Turning Nonmagnetic Two-Dimensional Molybdenum Disulfides into Room-Temperature Ferromagnets by the Synergistic Effect of Lattice Stretching and Charge Injection

Exploring two-dimensional (2D) room-temperature magnetic materials in the field of 2D spintronics remains a formidable challenge. The vast array of nonmagnetic 2D materials provides abundant resources for exploration, but the strategy to convert them into intrinsic room-temperature magnets remains elusive. To address this challenge, we present a general strategy based on surface halogenation for the transition from nonmagnetism to intrinsic room-temperature ferromagnetism in 2D MoS2 based on first-principles calculations. The derived 2D halogenated MoS2 are half-semimetals with a high Curie temperature (TC) of 430–589 K and excellent stability. In-depth mechanistic studies revealed that this marvelous nonmagnetism-to-ferromagnetism transition originates from the modulation of the splitting as well as the occupation of the Mo d orbitals by the synergy of lattice stretching and charge injection induced by the surface halogenation. This work establishes a promising route for exploring 2D room-temperature magnetic materials from the abundant pool of 2D nonmagnetic counterparts

Two-Dimensional Transition Metal Boron Cluster Compounds (MB_<i>n</i>enes) with Strain-Independent Room-Temperature Magnetism

Two-dimensional (2D) metal borides (MBenes) with unique electronic structures and physicochemical properties hold great promise for various applications. Given the abundance of boron clusters, we proposed employing them as structural motifs to design 2D transition metal boron cluster compounds (MBnenes), an extension of MBenes. Herein, we have designed three stable MBnenes (M4(B12)2, M = Mn, Fe, Co) based on B12 clusters and investigated their electronic and magnetic properties using first-principles calculations. Mn4(B12)2 and Co4(B12)2 are semiconductors, while Fe4(B12)2 exhibits metallic behavior. The unique structure in MBnenes allows the coexistence of direct exchange interactions between adjacent metal atoms and indirect exchange interactions mediated by the clusters, endowing them with a Néel temperature (TN) up to 772 K. Moreover, both Mn4(B12)2 and Fe4(B12)2 showcase strain-independent room-temperature magnetism, making them potential candidates for spintronics applications. The MBnenes family provides a fresh avenue for the design of 2D materials featuring unique structures and excellent physicochemical properties

Refining Defect States in W₁₈O₄₉ by Mo Doping: A Strategy for Tuning N₂ Activation towards Solar-Driven Nitrogen Fixation

Photocatalysis may provide an intriguing approach to nitrogen fixation, which relies on the transfer of photoexcited electrons to the ultrastable NN bond. Upon N₂ chemisorption at active sites (e.g., surface defects), the N₂ molecules have yet to receive energetic electrons toward efficient activation and dissociation, often forming a bottleneck. Herein, we report that the bottleneck can be well tackled by refining the defect states in photocatalysts via doping. As a proof of concept, W₁₈O₄₉ ultrathin nanowires are employed as a model material for subtle Mo doping, in which the coordinatively unsaturated (CUS) metal atoms with oxygen defects serve as the sites for N₂ chemisorption and electron transfer. The doped low-valence Mo species play multiple roles in facilitating N₂ activation and dissociation by refining the defect states of W₁₈O₄₉: (1) polarizing the chemisorbed N₂ molecules and facilitating the electron transfer from CUS sites to N₂ adsorbates, which enables the NN bond to be more feasible for dissociation through proton coupling; (2) elevating defect-band center toward the Fermi level, which preserves the energy of photoexcited electrons for N₂ reduction. As a result, the 1 mol % Mo-doped W₁₈O₄₉ sample achieves an ammonia production rate of 195.5 μmol g_cat^–1 h^–1, 7-fold higher than that of pristine W₁₈O₄₉. In pure water, the catalyst demonstrates an apparent quantum efficiency of 0.33% at 400 nm and a solar-to-ammonia efficiency of 0.028% under simulated AM 1.5 G light irradiation. This work provides fresh insights into the design of photocatalyst lattice for N₂ fixation and reaffirms the versatility of subtle electronic structure modulation in tuning catalytic activity