Latest ArticlesHydrogen peroxide (H2O2), as a green and mild oxidant, exhibits unique application advantages in several fields, including catalytic systems for organic synthesis and environmental pollutant degradation. In recent years, semiconductor-based photocatalytic strategies for H2O2 production have attracted extensive attention due to their sustainable characteristics, which utilize H2O/O2 as primary reactants to achieve solar-driven chemical energy conversion. Covalent organic frameworks (COFs), with their stable crystalline porous structures, highly ordered π-conjugated systems, modular designability, and ultra-large specific surface areas, provide an ideal platform for photocatalytic H2O2 synthesis. Hybridizing COFs with other functional materials has emerged as an effective strategy to address challenges commonly faced by single-component COFs systems, such as low light utilization efficiency, insufficient redox capability, and rapid recombination of photogenerated charge carriers. This review summarizes research progress in COFs-based heterojunctions for photocatalytic H2O2 synthesis, beginning with a concise introduction to the photosynthesis mechanism of H2O2 and fundamental principles of common heterojunctions in the field, followed by a focused review of reported COFs-based heterojunctions. In addition, the various in-situ applications of H2O2 in the context of photosynthesis by COFs-based heterojunctions were discussed, including sterilization, organic pollutants degradation, biomedical applications and organic synthesis. Then concluding with an overview of current challenges and future prospects in this emerging research area. This work aims to promote practical applications of COFs in green energy sectors while providing insights for developing efficient photocatalysts to advance photocatalytic H2O2 production.
Two-dimensional (2D) materials exhibit great potential for osmotic power generation due to their high membrane selectivity. However, performance enhancement remains hindered by substantial resistance arising from tortuous ion transport pathways within 2D nanofluidic membranes. MXenes, a novel class of 2D layered materials, have garnered significant attention as promising candidates for reverse electrodialysis (RED) membranes due to their laminated nanochannels and surface-charged functional groups. Although MXene-derived ion-exchange membranes display exceptional ionic discrimination capabilities and enhanced charge transport properties, their implementation in practical systems is limited by structural fragility and compromised performance under hydrated conditions, primarily due to weak interlayer interactions, restricting their RED performance. This study demonstrates an MXene-sodium ligninsulfonate (MSL) lamellar architecture to feature record-low internal resistance, achieving breakthrough osmotic energy conversion efficiency through synergistic interfacial engineering. In addition, the well-aligned MXene framework significantly shortens ion permeation pathways, thus lowering internal resistance. As a result, the MSL membrane delivers a high power density of approximately 22.15 W/m2 when mixing artificial seawater and river water, representing a 6.78-fold improvement over pristine MXene membranes. This interfacial engineering protocol addresses the longstanding trade-off between ion selectivity and membrane durability in nanofluidic systems, paving the way for the practical implementation of MXene-based technologies in marine energy conversion.
Loading transition metal oxyhydroxides (TMOH) electrocatalyst on semiconductors (SC) improves the photoelectrochemical (PEC) water splitting performance. However, the inevitable interface charge recombination between SC and TMOH hinders the PEC efficiency. Herein, differing from the conventional charge transfer process, a novel charge modulation layer, i.e., Ce-CoOx, like a "hole transporter" has been incorporated into the SC/TMOH system. A series of electrochemical characterizations confirm that the "hole transporter" can directly and rapidly transfer holes from BiVO4 to FeNiOOH, resulting in a highly efficient charge separation. As expected, the BiVO4/Ce-CoOx/FeNiOOH photoanode presents a desirable photocurrent of 6.0 mA/cm2 and good stability. More importantly, the smart approach can also be extended to BiVO4/Ce-NiOx/FeNiOOH system, proving its universality. This work opens up a new avenue for designing efficient photoanode for PEC water splitting.
Hydrogen peroxide (H2O2) is a vital oxidant and a promising liquid fuel, serving as one of the 100 most essential chemicals. Covalent organic frameworks (COFs) have emerged as ideal candidates for pure H2O2 photosynthesis due to their fully designable structures and well-defined active sites. The microenvironment engineering of COFs presents exciting opportunities to optimize both selectivity and efficiency in H2O2 photosynthesis, while their precisely identifiable active sites enable rational design of next-generation high-performance COFs. Although significant progress has been made in regulating COFs’ active sites for H2O2 photosynthesis, a comprehensive review systematically analyzing this specific and significant area remains absent. Here, we provide a thorough overview of the recent advances and persistent challenges in the microenvironment engineering of COFs for H2O2 photosynthesis. To begin with, the basic principles of O2-to-H2O2 photocatalytic conversion and outline general strategies for microenvironment engineering of COFs are presented. Subsequently, we critically examine the current research progress in this field. The urgent challenges and the future development of the microenvironment engineering of COFs in H2O2 photosynthesis are finally proposed. This review will provide valuable theoretical guidance for developing the next generation of COF photocatalysts that promote H2O2 photosynthesis.
