Ionic Covalent Organic Framework Research Articles

Anionic covalent organic framework membranes for the removal of per- and polyfluoroalkyl substances with enhanced selectivity

Nanofiltration (NF) is an effective technology for removing per- and polyfluoroalkyl substances (PFAS), a group of emerging pollutants. However, conventional NF membranes often reject high levels of minerals, leading to low salt/PFAS selectivity. Herein, we introduce the use of continuous ionic covalent organic framework (COF) membranes as a novel approach to achieve effective PFAS removal with high selectivity. Thin TpPa-SO3H COF selective membrane layers were fabricated on polymer supports using a scalable counter-diffusion interfacial polymerization (IP) method to form thin film composite (TFC) membranes. These membranes feature a highly negative surface charge and ordered pore channels with suitable pore sizes, leading to impressive PFAS rejection rates, with over 99% rejection for perfluorooctanesulfonic acid (PFOS) and 90-95% rejection for perfluorooctanoic acid (PFOA) and two short-chain PFAS. Moreover, the TpPa-SO3H membranes allowed the passage of scale-forming salts, enabling selective PFAS removal with a high salt/PFAS selectivity. Furthermore, these continuous ionic COF membranes exhibited a high water permeance of 19.9-37.5 LMH/bar, outperforming commercial membranes like NF270 and other lab-made membranes.

Pompon mum-like ionic covalent organic framework nanocomposites for efficient solid-phase extraction of nonsteroidal anti-inflammatory drugs

Molecularly imprinted ionic covalent organic framework nanocomposites (MI-IC-COF@SnO2) were prepared as potential adsorbents for the enhanced adsorption of nonsteroidal anti-inflammatory drugs (NSAIDs) from aqueous solution. The resulting material exhibited a pompon mum-like structure, featuring a large surface area, and well-defined mesopores. The presence of uniform positive ions within the three-dimensional skeleton of MI-IC-COF@SnO2 facilitated a rapid adsorption rate and high adsorption capacity for target analytes. Thermodynamic fitting revealed the adsorption process of NSAIDs to be feasible, endothermic, and spontaneous. Additionally, the adsorbent material exhibited respectable selectivity, as evidenced by imprinting factor values ranging from 2.8 to 6.7. Utilizing MI-IC-COF@SnO2 as the sorbent, a solid-phase extraction method coupled with high-performance liquid chromatography-ultraviolet detection (SPE-HPLC-UV) was developed and optimized. The proposed method demonstrated good linear range with determination coefficients of 0.998-0.999, and low limit of detection (0.18-1.35 µg L−1). Recoveries of NSAIDs in urine and river water samples were 78.1%–106.1%, with relative standard deviations lower than 12.5%. This rapid and sensitive method enables the determination of NSAIDs at trace levels in complex matrices, providing reliable and reproducible results.

π-π+ Interaction Promoting the Absorption of Electroactive Chiral Selectors into the Cavity of Conductive Covalent Organic Framework for Enantioselective Sensing of Electrochemically Silent Molecules.

To date, achieving enantioselective electroanalysis for electrochemically silent chiral molecules is still highly desired. Here, an ionic covalent organic framework (COF) consisting of the pyridinium cation was derived from the tripyridinium Zincke salt and 1,4-phenylenediamine in a one-pot reaction. The electrochemical measurements revealed that the ionic backbone contributed to the electron transfer with a low charge transfer resistance. Besides, the π-π+ interaction between the pyridinium cation and ferrocenyl unit can promote the absorption of electroactive chiral ferrocenyl reagents into the hole of COF, so as to afford the electrochemical signals by themselves, replacing the testing enantiomers. As a result, the electroactive complex used as an electrochemical platform was highly effective at enantiomerically recognizing amino alcohols (prolinol, valinol, leucinol, and alaninol) and amino acids (methionine, serine, and penicillamine), giving the ratios of current intensity between l- and d-enantiomers in the range of 1.46-1.72. Moreover, the density functional theory calculations determined the possible intermolecular interactions between the testing enantiomers and chiral selector: namely, hydrogen bonds and electrostatic attractions. Overall, the present work offers an effective strategy to enlarge the electrochemical scope for chiral recognition based on electroactive chiral COFs.

