Porous crystalline materials usually include metal-organic frameworks (MOFs), covalent organic frameworks (COFs), hydrogen-bonded organic frameworks (HOFs) and zeolites, which exhibit exceptional porosity and structural/composition designability, promoting the increasing attention in memory and neuromorphic computing systems in the last decade. From both the perspective of materials and devices, it is crucial to provide a comprehensive and timely summary of the applications of porous crystalline materials in memory and neuromorphic computing systems to guide future research endeavors. Moreover, the utilization of porous crystalline materials in electronics necessitates a shift from powder synthesis to high-quality film preparation to ensure high device performance. This review highlights the strategies for preparing porous crystalline materials films and discusses their advancements in memory and neuromorphic electronics. It also provides a detailed comparative analysis and presents the existing challenges and future research directions, which can attract the experts from various fields (e.g., materials scientists, chemists, and engineers) with the aim of promoting the applications of porous crystalline materials in memory and neuromorphic computing systems. 

Porous crystalline materials for memories and neuromorphic computing systems.

Covalent organic framework (COF) membranes featuring uniform topological structures and devisable functions, show huge potential in water purification and molecular separation. Nevertheless, the inability of uniform COF membranes to be produced on an industrial scale and their nonenvironmentally friendly fabrication method are the bottleneck preventing their industrial applications. Herein, we report a new green and industrially adaptable scraping-assisted interfacial polymerization (SAIP) technique to fabricate scalable and uniform TpPa COF membranes. The process used non-toxic and low-volatility ionic liquids (ILs) as organic phase instead of conventional organic solvents for interfacial synthesis of TpPa COF layer on a support membrane, which can simultaneously achieve the purposes of (i) improving the greenness of membrane-forming process and (ii) fabricating a robust membrane that can function beyond the conventional membranes. This approach yields a large-area, continuous COF membrane (19×25 cm2 ) with a thickness of 78 nm within a brief period of 2 minutes. The resulting membrane exhibited an unprecedented combination of high permeance (48.09 L m-2 h-1 bar-1 ) and antibiotic desalination efficiency (e.g., NaCl/adriamycin separation factor of 41.8), which is superior to the commercial benchmarking membranes. 

Membranes based on Covalent Organic Frameworks through Green and Scalable Interfacial Polymerization using Ionic Liquids for Antibiotic Desalination.

Facile construction of multifunctional 3D smart MOF-based polyurethane sponges with photocatalytic ability for efficient separation of oil-in-water emulsions and co-existing organic pollutant

Covalent organic frameworks (COFs) are a new kind of crystalline porous materials composed of organic molecules connected by covalent bonds, processes the characteristics of low density, large specific surface area, adjustable pore size and structure, and easy to functionalize, which have been widely used in the field of membrane separation technology. Recently, there are more and more researches focusing on the preparation methods, separation application, and mechanism of COF membranes, which need to be further summarized and compared. In this review, we primarily summarized several conventional preparation methods, such as two-phase interfacial polymerization, in-situ growth on substrate, unidirectional diffusion method, layer-by-layer assembly method, mixed matrix membranes, and so on. The advantages and disadvantages of each method are briefly summarized. The application potential of COF membrane in liquid separation are introduced from four aspects: dyeing wastewater treatment, heavy metal removal, seawater desalination and oil-water separation. Then, the mechanisms including pore structure, hydrophilic/hydrophobic, electrostatic repulsion/attraction and Donnan effect are introduced. For the efficient removal of different kind of pollutions, researchers can select different ligands to construct membranes with specific pore size, hydrophily, salt or organic rejection ability and functional group. The ideas for the design and preparation of COF membranes are introduced. Finally, the future direction and challenges of the next generation of COF membranes in the field of separation are prospected.

COF-based membranes for liquid phase separation: Preparation, mechanism and perspective

Crystalline porous materials (CPMs), including covalent organic frameworks (COFs) and metal–organic frameworks (MOFs), are promising materials for advanced separation technologies. However, the challenge of transforming nanoscale CPMs into large‐area functional membranes hinders their application in the membrane separation process. Herein, a self‐standing pure COF (TpPa‐1) nanofiber membrane with high crystallinity, good flexibility, excellent mechanical properties, and scalability is prepared using an electrospinning process and polymer sacrificial template strategy. Subsequently, the COF nanofiber membrane is innovatively used to replace traditional inorganic discs, metal meshes, and polymer membranes as porous supports, and the COF–MOF composite CPM membrane is prepared through the tailorable and confined growth of zeolite imidazolium salt frame‐8 (ZIF‐8) on the surface of the COF membrane and in the gaps of the COF nanofibers. The COF–MOF composite membrane exhibits excellent permeability and significantly enhances separation selectivity for organic dyes. Moreover, MOF and COF form an interpenetrating network structure, and their similar chemical properties improve the interfacial stability between the two phases, giving the COF–MOF composite membrane good long‐term separation performance. This is the first self‐standing composite CPM membrane with excellent molecular sieving performance, which provides new insights into the design of high‐performance and robust composite membranes.