Antidepressants (ATDs) have negative impacts on the ecosystem and have been detected globally in concentrations ranging from approximately 0.17 ng/L to 4237 ng/L in municipal wastewater treatment plant influent. However, the removal of ATDs by biological methods is still unsatisfactory at present, due to the extremely complex removal pathway and various removal processes for different ATDs. Therefore, there is an urgent need for a systematic compendium to help people understand the biodegradation process of ATDs. This work provides an overview of the classification, physicochemical properties, and environmental sources of ATDs; systematically reviews the adsorption behaviors and transformation processes of various ATDs during biological treatment; examines the removal efficiency, degradation mechanisms, and critical operating conditions of bioreactors; and discusses the mechanism of ATD adsorption and removal by extracellular polymers secreted by microbial cells during the biological treatment of municipal wastewater. This work clarifies the evolution of different types of ATDs during municipal wastewater biological treatment and proposes future research avenues for the more efficient removal of ATDs.
Biological systems exploit their sophisticated hierarchical anisotropic architectures to achieve complex shape morphing under external stimuli. However, artificial soft intelligent actuators often suffer from limited response speeds and poor programmability of deformation, primarily due to densely crosslinked network designs and insufficient anisotropic resolution. Here, we report a synergistic method combining directional freezing-induced self-assembly and dynamic metal coordination crosslinked mechanical alignment to fabricate anisotropic hydrogels with fast multiple responsiveness and programmable three-dimensional (3D) deformation. Benefiting from an interconnected lamellar network and open-oriented mass transport channels, the hydrogel exhibits rapid anisotropic stimuli-responsive deformations with a shrinkage along the lamellar direction that is 1.9 times greater than that in the perpendicular direction in 5 s of thermal stimulation, and a complete recovery within 4 s upon cooling. By developing a spatially modulated coordination photodissociation strategy, a gradient crosslinking network is further constructed within the hydrogel, enabling diverse and programmable 3D deformations in response to external stimuli, which facilitate complex actuation behaviors such as object grasping, biomimetic gestures, and light-driven lifting. Thus, the hydrogel with hierarchically anisotropic structure and porous dynamic crosslinked network is potential for intelligent soft robotics requiring flexible controllable deformation.
Differentiating structural isomers in mass spectrometry (MS) poses significant challenges due to the difficulties in generating fragment ions by atmospheric pressure ionization and the spectral similarities encountered in tandem MS/MS analysis. The continuous arc plasma enables in-source dissociation fingerprinting analysis of isomers but presents a risk of solvent ignition during sample introduction because of high temperatures, posing safety concerns. To address these challenges, the tunable pulsed arc plasma (TPAP) ionization and dissociation device has been developed. The TPAP device converts continuous arc plasma into a pulsed mode, reduces plasma temperatures, enhances discharge stability and safety, and enables adjustable plasma energy for in-source compound dissociation. Programmable control over the pulsed arc plasma voltage allows the scanning of compounds under varying dissociation energies, facilitates the construction of compound-specific energy-resolved spectra. Validation experiments with disubstituted benzene species, chlorogenic acid derivatives, disaccharide and diacylglycerol have demonstrated the capability of TPAP-MS to effectively differentiate isomers through distinct energy-resolved spectra. The TPAP-MS requires minimal instrumental modifications and provides rapid and precise structural annotations directly from the ion source, offering broad potential applications in the analysis of structural isomers.
Ovarian cancer is among the deadliest cancers, with the highest mortality rate among gynecological cancers; thus, highly sensitive early diagnosis is of paramount importance. In this study, we developed an innovative biosensor that integrates DNA-functionalized covalent organic frameworks with CRISPR-Cas12a technology for dual-signal amplification to achieve ultra-sensitive detection of ovarian cancer biomarkers. The COFs were co-functionalized with aptamers specific to target protein biomarkers and a larger number of activators. Upon recognition and binding to target proteins, the activators anchored on the COF surface become accessible in the detection system, converting low-abundance protein signals into amplified nucleic acid signals, which represents the first stage of signal amplification. These activators subsequently trigger the trans-cleavage activity of CRISPR-Cas12a, leading to the cleavage of fluorophore–quencher reporters and resulting in further amplified fluorescence output, constituting the second stage of amplification. This dual-signal amplification strategy, integrated with a microfluidic chip, enabled the sensitive detection of CA125 and HE4, with detection limits as low as 0.001 U/mL and 0.2 pg/mL, respectively, providing a robust, accurate, and scalable platform for ovarian cancer diagnostics and demonstrating potential applications in clinical bioanalysis and diagnosis.
In gas separation mixed matrix membranes (MMMs), the interlayer stacking of nanosheet fillers directly leads to tortuous transport pathways that significantly reduce both membrane permeability and selectivity. To solve this issue, this study employs cellulose (MC) to interweave MXene for preparing cellulose-MXene (MC-MX) networks, which are then mixed with Pebax MH 1657 to prepare MMMs for enhancing CO2 separation performance. The MC-MX network mimics the tollgate-highway system within the MMMs. In this system, MX acts as a selective tollgate that preferentially recognizes CO2 through hydrogen bond interactions while improving CO2/CH4 selectivity in MMMs. Meanwhile, the hydroxyl–rich surfaces of MC provide low-resistance transport highway for accelerated CO2 transport within the MMMs. Compared to the pure Pebax membrane, the CO2 permeability of the Pebax/MC-MX-1wt% MMM increases to 580.46 Barrer (97%), and the CO2/CH4 selectivity increased to 41.48 (70%). Furthermore, the separation performance of the Pebax/MC-MX-1wt% MMM approaches the 2019 upper bound. The research results indicate that the tollgate-highway strategy effectively improves CO2/CH4 separation performance in MMMs, offering practical implications for the rational design of high-performance membranes.
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