The conversion of nitrogen to ammonia offers a sustainable and environmentally friendly approach for producing precursors for fertilizers and efficient energy carriers. Owing to the large energy density and significant gravimetric hydrogen content, NH3 is considered an apt next-generation energy carrier and liquid fuel. However, the low conversion efficiency and slow production of ammonia through the nitrogen reduction reaction (NRR) are currently bottlenecks, making it an unviable alternative to the traditional Haber-Bosch process for ammonia production. The rational design and engineering of catalysts (both photo- and electro-) represent a crucial challenge for improving the efficiency and exploiting the full capability of the NRR. In the present review, we highlight recent progress in the development of graphene-based systems and graphene derivatives as catalysts for the NRR. Initially, the history, fundamental mechanism, and importance of the NRR to produce ammonia are briefly discussed. We also outline how surface functionalization, defects, and hybrid structures (single-atom/multiatom as well as composites) affect the N2 conversion efficiency. The potential of graphene and graphene derivatives as NRR catalysts is highlighted using pertinent examples from theoretical simulations as well as machine learning based performance predictive methods. The review is concluded by identifying the crucial advantages, drawbacks, and challenges associated with principal scientific and technological breakthroughs in ambient catalytic NRR.

Centre for Incubation Innovation Research and Consultancy and Department of Chemistry Jyothy Institute of Technology Thataguni Off Kanakpura Road Bangalore Karnataka 560082 India

Centre for Materials Science School of Chemistry and Physics Queensland University of Technology 2 George Street Brisbane QLD 4001 Australia

CSIR Central Institute of Mining and Fuel Research Digwadih Campus PO FRI Dhanbad Jharkhand 828 108 India

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

Department of Energy and Materials Engineering Dongguk University Seoul 100 715 South Korea

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

Lehrstuhl für Anorganische Chemie 1 Technische Universität Dresden Bergstr 66 01069 Dresden Germany

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

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

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