Highly Flexible and Self‐Standing Covalent Organic Framework–Metal–Organic Framework (COF–MOF) Composite Crystalline Porous Material (CPM) Membrane for Molecular Separation

Smart superwetting COF membrane for controllable oil/water separation

Highly flexible and robust self‐standing covalent organic framework (COF) membranes with rapid preparation are important but technically challenging for achieving precise separation. Herein , a novel imine‐based 2D soft covalent organic framework (SCOF) membrane with a large area of 226.9 cm2, via ingeniously selecting an aldehyde flexible linker and a trigonal building block, is reported. The soft 2D covalent organic framework membrane is rapidly formed (≈5 min) based on the sodium dodecyl sulfate (SDS) molecular channel constructed at the water/dichloromethane (DCM) interface, which is the record‐fast SCOF membrane formation and 72 times faster than that in the reported literature. MD simulation and DFT calculation elucidate that the dynamic, self‐assembled SDS molecular channel facilitates faster and more homogeneous transfer of amine monomers in the bulk, thereby forming a soft 2D self‐standing COF membrane with more uniform pores. The formed SCOF membrane exhibits superb sieving capability for small molecules, robustness in strong alkaline (5 mol L−1 NaOH), acid (0.1 mol L−1 HCl), and various organic solutions, and sufficient flexibility with a large curvature of 2000 m−1 for membrane‐based separation science and technology.

A 2D Soft Covalent Organic Framework Membrane Prepared via a Molecular Bridge

Polymers of intrinsic microporosity (PIMs) are promising candidates for carbon dioxide (CO2) separation and capture from flue gas or natural gas. PIM-1, which has excellent gas permeation properties over the Robeson upper bound (1991), has been widely functionalized to further enhance the CO2 permeability or selectivity. In this work, a simple and readily processive surface modification method has been proposed via hydrolysis of the PIM-1 membrane. The two hydrolysis processes by the acid method, amidation and carboxylation processes, have been conducted to functionalize the surface of PIM-1 membranes forming NA-PIM-1 and CA-PIM-1 membranes. The TGA, FT-IR spectra and NMR results verify that the composition and structure inside the PIM-1 membrane remain unchanged. XPS and NMR spectra demonstrate that the nitrile group at the surface was successfully functionalized with an amine group or carboxyl group. The CO2 permeability and CO2/N2 selectivity of the NA-PIM-1 membrane both increased to 4593.2 Barrer and 28.5, respectively. Another advantage of NA-PIM-1 membranes is the coordination site from introduced nitrogen atoms with zinc ions to form NA-PIM-1-Zn, which could further react with PEI to introduce amine-rich groups on the surface of the PIM-1 membrane. The CO2/N2 selectivity of the NA-PIM-1-Zn-PEI membrane coated with PEI on the surface increases 45.4% compared to the unmodified PIM-1 membranes, with CO2 permeability decreasing only 15.5% compared to the unmodified PIM-1 membrane. The NA-PIM-1 and NA-PIM-1-Zn-PEI membranes both surpass the Robeson upper bound (2008) even under mixed gas feeding, suggesting that surface modification of PIM-1 is a promising approach for CO2 capture from natural gas and flue gas. 

Surface-engineered PIM-1 membranes for facile CO2 capture

Provided is a negative electrode composition for lithium secondary batteries, comprising: a core; at least one active material layer disposed on a surface of the core and undergoing a volume change upon a reaction with lithium ions; and a shell in which at least one inactive material layer having smaller volume change rate than the at least one active material layer is alternately laminated. According to the present invention, it is possible to reduce production costs while contributing to the production of high capacity negative electrode active materials.

Anode composition for lithium secondary battery and method of manufacturing the same and litium secondary battery comprising the same

The present invention provides an anode composition for a lithium secondary battery, which comprises: a core; and a shell disposed on the surface of the core and having at least one active material layer and at least one non-active material layer alternately laminated thereon, wherein the at least one active material layer changes in volume upon reaction with lithium ions and the at least one non-active material layer is smaller in volume change rate than the at least one active material layer.

Anode composition for lithium secondary battery, method for preparing same, and lithium secondary battery comprising same

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Smart superwetting COF membrane for controllable oil/water separation

A 2D Soft Covalent Organic Framework Membrane Prepared via a Molecular Bridge

Surface-engineered PIM-1 membranes for facile CO2 capture

Anode composition for lithium secondary battery and method of manufacturing the same and litium secondary battery comprising the same

Anode composition for lithium secondary battery, method for preparing same, and lithium secondary battery comprising same