Aperture-Adjustable and Repairable Metal-Based MOFs Catalysis Membrane for Water Purification

Precise adjustment of the pore size, damage repair, and efficient cleaning is all challenges for the wider application of inorganic membranes. This study reports a simple strategy of combining dry-wet spinning and electrosynthesis to fabricate stainless-steel metal–organic framework composite membranes characterized by customizable pore sizes, targeted reparability, and high catalytic activity for membrane cleaning. The membrane pore size can be precisely customized in the range of 14–212 nm at nanoscale, and damaged membranes can be repaired by targeted treatment in 120 s. In addition, advanced oxidation processes can be used to quickly clean the membrane and achieve 98% flux recovery. The synergistic actions of the membrane matrix and the selective layer increase the adsorption energy of active sites to oxidant, shorten the electron transfer cycle, and enhance the overall catalytic performance. This study can provide a new direction for the development of advanced membranes for water purification and high-efficiency membrane cleaning methods.     

Electrocatalysis of Fe-N-C Bonds Driving Reliable Interphase and Fast Kinetics for Phosphorus Anode in Sodium-Ion Batteries

Phosphorus exhibits high capacity and low redox potential, making it a promising anode material for future sodium-ion batteries. However, its practical applications are confined by poor durability and sluggish kinetics. Herein, an innovative in-situ electrochemically self-driven strategy is presented to embed phosphorus nanocrystal (≈10 nm) into a Fe-N-C-rich 3D carbon framework (P/Fe-N-C). This strategy enables rapid and high-capacity sodium ion storage. Through a combination of experimental assistance and theoretical calculations, a novel synergistic catalytic mechanism of Fe-N-C is reasonably proposed. In detail, the electrochemical formation of Fe-N-C catalytic sites facilitates the release of fluorine in ester-based electrolyte, inducing Na⁺-conducting-enhanced solid-electrolyte interphase. Furthermore, it also effectively induces the dissociation energy of the P-P bond and promotes the reaction kinetics of P anode. As a result, the unconventional P/Fe-N-C anode demonstrates outstanding rate-capability (267 mAh g⁻¹ at 100 A g⁻¹) and cycling stability (72%, 10 000 cycles). Notably, the assembled pouch cell achieves high-energy density of 220 Wh kg⁻¹.     

Fine-Tuning Alkyl Chains on Quinoxaline Nonfullerene Acceptors Enables High-Efficiency Ternary Organic Solar Cells with Optimizing Molecular Stacking and Reducing Energy Loss

Material design of guest acceptor is always a big challenge for improving the efficiency of ternary organic solar cells (OSCs). Here, a pair of isomeric nonfullerene acceptors based on quinoxaline core, Qx–p-C₇H₈O and Qx–m-C₇H₈O, is designed and synthesized. By moving the alkoxy chain attached on side phenyl from meta-position to para-position, both π–π stacking distance and crystallinity are enhanced simultaneously. They obtain the uplifted lowest unoccupied molecular orbital level. Compared to Qx–m-C₇H₈O, Qx–p-C₇H₈O exhibits wider absorption spectrum and higher extinction coefficient. Using D18-Cl:N3 as host materials, the addition of guest acceptor Qx–p-C₇H₈O significantly improves the power conversion efficiency (PCE) from 17.61% to 18.49% because of higher open-circuit voltage (0.875 V) and short-circuit current density (27.85 mA cm⁻²). This can be attributed to the faster exciton dissociation, more balanced carrier mobility, fine fiber morphology, and lower energy loss in the ternary devices. However, Qx–m-C₇H₈O-based ternary device achieves relatively low PCE of 17.17% because this device shows extremely low electron mobility. The results indicate that molecular stacking, film morphology, etc., can be effectively modulated by fine-tuning the side chains of guest materials, which may be an effective design rule for further improving the PCE of OSCs.     

Frontiers in Circularly Polarized Phosphorescent Materials

Circularly polarized luminescence (CPL) materials have received increasing attention in recent years. Amongst various CPL materials, circularly polarized phosphorescence (CPP) materials featuring long life-time represent a novel research frontier and exhibit promising applications in various fields. Herein, the state-of-the-art advances of CPP materials are systematically summarized, as classified into transition metal complexes, organic small molecules, polymers, and organic/inorganic hybrid materials. Besides, the recent applications of CPP materials in organic light-emitting diodes and encryption display are also summarized. Furthermore, the current challenges and future perspectives are put forward. It is expected that this review will offer more inspirations for the future rational design of advanced CPP materials, thus further promoting their future practical applications.     

