Long-Lifespan 522 Wh kg Lithium Metal Pouch Cell Enabled by Compound Additives Engineering.

Matching high-voltage cathodes with lithium metal anodes represents the most viable technological approach for developing secondary batteries with ultra-high energy density exceeding 500 Wh kg. Nevertheless, the instability of electrolyte/electrode interface film and commercial electrolytes with cut-off voltage above 4.3 V is still a major concern.

Practicable Zn metal batteries enabled by ultrastable ferromagnetic interface.

Rechargeable zinc (Zn) metal batteries (RZMBs) are demonstrated as sustainable and low-cost alternative in the energy storage industry of the future. However, the elusive Zn deposition behavior and water-originated parasitic reactions bring significant challenges to the fabrication and commercialization of Zn anodes, especially under high plating/stripping capacity. In this work, the ferromagnetic interface in conjunction with the magnetic field (MF) to effectively address these fabrication hurdles is proposed.

Multi-Scale Computer-Aided Design of Covalent Organic Frameworks for CO Capture in Wet Flue Gas.

Discovery of remarkable porous materials for CO capture from wet flue gas is of great significance to reduce the CO emissions, but elucidating the most critical structure features for boosting CO capture capabilities remains a great challenge. Here, machine-learning-assisted Monte Carlo computational screening on 516 experimental covalent organic frameworks (COFs) identifies the superior secondary building units (SBUs) for wet flue gas separation using COFs, which are tetraphenylporphyrin units for boosting CO adsorption uptake and functional groups for boosting CO/N selectivity. Accordingly, 1233 COFs are assembled using the identified superior SBUs.

Telluride Nanocrystals with Adjustable Amorphous Shell Thickness and Core-Shell Structure Modulation by Aqueous Cation Exchange.

Engineering the structure of core-shell colloidal semiconductor nanoparticles (CSNPs) is attractive due to the potential to enhance photo-induced charge transfer and induce favorable optical and electronic properties. Nonetheless, the sensitivity of telluride CSNPs to high temperatures makes it challenging to precisely modulate their surface crystallinity. Herein, we have developed an efficient strategy for synthesizing telluride CSNPs with thin amorphous shells using aqueous cation exchange (ACE).

POSS and imidazolium-constructed ionic porous hypercrosslinked polymers with multiple active sites for synergistic catalytic CO transformation.

In this work, we reported a facile one-pot approach to construct polyhedral oligomeric silsesquioxane (POSS) and imidazolium-based ionic porous hypercrosslinked polymers (denoted as iPHCPs) with multiple active sites towards efficient catalytic conversion of carbon dioxide (CO) to high value-added cyclic carbonates. The targeted iPHCPs were synthesized from a rigid molecular building block octavinylsilsesquioxane (VPOSS) and a newly-designed phenyl-based imidazolium ionic crosslinker through the AlCl-catalyzed Friedel-Crafts reaction. The desired multiple active sites come from the mixed anions including free Cl and Br anions, and in situ formed Lewis acidic metal-halogen complex anions [AlClBr] within imidazolium moieties and POSS-derived Si-OH groups during the synthetic process.

Carbon/Sulfur Aerogel with Adequate Mesoporous Channels as Robust Polysulfide Confinement Matrix for Highly Stable Lithium-Sulfur Battery.

The ability to restrict the shuttle of lithium polysulfide (LiPS) and improve the utilization efficiency of sulfur represents an important endeavor toward practical application of lithium-sulfur (Li-S) batteries. Herein, we report the crafting of a robust 3D graphene-wrapped, nitrogen-doped, highly mesoporous carbon/sulfur (G-NHMC/S) hierarchical aerogel as an effective polysulfide confinement matrix for a highly stable Li-S battery. Rich polar sites of NHMC firmly anchor LiPS on the matrix surface.

Metalated-bipyridine-based porous hybrid polymers with POSS-derived Si-OH groups for synergistic catalytic CO fixation.

Herein, we construct a new series of N-heterocyclic ligand bipyridine-based porous hybrid polymers (denoted Bpy-PHPs) from the Heck reaction of a rigid building unit octavinylsilsesquioxane (VPOSS) and 5,5'-dibromo-2,2'-bipyridine. Surprisingly, the typical sample Bpy-PHP-4 was found to be a metal-/halogen-free heterogeneous catalyst in the cycloaddition reaction of CO2 with a few epoxides under atmospheric pressure. After coordination with ZnBr2, the resultant ZnBr2@Bpy-PHP-4 afforded largely enhanced heterogeneous catalytic activities upon the conversion of carbon dioxide (CO2) and various epoxides into cyclic carbonates without using any co-catalysts under mild conditions.

An easy way to identify high performing covalent organic frameworks for hydrogen storage.

The complexity of secondary building units (SBUs), an indicator that can not only be calculated but also visually estimated, is proposed as a highly indicative predictor of hydrogen storage performance. With optimal pore sizes and void fractions, selecting COFs consisting of simple SBUs greatly improves the probability of top-performing COFs towards the ultimate DOE hydrogen storage target, as an easy principle for experimentalists to select hydrogen adsorbents.

