Engineering high-performance N-doped carbon catalysts for peroxymonosulfate (PMS) activation and elucidating their activation mechanism are crucial for the degradation of emerging pollutants. In this study, we propose a novel self-template carbonization strategy (NSCS) based on a N-containing conjugated microporous polymer (NCMP, poly(triphenylamine)) to fabricate high-performance N-doped porous carbon catalysts. Owing to the unique N-mediated catalytic sites within the confined micropores of the NCMP precursor, the NSCS approach enables the investigation of reactive oxygen species evolution and their formation mechanisms as carbonization temperature increases from 200 to 1400 °C.
View Article and Find Full Text PDFUtilizing membrane separation technology has displayed promising application potential for removing synthetic dyes; however, membrane performance tends to decline over time due to fouling caused by feed solution contaminants, leading to decreased separation efficiency and shortened membrane lifespan. Therefore, improving the antifouling properties of membranes is critical to ensure the long-term efficiency of water treatment systems. In this work, a high-performance catalyst, CuZn@ZC, with remarkable oxygen activation activity, was successfully prepared and subsequently integrated onto the membrane surface via simple pumping filtration, resulting in self-cleaning membranes with superior antifouling capabilities.
View Article and Find Full Text PDFConjugated microporous polymers (CMPs) present high promise for chemiresistive gas sensing owing to their inherent porosities, high surface areas, and tunable semiconducting properties. However, the poor conductivity hinders their widespread application in chemiresistive sensing. In this work, three typical CMPs (PSATA, PSATB, and PSATT) are synthesized and their chemiresistive gas sensing performance is investigated for the first time.
View Article and Find Full Text PDFTo meet the demand for longer driving ranges and shorter charging times of power equipment in electric vehicles, engineering fast-charging batteries with exceptional capacity and extended lifespan is highly desired. In this work, we have developed a stable ultrafast-charging and high-energy-density all-nanofibrous covalent organic framework (COF) battery (ANCB) by designing a series of imine-based nanofibrous COFs for the cathode, separator, and anode by Schiff-base reactions. Hierarchical porous structures enabled by nanofibrous COFs were constructed for enhanced kinetics.
View Article and Find Full Text PDFTuning the interfacial structure of metal oxide substrates is an essential strategy to induce electronic structure reconstruction of supported catalysts, which is of great importance in optimizing their catalytic activities. Herein, vanadium oxides-supported Ir catalysts (Ir-VO, Ir-VO, and Ir-VO) with different interfacial bonding environments (Ir-V, Ir-O, and Ir-O, respectively) were investigated for hydrogen evolution reaction (HER). The regulating mechanism of the influence of different interfacial bonding environments on HER activity was investigated by both experimental results and computational evidence.
View Article and Find Full Text PDFEngineering a catalytic membrane capable of efficiently removing emerging organic microcontaminants under ultrahigh flux conditions is of significance for water purification. Herein, drawing inspiration from the functional attributes of lymphatic vessels involved in immunosurveillance and fluid transport with minimal energy consumption, a novel hierarchical porous catalytic membrane is engineered. This membrane, based on an innovative nitrogen-rich conjugated microporous polymer (polytripheneamine, PTPA), is synthesized using an electrospinning coupled in situ polymerization approach.
View Article and Find Full Text PDFBipyridine-based covalent organic frameworks (COFs) have emerged as promising contenders for the photocatalytic generation of hydrogen peroxide (HO). However, the presence of imine nitrogen alters the mode of HO generation from an efficient one-step two-electron (2e) route to a two-step 2e oxygen reduction pathway. In this work, we introduce 3,3'-bipyridine units into imine-based COF skeletons, creating a pyridyl-imine structure with two adjacent nitrogen atoms between the pyridine ring and imine linkage.
View Article and Find Full Text PDFSmall Methods
October 2024
Solar energy is a primary form of renewable energy, and photothermal conversion is a direct conversion process with tunable conversion efficiency. Among various kinds of photothermal conversion materials, porous organic polymers (POP) are widely investigated owing to their controllable molecular design, tailored porous structures, good absorption of solar light, and low thermal conductivity. A variety of POP, such as conjugated microporous polymers (CMP), covalent organic frameworks (COF), hyper-crosslinked porous polymers (HCP), polymers of intrinsic microporosity (PIM), porous ionic polymers (PIP), are developed and applied in photothermal conversion applications of seawater desalination, latent energy storage, and biomedical fields.
View Article and Find Full Text PDFGradients play a pivotal role in membrane technologies, e.g., osmotic energy conversion, desalination, biomimetic actuation, selective separation, and more.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2023
Modification of the molecular packing of nonfullerene acceptors through fluorination represents one of the most promising strategies to achieve highly efficient organic solar cells (OSCs). In this work, three nonfused electron acceptors, namely, DTCBT-F ( = 0, 5, 9) with precisely controlled amounts of fluorine atoms in the side chains are designed and synthesized, and the effect of side chain fluorination is systematically studied. The results demonstrate that the light absorption, energy levels, molecular ordering, and film morphology could be effectively tuned by precisely controlling the side chain fluorination.
View Article and Find Full Text PDFWith the rapid development of energy storage technology, the operation of portable and wearable devices is inseparable from high energy density power supplies. However, the demand for high performance supercapacitors in movable smart electronics is still restrained by their insufficient areal capacitance and limited power/energy densities. In addition, some electroactive materials, including metal oxides, conductive polymers, graphene, porous carbons, etc.