Robust and highly proton conductive COF composite membranes for fuel cell and electrochemical hydrogen compression

Robust and highly conductive proton exchange membrane (PEM) is the unremitting pursuit of numerous electrochemical energy technologies such as fuel cell and the emerging electrochemical hydrogen compression. Ionic covalent organic framework nanosheets (iCONs) with long-range ordered nanochannels and abundant ionic groups show substantial potential as next-generation PEM materials. However, it is challenging to assemble iCONs into membranes with both robustness and flexibility due to the electrostatic repulsion and rigid framework. Herein, we propose a hydrogen-bond binding strategy to fabricate sulfonic iCON (SCON) composite membranes by co-assembling tannic acid (TA) nanoaggregates and SCONs. The abundant and dynamically reversible hydrogen-bond interactions introduced by TA nanoaggregates establish effective linkage between SCONs and allow some restricted movements, endowing membranes with remarkably improved mechanical properties. The stacked SCONs construct long-range ordered nanochannels with well-arranged sulfonic groups in membranes, and the hydrogen-bond networks further facilitate the proton transport through Grotthuss mechanism. Consequently, TA/SCON composite membranes displays significantly enhanced tensile strength of 101.9 MPa, good flexibility and high proton conductivity of 490.1 mS cm−1 at 80 °C and 100 % RH simultaneously. This hydrogen-bond binding strategy offers a promising approach to fabricate robust and highly conductive PEMs for various proton-conducting applications.

Covalent Organic Frameworks as Nano-Reservoir for Room Temperature RNA Storage.

The emerging role of Ribonucleic acids (RNAs) as therapeutics is alluring. However, RNAs are extremely labile under ambient conditions and typically need to be stored in cryogenic conditions (-20 °C to -80 °C). Hence, storage, stabilization, and transportation of RNA under ambient conditions have been an arduous task and remain an unsolved problem. In this work, a guanidinium-based ionic covalent organic framework (COF), TTGCl with nanotubular morphology, was synthesized and used as nano-reservoirs for room-temperature storage of RNA. To understand the role of the nanotubular morphology and chemical nature of TTGCl in stabilizing the RNA structure and for comparison purposes, a neutral COF, TMT-TT, is synthesized and studied. Further, density functional theory (DFT) studies confirmed non-covalent interaction between the COFs and the RNA nucleobases, facilitating reversible storage of RNA. RNA loaded in COFs was found to be resistant to enzymatic degradation when treated with RNase. Gel electrophoresis and sequencing confirmed the structural integrity of the recovered RNAs and their further processibility.

Ionic Covalent Organic Framework as a Dual Functional Sensor for Temperature and Humidity.

Visual sensing of humidity and temperature by solids plays an important role in the everyday life and in industrial processes. Due to their hydrophobic nature, most covalent organic framework (COF) sensors often exhibit poor optical response when exposed to moisture. To overcome this challenge, the optical response is set out to improve, to moisture by incorporating H-bonding ionic functionalities into the COF network. A highly sensitive COF, consisting of guanidinium and diformylpyridine linkers (TG-DFP), capable of detecting changes in temperature and moisture content is fabricated. The hydrophilic nature of the framework enables enhanced water uptake, allowing the trapped water molecules to form a large number of hydrogen bonds. Despite the presence of non-emissive building blocks, the H-bonds restrict internal bond rotation within the COF, leading to reversible fluorescence and solid-state optical hydrochromism in response to relative humidity and temperature.

Comprehensive insights into non-steroidal anti-inflammatory drugs adsorption by magnetic ionic covalent organic framework: Kinetics, isotherms, and mechanisms

Ionic covalent organic frameworks (iCOFs) have shown promise in non-steroidal anti-inflammatory drugs (NSAIDs) removal, but their recycling from solutions remains challenging. In this study, the development of a novel magnetic iCOF (M–TDiCOF) based on Schiff base reaction using amino functional group modified NH2-Fe3O4 as a magnetic source was reported. The resulting M–TDiCOF exhibits high adsorption capacity and fast kinetics, and can be easily separated and regenerated. Notably, M–TDiCOF achieves equilibrium adsorption of diclofenac sodium (DCF) within 30 min and shows a higher adsorption capacity under acidic conditions (371.27 mg/g, pH = 5). Kinetics and isotherms studies expose the adsorption of M–TDiCOF for DCF following the pseudo second-order kinetic model and Langmuir isotherm model. The correlation between the physicochemical properties of NSAIDs and the adsorption capacity of M–TDiCOF was illustrated. Moreover, the Independent gradient model based on Hirshfeld partition (IGMH) analysis revealed the interaction sites and the electrostatic potential (ESP) analysis highlighted the significance of electrostatic interactions. Finally, the adsorption mechanisms of M–TDiCOF are systematically confirmed. The abundant functional groups (guanidinium groups, hydroxyl groups, and aromatic groups) of M–TDiCOF facilitate electrostatic interactions, H-bond, π-π interactions, and ion exchange during water purification. Mung bean growth experiments verify the safety of M–TDiCOF system.

