A simple chemical protocol to prepare core–shell gold@spin‐crossover (Au@SCO) nanoparticles (NPs) based on the 1D spin‐crossover [Fe(Htrz)₂(trz)](BF₄) coordination polymer is reported. The synthesis relies on a two‐step approach consisting of a partial surface ligand substitution of the citrate‐stabilized Au NPs followed by the controlled growth of a very thin layer of the SCO polymer. As a result, colloidally stable core@shell spherical NPs with a Au core of ca. 12 nm and a thin SCO shell 4 nm thick, are obtained, exhibiting a narrow distribution in sizes. Differential scanning calorimetry proves that a cooperative spin transition in the range 340–360 K is maintained in these Au@SCO NPs, in full agreement with the values reported for pristine 4 nm SCO NPs. Temperature‐dependent charge‐transport measurements of an electrical device based on assemblies of these Au@SCO NPs also support this spin transition. Thus, a large change in conductance upon spin state switching, as compared with other memory devices based on the pristine SCO NPs, is detected. This results in a large improvement in the sensitivity of the device to the spin transition, with values for the ON/OFF ratio which are an order of magnitude better than the best ones obtained in previous SCO devices.

Antimonene, a novel group 15 two-dimensional material, is attracting great attention due to its outstanding physical and chemical properties. Despite its thermodynamic stability, the pronounced covalent character of the interlayer interactions imposes severe limitations on its exfoliation into mono- and few-layer. Here, we develop a systematic study of liquid phase exfoliation (LPE) with the aim to optimize antimonene production in terms of concentration and dimensional anisotropy, investigating the most relevant experimental factors affecting the exfoliation: pre-processing of pristine antimony, solvent selection based on Hansen solubility parameters and ultrasound conditions. Moreover, exhaustive characterization by means of turbidimetry, XRD, Raman spectroscopy, XPS, AFM, SEM, XEDS and TEM has been carried out. Indeed, we achieved concentration values of ca. 0.368 g L⁻¹ (∼yield of 37 wt%), up to ∼30 times higher compared to the highest value so far reported, with ca. 50% of the nanolayers with heights between 2 and 10 nm and lateral dimensions in the 40–300 nm range. Furthermore, it has been demonstrated that the yield of the process can be enhanced up to ∼90 wt% by recycling the sediment to perform a maximum of 7 cycles. Moreover, we have illustrated the usefulness of this approach by characterizing the electrochemical behaviour of antimonene as a catalyst for the hydrogen evolution reaction (HER). This study provides important insights into the LPE and electrochemical properties of antimonene, allowing its large-scale production and paving the way for its application in fields of utmost importance such as energy storage and conversion or catalysis.