View Article and Find Full Text PDFSimultaneous recovery of energy and carbon from recalcitrant wastewater has attracted ever-growing interest for water management. However, the existing technologies to break down recalcitrant pollutants are mainly energy and chemical intensive. Here, a novel hydrothermal reaction amended with activated carbon (AC) was demonstrated to enable an unprecedented 99.
View Article and Find Full Text PDFEngineering of conjugated microporous polymers (CMPs) with high porosity, redox activity, and electronic conductivity is of significant importance for their practical applications in electrochemical energy storage. Aminated-multiwall carbon nanotubes (NH -MWNT) are utilized to modulate the porosity and electronic conductivity of polytriphenylamine (PTPA), which is synthesized via Buchwald-Hartwig coupling reaction of tri(4-bromophenyl)amine and phenylenediamine as constitutional units in a one-step in situ polymerization process. Compared to PTPA, the specific surface area of core-shell PTPA@MWNTs has been greatly improved from 32 to 484 m g .
View Article and Find Full Text PDFStretchable organohydrogel fibers are attracting considerable interest for next-generation flexible and wearable soft strain sensors due to their excellent stability in harsh environments. However, due to the uniformly distributed ions and reduced number of carriers in the whole material, the sensitivity of organohydrogel fibers under subzero temperature is not desirable, which significantly hinders their practical application. Herein, a newly competitive proton-trapping strategy was designed to obtain anti-freezing organohydrogel fibers for high-performance wearable strain sensors a simple freezing-thawing process, in which tetraaniline (TANI), serving as the proton trapper, and representing the shortest repeated structural unit of polyaniline (PANI), was physically crosslinked with polyvinyl alcohol (PVA) (PTOH).
View Article and Find Full Text PDFThe role of N-heterocyclic carbene, a well-known reactive site, in chemical catalysis has long been studied. However, its unique binding and electron-donating properties have barely been explored in other research areas, such as metal capture. Herein, we report the design and preparation of a poly(ionic liquid)-derived porous organic polycarbene adsorbent with superior gold-capturing capability.
View Article and Find Full Text PDFDesigning porous FeNC nanomaterials with highly efficient active sites is an effective strategy for constructing high-performance oxygen reduction reaction (ORR) electrocatalysts. N-containing porous organic polymers (POPs) have emerged as promising candidates for the preparation of porous FeNC catalysts. Here, N-rich tripolycyanamide-based microporous polymer (TCAMP)-coated SiO nanospheres (SiO@TACMP) were prepared as the precursors of an Fe-N doped hierarchical meso-micro porous carbon (Fe-N-HMC) electrocatalyst for the ORR.
View Article and Find Full Text PDFWith the emerging of the Internet of Things, chemiresistive gas sensors have been extensively applied in industrial production, food safety, medical diagnosis, and environment detection, etc. Considerable efforts have been devoted to improving the gas-sensing performance through tailoring the structure, functions, defects and electrical conductivity of sensitive materials. Among the numerous sensitive materials, mesoporous semiconductor metal oxides possess unparalleled properties, including tunable pore size, high specific surface area, abundant metal-oxygen bonds, and rapid mass transfer/diffusion behavior (Knudsen diffusion), which have been regarded as the most potential sensitive materials.
View Article and Find Full Text PDFFabrication of adsorbents with excellent adsorption capacity, outstanding stability, easy separation ability, excellent recyclability and widely generality for organic dyes removal from wastewater remains challenging. Herein, three-dimensional polyaniline/poly(vinyl alcohol)/montmorillonite (PANI/PVAL/MMT) hybrid aerogels with easy separation performance and highly effective reusable adsorption on both anionic and cationic dyes were fabricated by a simple in-situ polymerization method. As-prepared hybrid aerogels were characterized via infrared and Raman spectra, scanning electron microscopy, energy dispersive spectra mapping, small and wide-angle X-ray scattering, thermogravimetric analysis, mercury intrusion porosimetry and elemental analysis.
View Article and Find Full Text PDFSince discovered in 2007, conjugated microporous polymers (CMPs) have been developed for numerous applications including gas adsorption, sensing, organic and photoredox catalysis, energy storage, etc. While featuring abundant micropores, the structural rigidity derived from CMPs' stable π-conjugated skeleton leads to insolubility and thus poor processability, which severely limits their applicability, e.g.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2022
Seawater evaporation realized by solar-thermal conversion represents one of the most sustainable and effective strategies to obtain fresh water. Many approaches have been proposed to achieve high efficiencies of solar-thermal conversion, but their practical applications are limited by the low scalability. Herein, novel porphyrin/aniline-based conjugated microporous polymers (PACMPs) are synthesized a Buchwald-Hartwig coupling reaction, which are then integrated with polyurethane sponges a simple dip-coating technique.
View Article and Find Full Text PDFConductive composite inks are widely used in various applications such as flexible electronics. However, grand challenges still remain associated with their relatively low electrical conductivity and require heavy use of organic solvents, which may limit their high performance in broad applications and cause environmental concerns. Here, we report a generalized and eco-friendly strategy to fabricate highly conductive aqueous inks using silver nanowires (AgNWs) and biomass-derived organic salts, including succinic acid-chitosan (SA-chitosan) and sebacic acid-chitosan.
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