Rational design of ionic covalent organic frameworks for PPCPs elimination: Insights into ibuprofen adsorption performance and mechanism

Over the last few years, non-steroidal drugs (including ibuprofen (IBP)) have been used extensively due to the impacts of COVID-19, with the resulting environmental contamination attracting the attention of researchers. For this study, an ionic covalent organic framework (iCOF), synthesized from 1,2,4,5-tetrakis (4-formylphenyl) benzene (TFPB) and 1,3-diaminoguanidine hydrochloride (DgCl) under hydrothermal conditions, was employed for the effective elimination of non-steroidal anti-inflammatory drugs (NSAIDs) from aqueous media. COFs are relatively ordered spherical structures with excellent adsorption capacities for NSAIDs (IBP, diclofenac (DCF), and indomethacin (IDM)) with a removal rate of more than 99%. The adsorption kinetics and isotherm experiments of the COFs were investigated with IBP as a target contaminant, which revealed that its adsorption attained equilibrium within 120 min. Further, increased temperatures promoted the adsorption of IBP, where its maximum adsorption at 45 °C was calculated by the Langmuir isotherm model up to 434.78 mg·g-1. In addition, different pH, ionic influences, and repeated cycling experiments also confirmed the practical applicability of the COFs. Finally, it was demonstrated that the adsorption kinetics of IBP by TFPB-DgCl-COF could be explained by electrostatic and π-π interactions.

Exploring metal-free ionic covalent organic framework nanosheets as efficient OER electrocatalysts via cationic-π interactions

Metal-free electrocatalysts play a crucial role in enabling practical water splitting for future clean energy production by facilitating the oxygen evolution reaction (OER). However, the preparation of such electrocatalysts presents significant challenges due to the limitations of the kinetically sluggish anodic half-cell reaction, which restricts the attainment of high energy inputs. In this study, we present a metal- and pyrolysis-free ionic covalent organic framework (COF) nanosheet, denoted as JUC-627-NS, and investigate its potential as an efficient electrocatalyst for OER by introducing cationic-π interactions. Notably, through the utilization of positively charged JUC-627-NS as cationic donors and π-conjugated graphene as electron donors for the first time, the JUC-627-NS@G-2 composite exhibits an exceptional ultralow overpotential of 275 mV at a current density of 10 mA cm−2, ranking among the top-performing metal- and pyrolysis-free electrocatalysts reported thus far. Combining theoretical calculations with in-situ infrared spectroscopy, we validate that the imidazolium salt moiety of JUC-627-NS serves as the active center of the electrocatalyst, while the robust cation-π interaction within the complex brings the reaction site closer to graphene, acting as a conductive agent. These findings highlight a novel strategy for advancing the development of metal-free OER electrocatalysts based on ionic COF materials, with promising applications in energy conversion and storage devices.

Multivariate surface self-assembly strategy to fabricate ionic covalent organic framework surface grafting monolithic sorbent for enrichment of aristolochic acids prior to high performance liquid chromatography analysis

Herein, an ionic covalent organic framework (iCOF) surface grafting monolithic sorbent was prepared by the multivariate surface self-assembly strategy for in-tube solid-phase microextraction (SPME) of trace aristolochic acids (AAs) in serum, traditional Chinese medicines (TCMs) and Chinese patent drug. Via adjusting the proportion of ionic COF building block during the self-assembly, the density of quaternary ammonium ions in the iCOF was modulated for the enhanced adsorption of AAs. The successful preparation of iCOF surface grafting monolithic sorbent was confirmed by different means. A multiple mode mechanism involving π-π stacking, hydrophobic, electrostatic and hydrogen-bonding interactions was primarily attributed to the adsorption. Several in-tube SPME operating conditions, such as the dosage of ionic COF building block, ACN percentage and TFA percentage in the sampling solution, ACN percentage and TFA percentage in eluent and the collection time span, were optimized to develop the online in-tube SPME-HPLC method for analysis of AAs. Under the optimized conditions, a good linearity was obtained in the concentration range of 20–1000 ng/mL for target AAs in serum samples, the limits of detection (LODs) were less than 10 ng/mL, while the recoveries ranged from 90.3 % to 98.7 % with RSDs (n = 5) below 7.9 %. This study developed a feasible approach to iCOF functionalized monolithic sorbent for SPME and further exhibited the vast potential for the application of COF based monolithic sorbent in sample preparation.

