Recent advances in ordered porous materials, including metal‐organic (MOF) and covalent organic frameworks (COF), are set to revolutionize the strategies used for wastewater treatment. This is attributed to the large surface area, high crystallinity, structural tunability, thermal and chemical stability, and well‐defined structures of MOF and COF. Despite the distinctive properties exhibited by the single system (either MOF or COF), the combination of COF and MOF, as a hybrid construct, offers a remarkable opportunity to achieve superior functionality and performance. The favorable features of COF–MOF hybrids in different wastewater treatment sectors have opened new venues for effective environmental remediation. This review presents the state‐of‐the‐art design, synthesis, and application of COF–MOF hybrids. The synthesis principles, including MOF‐first, COF‐first, and post‐synthetic linkage of pre‐synthesized COFs and MOFs are summarized. The potential of these novel materials is evaluated by considering contaminant sensing, adsorptive removal, and catalytic photodegradation.The conclusion is drawn by assessing the existing hurdles and potential opportunities in the development of COF‐MOF hybrids as an innovative yet viable approach for addressing wastewater treatment.

COF and MOF Hybrids: Advanced Materials for Wastewater Treatment

Herein, we designed an on-site and portable colorimetric assay using cellulose acetate polymeric films incorporated with HKUST-1 metal-organic framework while immersed in a solution of methyl red and brilliant cresyl blue organic dyes as an indicator for monitoring ammonia levels. Ammonia serves as a significant biomarker of food spoilage which falls under the category of volatile organic compounds (VOCs). The designed colorimetric solid-state sensor was comprehensively characterized using FE-SEM, EDS-mapping, XRD, FTIR, and contact angle analyses. The results confirmed the superior stability, water permeability, good crystallinity and desirable morphology of the prepared sensor platform. Additionally, customized smartphone was developed and applied for online signaling and colorimetric analysis. The findings demonstrated two linear ranges: 1–100 ppb and 0.1–1340 ppm with a detection limit of 0.02 ppm. The solid-state sensor exhibited high selectivity in the presence of other VOCs such as methanol, ethanol, acetone, 2-propanol, toluene, humidity, and hexane. It displayed acceptable repeatability in both inter-day (RSD = 3.38 %) and intraday (RSD = 3.86 %), long-term stability over 4 days as well as reusability over 3 cycles. We successfully applied this sensing platform for ammonia monitoring in spoiled meat foods including veal, fish and chicken. The results indicated favorable percentage recovery and repeatability, confirming the feasibility and potential applicability of this intelligent packaging system for monitoring freshness. The platform allows for real-time monitoring and data analysis via smartphone-based online signaling, providing a convenient and effective method for ensuring food quality. 

Cellulose acetate/MOF film-based colorimetric ammonia sensor for non-destructive remote monitoring of meat product spoilage.

Abstract Core–shell structures, where the “guest” material is encapsulated within a protective shell, integrate the advantages of different materials to enhance the overall properties of the composite. Covalent–organic frameworks (COFs) are favorable candidates for composing core–shell structures due to their inherent porosity, good activity, excellent stability, and other advantages. In particular, COFs as shells to encapsulate other functional materials are becoming increasingly popular in the fields of environmental remediation and energy conversion. However, there is a lack of reviews on COF‐based core–shell materials. In this context, this review provides a systematic summary of the current research on COF‐based core–shell composites. First, a simple classification is made for COF‐based core–shell composites. The second part of the review describes the main synthesis methods. The changes brought about by the COF shell and core–shell structures on the properties of the composites and their applications in photocatalysis, electrocatalysis, adsorption, sensing, and supercapacitors are then emphasized. Finally, new perspectives on the future development and challenges of composites are presented. The purpose of this study is to provide future insights into the design and application of COF‐based core–shell composites. 

