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In the field of heterogeneous organic catalysis, molybdenum disulfide (MoS 2 ) is gaining increasing attention as a catalytically active material due to its low toxicity, earth abundance, and affordability. Interestingly, the catalytic properties of this metal-based material can be improved by several strategies. In this Perspective, through the analysis of some explicative examples, the main approaches used to prepare highly efficient MoS 2 -based catalysts in relevant organic reactions are summarized and critically discussed, namely: i) increment of the specific surface area, ii) generation of the metallic 1T phase, iii) introduction of vacancies, iv) preparation of nanostructured hybrids/composites, v) doping with transition metal ions, and vi) partial oxidation of MoS 2 . Finally, emerging trends in MoS 2 -based materials catalysis leading to a richer organic synthesis are presented., (© 2024 The Author(s). Small published by Wiley‐VCH GmbH.)

Controlling the deposition of spin-crossover (SCO) materials constitutes a crucial step for the integration of these bistable molecular systems in electronic devices. Moreover, the influence of functional surfaces, such as 2D materials, can be determinant on the properties of the deposited SCO film. In this work, ultrathin films of the SCO Hofmann-type coordination polymer [Fe(py) 2 {Pt(CN) 4 }] (py = pyridine) onto monolayers of 1T and 2H MoS 2 polytypes are grown. The resulting hybrid heterostructures are characterized by GIXRD, XAS, XPS, and EXAFS to get information on the structure and the specific interactions generated at the interface, as well as on the spin transition. The use of a layer-by-layer results in SCO/2D heterostructures, with crystalline and well-oriented [Fe(py) 2 {Pt(CN) 4 }]. Unlike with conventional Au or SiO 2 substrates, no intermediate self-assembled monolayer is required, thanks to the surface S atoms. Furthermore, it is observed that the higher presence of Fe 3+ in the 2H heterostructures hinders an effective spin transition for [Fe(py) 2 {Pt(CN) 4 }] films thinner than 8 nm. Remarkably, when using 1T MoS 2 , this transition is preserved in films as thin as 4 nm, due to the reducing character of this metallic substrate. These results highlight the active role that 2D materials play as substrates in hybrid molecular/2D heterostructures., (© 2023 The Authors. Small published by Wiley-VCH GmbH.)