphene@MOF composites as well as the associated structure-property-performance relationships. Synthetic strategies for preparing graphene@MOF composites and tuning their properties are also comprehensively reviewed together with their applications in gas storage/separation, water purification, catalysis (organo-, electro-, and photocatalysis), and electrochemical energy storage and conversion. Current challenges in the development of graphene@MOF hybrids and their practical applications are addressed, revealing areas for future investigation. We hope that this review will inspire further exploration of new graphene@MOF hybrids for energy, electronic, biomedical, and photocatalysis applications as well as studies on previously unreported properties of known hybrids to reveal potential "diamonds in the rough".

Analytical Chemistry Center for Electrochemical Sciences Faculty of Chemistry and Biochemistry Ruhr Universität Bochum Universitätsstrasse 150 Bochum D 44780 Germany

Department of Chemistry Indian Institute of Technology Jammu Jammu and Kashmir 181221 India

Inorganic and Metal Organic Chemistry Department of Chemistry and Catalysis Research Centre Technical University of Munich Garching 85748 Germany

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

Lehrstuhl für Anorganische Chemie 1 Technische Universität Dresden Bergstrasse 66 Dresden 01067 Germany

Max Planck Institute for Chemical Energy Conversion Stiftstrasse 34 36 Mülheim an der Ruhr D 45470 Germany

Nachwuchsgruppe Gestaltung des Sauerstoffentwicklungsmechanismus Helmholtz Zentrum Berlin für Materialien und Energie GmbH Hahn Meitner Platz 1 Berlin 14109 Germany

Nanotechnology Centre CEET VŠB Technical University of Ostrava 17 Listopadu 2172 15 Ostrava Poruba 708 00 Czech Republic

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

School of Chemistry and Physics Queensland University of Technology 2 George Street Brisbane Queensland 4001 Australia

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