Metal–Organic-Framework-Based Photocatalysts Optimized by Spatially Separated Cocatalysts for Overall Water Splitting

Efficient charge separation and utilization are critical factors in photocatalysis. Herein, it is demonstrated that the complete spatial separation of oxidation and reduction cocatalysts enhances the efficacy of charge separation and surface reaction. Specifically, a Pt@NH₂-UiO-66@MnO_x (PUM) heterostructured photocatalyst with Pt and MnO_x as cocatalysts is designed for the optimization of the NH₂-UiO-66 photocatalyst. Compared with the pristine NH₂-UiO-66, Pt@NH₂-UiO-66 (PU), and NH₂-UiO-66@MnO_x (UM) samples, the PUM sample exhibits the highest hydrogen production activity. As cocatalysts, Pt favors trapping of electrons, while MnO_x tends to collect holes. Upon generation from NH₂-UiO-66, electrons and holes flow inward and outward of the metal–organic framework photocatalyst, accumulating on the corresponding cocatalysts, and then take part in the redox reactions. The PUM photocatalyst greatly prolongs the lifetime of the photogenerated electrons and holes, which favors the electron–hole separation. Furthermore, the PUM sample facilitates overall water splitting in the absence of sacrificial agents, thereby demonstrating its potential as a modification method of MOF-type semiconductors for the overall water-splitting reaction.     

Highly dispersed NiCu nanoparticles on SBA-15 for selective hydrogenation of methyl levulinate to γ-valerolactone

Copper and nickel nanoparticles highly dispersed on an ordered mesoporous silica support (SBA-15) were prepared by a glycol-assisted impregnation method and tested for the catalytic transfer hydrogenation reaction of methyl levulinate to γ-valerolactone (GVL). Characterizations by high resolution transmission electron microscopy, X-ray diffraction, N₂ sorption, H₂ temperature-programmed reduction and X-ray absorption spectroscopy confirm that the highly dispersed nanoparticles were well-anchored to the mesopores of SBA-15 with the strong interaction. Comparing to a catalyst synthesized by a conventional aqueous impregnation method, our catalyst shows a higher conversion and greater selectivity towards GVL of reaction at 140–170 °C using 2-propanol as a solvent and a hydrogen donor. Results showed that NiCu/SBA-15 (EG) had much better activity, providing 91.3% conversion of ML with 89.7% selectivity towards GVL in 3 h at 140 °C. The high compositional homogeneity, uniform distribution of the nanoparticles in the mesoporous channels and the strong interaction between the metal nanoparticles and SBA-15 contribute to the superior catalytic performance. This catalyst also demonstrates superb stability over the course of 5 reaction cycles without significant loss in catalytic activity and selectivity towards GVL formation.     

Ionic conductive polymers as artificial solid electrolyte interphase films in Li metal batteries – A review

Lithium (Li) metal has been considered as the ultimate anode material for next-generation rechargeable batteries due to its ultra-high theoretical specific capacity (3860 mAh g⁻¹) and the lowest reduction voltage (−3.04 V vs the standard hydrogen electrode). However, the dendritic Li formation, uncontrolled interfacial reactions, and huge volume variations lead to unstable solid electrolyte interphase (SEI) layer, low Coulombic efficiency and hence short cycling lifetime. Designing artificial solid electrolyte interphase (artificial SEI) films on the Li metal electrode exhibits great potential to solve the aforementioned problems and enable Li–metal batteries with prolonged lifetime. Polymer materials with good ionic conductivity, superior processability and high flexibility are considered as ideal artificial SEI film materials. In this review, according to the ionic conductive groups, recent advances in polymeric artificial SEI films are summarized to afford a deep understanding of Li ion plating/stripping behavior and present design principles of high-performance artificial SEI films in achieving stable Li metal electrodes. Perspectives regarding to the future research directions of polymeric artificial SEI films for Li–metal electrode are also discussed. The insights and design principles of polymeric artificial SEI films gained in the current review will be definitely useful in achieving the Li–metal batteries with improved energy density, high safety and long cycling lifetime toward next-generation energy storage devices.