MXenes are currently one of the most widely studied two-dimensional materials due to their properties. However, obtaining highly dispersed MXene materials in organic solvent remains a significant challenge for current research. Here, we have developed a method called the tuned microenvironment method (TMM) to prepare a highly concentrated Ti 3 C 2 T x organic solvent dispersion by tuning the microenvironment of Ti 3 C 2 T x . The as-proposed TMM is a simple and efficient approach, as Ti 3 C 2 T x can be dispersed in N,N-dimethylformamide and other solvents by stirring and shaking for a short time, without the need for a sonication step. The delaminated single-layer MXene yield can reach 90% or greater, and a large-scale synthesis has also been demonstrated with TMM by delaminating 30 g of multilayer Ti 3 C 2 T x raw powder in a one-pot synthesis. The synthesized Ti 3 C 2 T x nanosheets dispersed in an organic solvent possess a clean surface, uniform thickness, and large size. The Ti 3 C 2 T x dispersed in an organic solvent exhibits excellent oxidation resistance even under aerobic conditions at room temperature. Through the experimental investigation, the successful preparation of a highly concentrated Ti 3 C 2 T x organic solvent dispersion via TMM can be attributed to the following factors: (1) the intercalation of the cation can lead to the change in the hydrophobicity and surface functionalization of the material; (2) proper solvent properties are required in order to disperse MXene nanosheets well. To demonstrate the applicability of the highly concentrated Ti 3 C 2 T x organic solvent dispersion, a composite fiber with excellent electrical conductivity is prepared via the wet-spinning of a Ti 3 C 2 T x (dispersed in DMF) and polyacrylonitrile mixture. Finally, various types of MXenes, such as Nb 2 CT x , Nb 4 C 3 T x , and Mo 2 Ti 2 C 3 T x , can also be prepared as highly concentrated MXene organic solvent dispersions via TMM, which proves the universality of this method. Thus, it is expected that this work demonstrates promising potential in the research of the MXene material family.
The preparation of highly dispersed metal catalysts with strong electronic metal−support interactions (EMSIs) is of great significance. In this study, oxygen vacancies (OVs) were generated on the surfaces of Co 3 O 4 nanorods (NRs) through NaBH 4 treatment, and then the generated surface OVs were used to anchor gold clusters. The resulting catalyst was used for the hydrodeoxygenation (HDO) of vanillin based on transfer hydrogenation with alcohol donors. The conversion of vanillin and the selectivity to 2-methoxy-4-methylphenol (MMP) both reached 99% under the optimized reaction conditions, and these values were significantly higher than those obtained for the gold catalyst supported on the untreated Co 3 O 4 NRs. The obtained results were verified by theoretical calculations and experimental data and confirmed the existence of strong EMSIs between the OV-enriched Co 3 O 4 NRs (Co 3 O 4 NRs-OVs) and the gold clusters, which allows electron transfer from the Co 3 O 4 NRs to gold. Increasing the number of electrons on the gold surface can promote the catalytic hydrogen transfer of alcohol, in addition to selectively adsorbing the CO group in vanillin to improve the selectivity toward MMP. This strategy based on the OV-anchoring of metals onto the surface of a support can be extended to other metals, thereby providing a promising method for the design of advanced and highly efficient metal catalysts.
Evaluating the delamination process in the synthesis of MXenes (2D transition metal carbides and nitrides) is critical for their development and applications. However, the preparation of large defect-free MXene flakes with high yields is challenging. Here, a power-focused delamination (PFD) strategy is demonstrated that can enhance both the delamination efficiency and yield of large Ti 3 C 2 T x MXene nanosheets through repetitive precipitation and vortex shaking processes. Following this protocol, a colloidal concentration of 20.4 mg mL -1 of the Ti 3 C 2 T x MXene can be achieved after five PFD cycles, and the yield of the basal-plane-defect-free Ti 3 C 2 T x nanosheets reaches 61.2%, which is 6.4-fold higher than that obtained using the sonication-exfoliation method. Both nanometer-thin devices and self-supporting films exhibit excellent electrical conductivities (≈25 000 and 8260 S cm -1 for a 1.8 nm thick monolayer and 11 μm thick film, respectively). Hydrodynamic simulations reveal that the PFD method can efficiently concentrate the shear stress on the surface of the unexfoliated material, leading to the exfoliation of the nanosheets. The PFD-synthesized large MXene nanosheets exhibit superior electrical conductivities and electromagnetic shielding (shielding effectiveness per unit volume: 35 419 dB cm 2 g -1 ). Therefore, the PFD strategy provides an efficient route for the preparation of high-performance single-layer MXene nanosheets with large areas and high yields.
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