Two-in-one: construction of hydroxyl and imidazolium-bifunctionalized ionic networks in one-pot toward synergistic catalytic CO fixation.

A succinct strategy was demonstrated for constructing a hydroxyl group and imidazolium-bifunctionalized ionic network via a one-pot quaternization. Key to success lies in the rational design of multi-imidazole precursor and hydroxyl-containing counterpart. Unique properties of the resultant ionic network render its high catalytic efficiency toward CO2 fixation under ambient conditions.

Ultrathin Two-Dimensional Membranes Assembled by Ionic Covalent Organic Nanosheets with Reduced Apertures for Gas Separation.

Covalent organic frameworks (COFs) are a promising category of porous materials possessing extensive chemical tunability, high porosity, ordered arrangements at a molecular level, and considerable chemical stability. Despite these advantages, the application of COFs as membrane materials for gas separation is limited by their relatively large pore apertures (typically >0.5 nm), which exceed the sieving requirements for most gases whose kinetic diameters are less than 0.

Facile synthesis of crystalline viologen-based porous ionic polymers with hydrogen-bonded water for efficient catalytic CO fixation under ambient conditions.

In this work, we report a series of crystalline viologen-based porous ionic polymers (denoted VIP-X, X = Cl or Br), that have formed dicationic viologens paired with halogen anions and intrinsic hydrogen-bonded water molecules, towards metal-free heterogeneous catalytic conversion of carbon dioxide (CO) under mild conditions. The targeted VIP-X materials were facilely constructed the Menshutkin reaction of 4,4'-bipyridine with 4,4'-bis(bromomethyl)biphenyl (BCBMP) or 4,4'-bis(chloromethyl)biphenyl (BBMBP) monomers. Their crystalline and porous structures, morphological features and chemical structures and compositions were fully characterized by various advanced techniques.

Materials genomics methods for high-throughput construction of COFs and targeted synthesis.

Materials genomics represents a research mode for materials development, for which reliable methods for efficient materials construction are essential. Here we present a methodology for high-throughput construction of covalent organic frameworks (COFs) based on materials genomics strategy, in which a gene partition method of genetic structural units (GSUs) with reactive sites and quasi-reactive assembly algorithms (QReaxAA) for structure generation were proposed by mimicking the natural growth processes of COFs, leading to a library of 130 GSUs and a database of ~470,000 materials containing structures with 10 unreported topologies as well as the existing COFs. As a proof-of-concept example, two generated 3D-COFs with ffc topology and two 2D-COFs with existing topologies were successfully synthesized.

Constructing POSS and viologen-linked porous cationic frameworks induced by the Zincke reaction for efficient CO capture and conversion.

POSS and viologen-linked porous cationic frameworks (V-PCIF-X, X = Cl, Br) are constructed via the Zincke reaction between octa(aminophenyl)silsesquioxane and viologen linkers. The typical V-PCIF-Br has a high surface area with abundant ionic sites, micro-/mesopores and Si-OH groups, serving as an efficient porous adsorbent and metal-free catalyst for simultaneous CO2 capture and conversion.

An in situ self-assembly template strategy for the preparation of hierarchical-pore metal-organic frameworks.

Metal-organic frameworks (MOFs) have recently emerged as a new type of nanoporous materials with tailorable structures and functions. Usually, MOFs have uniform pores smaller than 2 nm in size, limiting their practical applications in some cases. Although a few approaches have been adopted to prepare MOFs with larger pores, it is still challenging to synthesize hierarchical-pore MOFs (H-MOFs) with high structural controllability and good stability.

Effect of central metal ions of analogous metal-organic frameworks on adsorption of organoarsenic compounds from water: plausible mechanism of adsorption and water purification.

The adsorptive removal of organoarsenic compounds such as p-arsanilic acid (ASA) and roxarsone (ROX) from water using metal-organic frameworks (MOFs) has been investigated for the first time. A MOF, iron benzenetricarboxylate (also called MIL-100-Fe) exhibits a much higher adsorption capacity for ASA and ROX than activated carbon, zeolite (HY), goethite, and other MOFs. The adsorption of ASA and ROX over MIL-100-Fe is also much more rapid than that over activated carbon.

Revealing the structure-property relationship of covalent organic frameworks for CO₂ capture from postcombustion gas: a multi-scale computational study.

With the aid of multi-scale computational methods, a diverse set of 46 covalent organic frameworks (COFs), covering the most typical COFs synthesized to date, were collected to study the structure-property relationship of COFs for CO2 capture. For this purpose, CO2 capture from postcombustion gas (CO2-N2 mixture) under industrial vacuum swing adsorption (VSA) conditions was considered as an example. This work shows that adsorption selectivity, CO2 working capacity and the sorbent selection parameter of COFs all exhibit strong correlation with the difference in the adsorbility of adsorbates (ΔAD), highlighting that realization of large ΔAD can be regarded as an important starting point for designing COFs with improved separation performance.