Oriented ionic covalent organic framework membranes for efficient organic solvent nanofiltration

Developing effective organic solvent nanofiltration (OSN) membranes to separate molecular solutes from organic solvents is highly desired yet requires a suitable material platform and an in-depth investigation of membrane selectivity. Herein, an oriented ionic covalent organic framework membrane (oi-COM) was fabricated, which features well-ordered channels that are vertically aligned towards the membrane surface and lined with abundant sulfonate groups. Filtration experiments of multifarious organic solvents and solutes with different charges and molecular sizes were conducted. The oi-COM exhibited above 99% rejection for negatively charged dye (Evans blue), much higher than that for positively charged dye with similar molecular size, while maintaining high solvent permeance for ethanol of 63 L m−2 h−1 bar−1. These results demonstrated the significance of electrostatic repulsion effect in membrane selectivity, providing insights for the design of high-performance OSN membranes.

Incorporating graphene oxide into COF membranes enables ultrahigh proton conductivity and ultralow H2 crossover

Proton exchange membranes (PEMs) are the core components of electrochemical hydrogen energy production, storage and conversion devices. It is a great challenge to develop PEMs with a combination of high proton conductivity, minimal H2 crossover and mechanical robustness for achieving high efficiency and long-term stability in these devices. Here, a co-assembled PEM composed of ionic covalent organic framework (iCOF) nanosheets and functionalized graphene oxide (GO) nanosheets was presented. The iCOF (TpPa-SO3H) nanosheets and polydopamine-modified graphene oxide (DGO) nanosheets were co-assembled into TpPa-SO3H/DGO mixed nanosheets with ultrahigh aspect ratio, which were readily further processed into TpPa-SO3H/DGO co-assembled membranes. The abundant and uniformly distributed –SO3H groups on TpPa-SO3H nanosheets and the acid-base pairs formed between TpPa-SO3H and DGO nanosheets promoted proton conduction significantly. Additionally, the dense structured DGO nanosheets inhibited H2 crossover remarkably, and the multiple interactions between TpPa-SO3H and DGO nanosheets enhanced mechanical strength. The resultant TpPa-SO3H/DGO co-assembled membrane exhibited an ultrahigh proton conductivity of 916.4 mS cm−1 (80 °C, 100% RH), an unprecedently low H2 crossover of 9.7 barrer and a sufficient tensile stress of 87.8 MPa. The enhanced proton conduction and H2 barrier property led to enhanced performance in both electrochemical hydrogen compression and single hydrogen fuel cells.

3D covalent organic framework membrane with fast and selective ion transport

3D ionic covalent organic framework (COF) membranes, which are envisioned to be able to break the trade-off between ion conductivity and ion selectivity, are waiting for exploitation. Herein, we report the fabrication of a 3D sulfonic acid-functionalized COF membrane (3D SCOF) for efficient and selective ion transport, using dual acid-mediated interfacial polymerization strategy. The 3D SCOF membranes possess highly interconnected ion transport channels, ultramicroporous pore sizes (0.97 nm), and abundant sulfonate groups (with a high ion exchange capacity of 4.1 mmol g−1), leading to high proton conductivity of 843 mS cm−1 at 90 °C. When utilized in osmotic energy conversion, a high power density of 21.2 W m−2, and a remarkable selectivity of 0.976 and thus an exceptional energy conversion efficiency of 45.3% are simultaneously achieved. This work provides an alternative approach to 3D ionic COF membranes and promotes the applications of 3D COFs in ion transport and separation.

