2D Co‐Mo‐Hydroxide‐Based Multifunctional Material for the Development of H ₂ ‐Based Clean Energy Technologies

Layered double hydroxides (LDH) based on transition metals are highly flexible in tailoring their dimensionality, lattice, and electronic structures, making them promising candidates as multifunctional 2D materials for the development of clean energy technologies and boosting the use of hydrogen as an energy vector. In this paper, strategic anion substitution in cobalt LDH is an appealing strategy to produce a material with two-fold functionality, electrochemical and magnetocaloric response, offering a sustainable alternative to existing electrocatalysts and cryogenic refrigerants. It is unambiguously demonstrated that (poly)oxomolybdate-based specimens interleave in Co LDH nanosheets up to a Co:Mo = 1:0.4 ratio, leading to an interstratified material. This intercalation greatly benefits the kinetics of the oxygen evolution reaction for H₂ production, boosting the catalytic sites due to the expansion of the interlayer space, induced by the bulky molybdates which also partially modify the Co oxidation state of αCo(OH)₂ nanolayers, favoring charge transfer. In parallel, the interleaved Mo species strengthen superexchange interactions compared with pristine α-Co(OH)₂, effectively adjusting the operating temperature toward the liquid hydrogen range (2030 K). This specific temperature range allows to fill a critical gap in magnetocaloric materials, as few systems can simultaneously achieve both large magnetic entropy changes and structural stability.