Grafted MXenes Based Electrolytes for 5V-Class Solid-State Batteries

Polymer blends based solid polymer electrolytes (SPEs), combining the advantages of multiple polymers, are promising for the utilization of 5 V-class cathodes (e.g., LiCoMnO₄ (LCMO)) with enhanced safety. However, severe macro-phase separation with defects and voids in polymer blends restrict the electrochemical stability and ionic migration of SPEs. Herein, inorganic compatibilizer polyacrylonitrile grafted MXene (MXene-g-PAN) is exploited to improve the miscibility of the poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF)/PAN blends and suppress the consolidation of phase particles. The resulting SPE exhibits a high anodic stability with an ionic conductivity of 2.17 × 10⁻⁴ S cm⁻¹, enabling a stable and reversible Li platting/stripping (over 2500 h). The fabricated solid Li‖LCMO cell delivers a 5.1 V discharge voltage with a decent capacity (131 mAh g⁻¹) and cycling performance. Subsequently, the solid all-in-one graphite‖LCMO battery is also constructed to extend the application of MXene based SPEs in flexible batteries. Benefiting from the interface-less design, outstanding mechanical flexibility and stability is achieved in the battery, which can endure various deformations with a low-capacity loss (< ≈10%). This study signifies a significant development on solid flexible lithium ion batteries with enhanced performance, stability, and reliability by investigating the miscibility of polymer blends, benefiting for the design of high-performance SPEs.     

Pre-Activation of CO2 at Cobalt Phthalocyanine-Mg(OH)2 Interface for Enhanced Turnover Rate

Cobalt phthalocyanine (CoPc) anchored on heterogeneous scaffold has drawn great attention as promising electrocatalyst for carbon dioxide reduction reaction (CO₂RR), but the molecule/substrate interaction is still pending for clarification and optimization to maximize the reaction kinetics. Herein, a CO₂RR catalyst is fabricated by affixing CoPc onto the Mg(OH)₂ substrate primed with conductive carbon, demonstrating an ultra-low overpotential of 0.31 ± 0.03 V at 100 mA cm⁻² and high faradaic efficiency of >95% at a wide current density range for CO production, as well as a heavy-duty operation at 100 mA cm⁻² for more than 50 h in a membrane electrode assembly. Mechanistic investigations employing in situ Raman and attenuated total reflection surface-enhanced infrared absorption spectroscopy unravel that Mg(OH)₂ plays a pivotal role to enhance the CO₂RR kinetics by facilitating the first-step electron transfer to form anionic *CO₂⁻ intermediates. DFT calculations further elucidate that introducing Lewis acid sites help to polarize CO₂ molecules absorbed at the metal centers of CoPc and consequently lower the activation barrier. This work signifies the tailoring of catalyst-support interface at molecular level for enhancing the turnover rate of CO₂RR.     

Freely Tailorable Yolk-Shell Encapsulation: Versatile Applications in Ultralow-k Dielectric,Drug Delivery Systems,and Catalysts

Herein, a facile, controllable, and versatile method is reported to prepare monodisperse yolk-shell and yolk-multishell silica nanoparticles (NPs) with mesoporous shells by a novel selective etching strategy. The mechanism of selective etching based on fluoride-silica chemistry is investigated in detail and thus provides a fundamentally novel principle for the fabrication of yolk-shell NPs. Specifically, this unprecedented and versatile synthesis strategy can be used to encapsulate essentially any silica-based, carbon-based, metal, metal oxide, or other possible NPs. Noteworthy is that most of the yolk-shell mesoporous silica (mSiO₂) NPs are prepared for the first time. To demonstrate the major structural and compositional advantages of the designed yolk-shell NPs, their applications in the fields of ultralow-dielectric constant (k) materials, drug delivery systems, and catalysts were explored. In detail, the lowest k value of the prepared yolk-shellordered mesoporous silica@mSiO₂/fluorinated polybenzoxazole composite films is 2.02; The obtained yolk-shell mSiO₂/C@mSiO₂/C NPs possess high hydrophilicity and pH-responsive sensitivity; The conversion of the catalytic reaction of the designed magnetic yolk-shell hollow Fe₃O₄@SiO₂/Au@mSiO₂ NPs at 20 min is 97% with a high conversion rate (92%) and recyclability even after 10 reuses. This innovative work lays a solid foundation for freely tailorable yolk-shell encapsulation and will greatly stimulate more efforts devoted to relevant research and development.