Achieving multi-dimensional Li+ transport nanochannels via spatial-partitioning in crystalline ionic covalent organic frameworks for highly stable lithium metal anode

The fragile solid electrolyte interphase (SEI) and anisotropic dendrite growth during Li plating/stripping have posed as intractable handicaps to the practical implementation of lithium metal batteries (LMBs). The Li+ uniform distribution and unimpeded transfer play significant roles to enable protuberance-free Li textures. Herein, the highly-crystalline TFSI− ionic-covalent organic framework (I-COF) endowed with designated mixed-dimensional channels was constructed as an artificial SEI layer via anionic post-modification. Benefiting from the desirable spatial-partitioning effect triggered by nanochannels reconfiguration, the I-COF with expanded multi-dimensional Li+ transport channels and scaled-down pore volume could effectively disperse the local concentration gradient of Li+ flux and inhibit growth of Li dendrites. Besides, the coordinated TFSI− anions with a high tLi+ of 0.76 can selectively restrict the delivery and decomposition of homogeneous ions. To understand the interfacial charge transfer mechanisms, the lithophilic properties and the energy barriers for Li+ migration were also calculated. Correspondingly, the I-COF(TI−) modified Li|Li symmetric cell showed superb durability over 5500 h at 4 mA cm−2 with extraordinary overpotential. The Li|S full cell also displayed prolonged lifespan and excellent rate performance. The comprehension of the mixed-dimensional interfacial strategy via spatial-partitioning provides new insights into the fabrication of solid–solid interfaces, which can aid in the improved design and development of advanced lithium-metal batteries (LMBs).

Guanidinium-functionalized ionic covalent organic framework for selective and efficient recovery of palladium(II) from metallurgical wastewater

Efficient and selective recovery of palladium from acidic metallurgical wastewater is of great economic and environmental importance but remains challenging. Here, two novel ionic covalent organic frameworks (iCOFs), Tp-DGCl and BT-DGCl, were synthesized by reaction of 1,3-diaminoguanidine hydrochloride with 1,3,5-triformyphloroglucinol and benzene-1,3,5-triscarbaldehyde, respectively, and then applied to the recovery of Pd(II) from metallurgical wastewater. The maximum adsorption capacities of Tp-DGCl and BT-DGCl at pH 2.0 and 298.15 K were 342.1 mg g−1 and 231.1 mg g−1, which are higher than the majority of similar reported adsorbents. The adsorption isotherms of Pd(II) on iCOFs were highly consistent with the Langmuir isotherm model. Furthermore, the kinetics of the adsorptions by Tp-DGCl and BT-DGCl conformed to the quasi-second-order kinetic model, indicating that the controlling step of adsorption is chemical adsorption. Thermodynamic studies revealed that elevated temperatures are beneficial for the recovery of Pd(II). At the same time, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, zeta potential, and density functional theory computational analysis confirmed that electrostatic attraction and coordination are the main mechanisms for Pd(II) adsorption on iCOFs. This work not only highlights that the prepared iCOFs can be used as effective reusable adsorbents to selectively adsorb Pd(II) but also opens the door for the practical application of iCOFs in recovering palladium from complex metallurgical wastewater.

An ultrastable cationic covalent organic framework for selective capture of silver from aqueous solution

Recovery of silver from wastewater is a promising alternative from the economic and environmental perspective. Herein, we present an ultrastable ionic covalent organic framework (COF) as a recyclable adsorbent for Ag(I) recovery. The COF exhibits a large surface area, regular pores, and extremely high chemical stability combined with the confined ionic interface, which makes it an excellent material for silver adsorption with fast adsorption kinetics, excellent selectivity, and high saturated adsorption capacity (up to 349.6 mg/g). The superb uptake performance of the cationic COF is attributed to the in-situ precipitation of AgBr and adsorption as well as the coordination of O atoms on the framework to silver.

Europium chelate-anionic exchange functionalized covalent organic frameworks for the sensing of aristolochic acid a in humans and sulfamethoxazole/trimethoprim in surface water

The application of covalent organic frameworks (COFs) in fluorescence detection is of great interest. Herein, we have synthesized the ionic covalent organic framework TGH+·PD: Eu(TTA)4 with the characteristic emission of lanthanides by a straightforward ion-exchange method. This is the first time that aristolochic acid A (AA), a key biomarker for absorption and metabolism in the body for early diagnosis of diseases, has been detected by using COF as a fluorescent probe, which exhibits a good linear correlation with the AA concentration over a range from 5.0 to 1000 μM with a detection limit of 0.0808 μM. In addition, the selective response to sulfamethoxazole (SMZ)/trimethoprim (TMP) is achieved by varying the excitation wavelength with detection lines of 30.2 nM and 2.898 μM, respectively. It is worth mentioning that BNPP has been developed for the accurate determination of SMZ in uncertain samples. In a word, the prepared TGH+·PD: Eu(TTA)4-based sensor can be used for the quantitative detection of AA and SMZ/TMP, separately, effectively extending the application of COFs in the field of fluorescence sensing.