Covalent–Organic Framework (COF)‐Core–Shell Composites: Classification, Synthesis, Properties, and Applications

Biotic and abiotic stresses are well known to increase the emission of volatile organic compounds (VOCs) from plants. The analysis of VOCs emissions from plants enables timely diagnostic of plant diseases, which is critical for prompting sustainable agriculture. Previous studies have predominantly focused on the utilization of commercially available devices, such as electronic noses, for diagnosing plant diseases. However, recent advancements in nanomaterials research have significantly contributed to the development of novel VOCs sensors featuring exceptional sensitivity and selectivity. This comprehensive review presents a systematic analysis of VOCs monitoring technologies for plant diseases diagnosis, providing insights into their distinct advantages and limitations. Special emphasis is placed on custom-made VOCs sensors, with detailed discussions on their design, working principles, and detection performance. It is noteworthy that the application of VOCs monitoring technologies in the diagnostic process of plant diseases is still in its emerging stage, and several critical challenges demand attention and improvement. Specifically, the identification of specific stress factors using a single VOC sensor remains a formidable task, while environmental factors like humidity can potentially interfere with sensor readings, leading to inaccuracies. Future advancements should primarily focus on addressing these challenges to enhance the overall efficacy and reliability of VOCs monitoring technologies in the field of plant disease diagnosis. 

Challenges and applications of volatile organic compounds monitoring technology in plant disease diagnosis.

Due to the large specific surface area and continuous pores in structures, metal-organic frameworks (MOFs) show great advantages in the adsorption of volatile organic compounds (VOCs). Photonic crystal (PC) sensors derived from MOFs are promising for the visual detection of VOC gases. However, they still have problems of low sensitivity and poor color saturation and tunability. Here, inspired by vapor-sensitive scales of Tmesisternus isabellae beetle and scattering light absorption of polydopamine, a porous one-dimensional PC sensor is constructed by combining ZIF-8 with TiO2@PDA nanoparticles. The PC sensor shows significant color changes under different concentrations of benzene vapor and reaches a detection limit of 0.8 g/m3. It has a response time of less than 1 s and maintains stable optical performance after 100 times of reuse. Moreover, ZIF-67 and ZIF-7 are both incorporated into the PCs for comparison; it reveals that ZIF-8 shows superior benzene detecting property. Additionally, the synergistic adsorption of VOCs in inner and outer holes of the ZIF-8 layer is demonstrated by real-time mass monitoring with quartz crystal microbalance with dissipation. This study provides a valuable reference for the fabrication of high-quality MOF-based PC sensors and sensing mechanism study between microscopic molecular adsorption and macroscopic performance.

Biomimetic Metal-Organic Framework-Based Photonic Crystal Sensor for Highly Sensitive Visual Detection and Effective Discrimination of Benzene Vapor.

As a class of important artificial olfactory system, the colorimetric sensor array possesses great potential for commercialization due to its cost-effectiveness and portability. However, when applied to practical applications, the humidity interference from ambient environment and dissatisfactory sensitivity for trace target VOCs are largely unsolved problems. To overcome the problems, we developed a series of dye/MOFs@COFs gas-sensing materials with core-shell structure using a hydrophobization strategy by encapsulation of dye/metal-organic frameworks (MOFs) into hydrophobic covalent organic frameworks (COFs). Benefiting from the hydrophobic property of the COF shell, the dye/MOFs@COFs composites were endowed with excellent humidity-resistance even under 100% relative humidity (RH). Moreover, due to the uniform distribution of dyes on the porous MOFs, the dye/MOFs@COFs sensors also exhibited improved sensitivity at the sub-ppm level, compared with conventional dye sensors. On basis of the excellent humidity-resistance and improved sensitivity, an artificial olfactory array based on dye/MOFs@COFs composites was proven to be a successful practical application in early and accurate detection of wheat scab (1 day after inoculation) by monitoring its released VOC markers. The synthetic strategy for core-shell dye/MOFs@COFs is applicable to a wide range of colorimetric sensor arrays, endowing them with excellent humidity-resistance and sensitivity for the feasibility of practical applications.

Humidity-Independent Artificial Olfactory Array Enabled by Hydrophobic Core-Shell Dye/MOFs@COFs Composites for Plant Disease Diagnosis.

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Humidity-Independent Artificial Olfactory Array Enabled by Hydrophobic Core-Shell Dye/MOFs@COFs Composites for Plant Disease Diagnosis.