Covalent organic frameworks (COFs) have gained considerable attention due to their design possibilities as the molecular organic building blocks that can stack in an atomically precise spatial arrangement. Since the inception of COFs in 2005, there has been a continuous expansion in the product range of COFs and their derivatives. This expansion has led to the evolution of three-dimensional structures and various synthetic routes, propelling the field towards large-scale preparation of COFs and their derivatives. This review will offer a holistic analysis and comparison of the spatial structure and synthesis techniques of COFs and their derivatives. The conventional methods of COF synthesis (i.e., ultrasonic chemical, microwave, and solvothermal) are discussed alongside the synthesis strategies of new COFs and their derivatives. Furthermore, the applications of COFs and their derived materials are demonstrated in air, water, and soil pollution management such as gas capture, catalytic conversion, adsorption, and pollutant removal. Finally, this review highlights the current challenges and prospects for large-scale preparation and application of new COFs and the derived materials. In line with the United Nations Sustainable Development Goals (SDGs) and the needs of digital-enabled technologies (AI and machine learning), this review will encompass the future technical trends for COFs in environmental pollution control.

Ammonia borane (AB), a liquid hydrogen storage material, has attracted increasing attention for hydrogen utilization because of its high hydrogen content. However, the slow kinetics of AB hydrolysis and the indefinite catalytic mechanism remain significant problems for its large‐scale practical application. Thus, the development of efficient AB hydrolysis catalysts and the determination of their catalytic mechanisms are significant and urgent. A summary of the preparation process and structural characteristics of various supported catalysts is presented in this paper, including graphite, metal‐organic frameworks (MOFs), metal oxides, carbon nitride (CN), molybdenum carbide (MoC), carbon nanotubes (CNTs), boron nitride (h‐BN), zeolites, carbon dots (CDs), and metal carbide and nitride (MXene). In addition, the relationship between the electronic structure and catalytic performance is discussed to ascertain the actual active sites in the catalytic process. The mechanism of AB hydrolysis catalysis is systematically discussed, and possible catalytic paths are summarized to provide theoretical considerations for the designing of efficient AB hydrolysis catalysts. Furthermore, three methods for stimulating AB from dehydrogenation by‐products and the design of possible hydrogen product‐regeneration systems are summarized. Finally, the remaining challenges and future research directions for the effective development of AB catalysts are discussed.

The structural reconstruction mechanism of lignin and cellulose-derived biochars during direct graphitization under ultra-high temperatures was intensively investigated. It was demonstrated that cellulose-derived char was almost composed of carbon microcrystallites, whereas lignin-derived char reserved some of its skeleton structures, and such structural difference played a vital role in the morphology of formed graphitic layers. The results illustrated that the graphitized lignin-derived sample under 2800 ℃ had graphitic degree of 89.53%, interlayer spacing of 0.3363 nm and electronic conductivity of 104.6 S cm⁻¹, while cellulose-derived sample had graphitic degree of 76.74%, layer distance of 0.3374 nm, and electronic conductivity of only 48.8 S cm⁻¹. Combined with the results of structural analysis of the chars derived from lignin and cellulose, it was inferred that the stable and aromatic ring containing skeleton structure in lignin was beneficial to the ring-enlarging reconstruction and the formation of large areas of continuous graphitic layers during graphitizing process, leading to high electronic conductivity. Meanwhile, the interwoven microcrystallites in cellulose-derived char strongly restricted the expanding of continuous lamellar graphitic areas even at such ultra-high temperature, causing the formation of turbostratic structure with numerous structural defects as well, and finally resulting in relatively lower electronic conductivity. This work is expected to provide theoretical guidance for preparing high-performance functional carbon materials from lignocellulosic biomass. Graphical Abstract

Carbon nanomaterials show outstanding promise as electrocatalysts for hydrogen peroxide (H₂O₂) synthesis via the two-electron oxygen reduction reaction. However, carbon-based electrocatalysts that are capable of generating H₂O₂ at industrial-level current densities (>300 mA cm⁻²) with high selectivity and long-term stability remain to be discovered. Herein, few-layer boron nanosheets are in-situ introduced into a porous carbon matrix, creating a metal-free electrocatalyst (B_n-C) with H₂O₂ production rates of industrial relevance in neutral or alkaline media. B_n-C maintained > 95% Faradaic efficiency during a 140-hour test at 300 mA cm⁻² and 0.1 V vs. RHE, and delivered a mass activity of 25.1 mol g_catalyst⁻¹ h⁻¹ in 1.0 M Na₂SO₄ using a flow cell. Theoretical simulations and experimental studies demonstrate that the superior catalytic performance originates from B atoms with adsorbed O atoms in the boron nanosheets. B_n-C outperforms all metal-based and metal-free carbon catalysts reported to date for H₂O₂ synthesis at industrial-level current densities.

Activated carbon (AC) with a very high surface area of over 2000 m²/g was produced from low sulfur acid hydrotropic lignin (AHL) from poplar wood using H₃PO₄ at a moderate temperature of 450 °C (AHL-AC6). ACs with similar surface areas were also obtained under the same activation condition from commercial hardwood alkali lignin and lignosulfonate. Initial evaluation of AC performance was carried out using nitrogen adsorption-desorption and dye adsorption. AHL-AC6 exhibited the best specific surface area and dye adsorption performance. Furthermore, the adsorption results of congo red (CR) and methylene blue (MB) showed AHL-AC6 had greater adsorption capacity than those reported in literature. The dye adsorption data fit to the Langmuir model well. The fitting parameter suggests the adsorption is nearly strong and near irreversible, especially for MB. The present study for the first time provided a procedure for producing AC from lignin with Brunauer–Emmett–Teller (BET) surface area >2000 m²/g using low cost and low environmental impact H₃PO₄ at moderate temperatures.