Water/Vapor Assisted Fabrication of Large-Area Superprotonic Conductive Covalent Organic Framework Membranes.

Fabrication of large-area ionic covalent organic framework membranes (iCOMs) remains a grand challenge. Herein, the authors report the liquid water and water vapor-assisted fabrication of large-area superprotonic conductive iCOMs. A mixed monomer solution containing 1,3,5-triformylphloroglucinol (TFP) in 1,4-dioxane and p-diaminobenzenesulfonic acid (DABA) in water is first polymerized to obtain a pristine membrane which subsequently underwent crystallization process in mixed vapors containing water vapor. During the polymerization stage, water played a role of a diluting agent, weakening the Coulombic repulsion between sulfonic acid groups. During the crystallization stage, water vapor played a role of a structure-directing agent to facilitate the formation of highly crystalline, large-area iCOMs. The resulting membranes achieved a proton conductivity value of 0.76 S cm-1 at 90 °C under 100% relative humidity, which is among the highest ever reported. Using liquid water and water vapor as versatile additives open a novel avenue to the fabrication of large-area membranes from covalent organic frameworks and other kinds of crystalline organic framework materials.

Magnetic Resonance Diagnosis of Early Triple-Negative Breast Cancer Based on the Ionic Covalent Organic Framework with High Relaxivity and Long Retention Time.

Patients with triple-negative breast cancer (TNBC) have dismal prognoses due to the lack of therapeutic targets and susceptibility to lymph node (LN) metastasis. Therefore, it is essential to develop more effective approaches to identify early TNBC tissues and LNs. In this work, a magnetic resonance imaging (MRI) contrast agent (Mn-iCOF) was constructed based on the Mn(II)-chelated ionic covalent organic framework (iCOF). Because of the porous structure and hydrophilicity, the Mn-iCOF has a high longitudinal relaxivity (r1) of 8.02 mM-1 s-1 at 3.0 T. For the tumor-bearing mice, a lower dose (0.02 mmol [Mn]/kg) of Mn-iCOF demonstrated a higher signal-to-noise ratio (SNR) value (1.8) and longer retention time (2 h) compared to a 10-fold dose of commercial Gd-DOTA (0.2 mmol [Gd]/kg). Moreover, the Mn-iCOF can provide continuous and significant MR contrast for the popliteal LNs within 24 h, allowing for accurate evaluation and dissection of LNs. These excellent MRI properties of the Mn-iCOF may open new avenues for designing more biocompatible MRI contrast agents with higher resolutions, particularly in the diagnosis of TNBC.

Leaf-like ionic covalent organic framework for the highly efficient and selective removal of non-steroidal anti-inflammatory drugs: Adsorption performance and mechanism insights

In recent years, ionic covalent organic frameworks (iCOFs) have become popular for the removal of contaminants from water. Herein, we employed 2-hydroxybenzene-1,3,5-tricarbaldehyde (TFP) and 1,3-diaminoguanidine monohydrochloride (DgCl) to develop a novel leaf-like iCOF (TFP-DgCl) for the highly efficient and selective removal of non-steroidal anti-inflammatory drugs (NSAIDs). The uniformly distributed adsorption sites, suitable pore sizes, and functional groups (hydroxyl groups, guanidinium groups, and aromatic groups) of the TFP-DgCl endowed it with powerful and selective adsorption capacities for NSAIDs. Remarkably, the optimal leaf-like TFP-DgCl demonstrated an excellent maximum adsorption capacity (1100.08 mg/g) for diclofenac sodium (DCF), to the best of our knowledge, the largest adsorption capacity ever achieved for DCF. Further testing under varying environmental conditions such as pH, different types of anions, and multi-component systems confirmed the practical suitability of the TFP-DgCl. Moreover, the prepared TFP-DgCl exhibited exceptional reusability and stability through six adsorption–desorption cycles. Finally, the adsorption mechanisms of NSAIDs on leaf-like TFP-DgCl were confirmed as electrostatic interactions, hydrogen bonding, and π-π interactions. This work significantly supplements to our understanding of iCOFs and provides new insights into the removal of NSAIDs from wastewater.