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Purposefully designing the well-defined catalysts for the selective electroreduction of CO2 to C2 H4 is an extremely important but challenging work. In this work, three crystalline trinuclear copper clusters (Cu3 -X, X=Cl- , Br- , NO3- ) have been designed, containing three active Cu sites with the identical coordination environment and appropriate spatial distance, delivering high selectivity for the electrocatalytic reduction of CO2 to C2 H4 . The highest faradaic efficiency of Cu3 -X for CO2 -to-C2 H4 conversion can be adjusted from 31.90 % to 55.01 % by simply replacing the counter anions (NO3- , Cl- , Br- ). The DFT calculation results verify that Cu3 -X can facilitate the C-C coupling of identical *CHO intermediates, subsequently forming molecular symmetrical C2 H4 product. This work provides an important molecular model system and a new design perspective for electroreduction of CO2 to C2 products with symmetrical molecular structure.

The exploration of novel systems for the electrochemical CO2 reduction reaction (CO2 RR) for the production of hydrocarbons like CH4 remains a giant challenge. Well-designed electrocatalysts with advantages like proton generation/transferring and intermediate-fixating for efficient CO2 RR are much preferred yet largely unexplored. In this work, a kind of Cu-porphyrin-based large-scale (≈1.5 μm) and ultrathin nanosheet (≈5 nm) has been successfully applied in electrochemical CO2 RR. It exhibits a superior FE CH 4 of 70 % with a high current density (-183.0 mA cm-2 ) at -1.6 V under rarely reported neutral conditions and maintains FE CH 4 >51 % over a wide potential range (-1.5 to -1.7 V) in a flow cell. The high performance can be attributed to the construction of numerous hydrogen-bonding networks through the integration of diaminotriazine with Cu-porphyrin, which is beneficial for proton migration and intermediate stabilization, as supported by DFT calculations. This work paves a new way in exploring hydrogen-bonding-based materials as efficient CO2 RR catalysts.

Multidimensional fabrication of metal-organic frameworks (MOFs) into multilevel channel integrated devices are in high demanded for Li-S separators. Such separators have advantages in pore-engineering that might fulfill requirements such as intercepting the diffusing polysulfides and improving the Li+ /electrolyte transfer in Li-S batteries. However, most reported works focus on the roles of MOFs as ionic sieves for polysulfides while offering limited investigation on the tuning of Li+ transfer across the separators. A photoinduced heat-assisted processing strategy is proposed to fabricate MOFs into multidimensional devices (e.g., hollow/Janus fibers, double-or triple-layer membranes). For the first time, a triple-layer separator with stepped-channels has been designed and demonstrated as a powerful separator with outstanding specific capacity (1365.0 mAh g-1 ) and cycling performance (0.03 % fading per cycle from 100th to 700th cycle), which is superior to single/double-layer and commercial separators. The findings may expedite the development of MOF-based membranes and extend the scope of MOFs in energy-storage technologies.

Summary γ-butyrolactone (γ-BL), serving as the monomer of biocompatible and recyclable poly(γ-butyrolactone) plastic, faces a giant challenge in ring-opening polymerization (ROP) due to its low strain energy. The ROP of γ-BL is generally achieved under harsh conditions (e.g., high-pressure or gas-protected atmosphere) and is mostly based on homogeneous systems. Here, we synthesize a series of lanthanum metal-organic framework-based porous nanospheres and successfully apply them as heterogeneous catalysts in efficient ROP of γ-BL under mild conditions. Specifically, NNU-mIM-3 presents a yield of 24.6% with low polydispersity distribution centered at 3.6 kDa and the obtained PγBL can be completely and quantitatively recycled into monomers by simple heat treatment. Besides, the ROP catalysis systems have been intensively explored with various imine-based additives, proven to exhibit largely improved performance with PγBL yield of ~50% and Mw of ~8 kDa. This work paves a new way to explore novel heterogeneous catalysts in producing biocompatible and degradable plastics.

Electrochemical CO2 reduction reaction (CO2RR) to formate is economically viable considering the energy input and market value. Through learning nature, a series of chloroplast-like porous bismuth-based core–shell (CPBC) materials have been designed. In these materials, the porous carbon can enrich and transfer CO2 to the core–shell Bi@Bi2O3 in CO2 reduction process, during which Bi2O3 layer can be transformed into activated metastable layer to efficiently convert CO2 into formate and Bi can provide abundant electrons. Based on this, superior performances for most of important parameters in CO2RR can be achieved and best of them, CPBC-1 presents remarkable Faradaic efficiency (FEformate > 94%) over a wide potential range (−0.65 to −1.0 V) with high catalysis durability (>72 h). Noteworthy, its maximum energy efficiency is as high as 76.7% at −0.7 V, the highest one in reported bismuth-based materials. This work opens novel perspectives in designing nature-inspired CO2RR electrocatalysts.

Purposefully designing the well-defined catalysts for the selective electroreduction of CO

Microplastics are a worldwide problem that poses a giant threat to organisms in the ecosystem and even to human health. The removal of microplastics is a severe challenge that needs to be solved urgently. Herein, a series of zirconium metal–organic framework-based foam materials with interpenetrated pores, high MOF uniformity and excellent durability have been successfully fabricated and applied in simulated microplastics removal in water or seawater conditions. They can be applied to various types and concentrations of microplastics suspensions. It is worth noting that the best of them, UiO-66-OH@MF-3, can efficiently remove microplastics with an efficiency of up to 95.5 ± 1.2% and can maintain high performance in recycling and large-quantity filtration experiments. Besides, we proposed an automatic filtration system powered by sunlight and accomplished it on the lab-scale. The high performances of these foam materials combined with the new concept of automatic filtration systems might shed some light on the development of novel techniques for microplastics removal.

Polyester plastics such as poly(ethylene terephthalate) (PET) are utilized commonly in everyday life, yet only a small portion of these plastics are recycled, and typically, the recycling procedure...

The exploration of novel systems for the electrochemical CO

Metal–organic framework (MOF) based mixed matrix membranes (MMMs) have received significant attention in applications such as gas separation, sensing, and energy storage. However, the mass production of MOF‐based MMMs with retained porosity remains a longstanding challenge. Herein, an in situ heat‐assisted solvent‐evaporation method is described to facilely produce MOF‐based MMMs. This method can be extended into various MOFs and polymers with minimum reaction time of 5 min. Thus‐obtained MMMs with high uniformity, excellent robustness, well‐tuned loading, and thickness can be massively produced in industrial‐level efficiency (≈4 m in a batch experiment). Furthermore, they can be readily applied as powerful separators for Li–S cell with high specific capacity (1163.7 mAh g−1) and a capacity retention of 500.7 mAh g−1 after 700 cycles at 0.5 C (0.08% fading per cycle). This work may overcome the longstanding challenge of processing MOFs into MMMs and largely facilitate the industrialization process of MOFs., An in situ heat‐assisted solvent‐evaporation method is developed to facilely fabricate porous and robust metal–organic framework‐based mixed matrix membranes (MMMs). The obtained MMMs with high uniformity, excellent robustness, well‐tuned loading, and thickness can be massively produced (≈4 m in a batch experiment in lab scale) and exhibit high performances in separators for Li–S battery.