Strong Interfacial Interaction Research Articles

Assembling an S-type heterojunction comprising vacancy-rich CeO2-x and CuBi2O4 for improved photocatalytic oxidation of gaseous toluene

The exploration of highly efficient methods for degrading VOCs, with concurrent low energy consumption and lasting reusability, holds significant appeal. In this regard, an S-type CuBi2O4/CeO2-x heterojunction with the robust interfacial interactions is presented as an active photocatalyst for the efficient decomposition of gaseous toluene under full-spectrum irradiation. The optimal sample CC15 effectively degrades gaseous toluene at a high concentration of 1800 ppm within 2 h, achieving a notable CO2 yield of 87.05 %, and a TOC (total organic carbon) removal rate of 89.33 %. Furthermore, CuBi2O4/CeO2-x exhibits exceptional stability, maintaining its 100 % degradation capability over 32 cycles for nearly 64 h. Comparative characterization reveals that the superior performance derives from an abundance of oxygen vacancies and effective pre-adsorption capabilities, which facilitate rapid adsorption of VOCs on the catalyst surface, thereby increasing the likelihood of degradation reactions. Additionally, the formation of an S-type heterojunction, valence pairing between Bi3+ and Ce3+/4+ ions, and strong interfacial interactions serve as the primary pathways for the efficient separation of photogenerated carriers, contributing to the high CO2 production rate and prolonged cycle stability. The present investigation underscores the significant potential of vacancy-rich S-type heterojunctions and interfacial interactions between composite components, offering excellent activity and long-term availability for VOCs removal.

Hydrophobic enrichment-induced augmentation of NH2-UiO-66 particle interactions for enhanced pervaporation performance of polydimethylsiloxane membrane

BackgroundIn this research, we aimed to improve the hydrophobic property of NH2-UiO-66 particles by palmitoyl chloride (PC) modification. PC-UiO-66 particles were mixed in the selective layer of PDMS (polydimethylsiloxane)-PVDF (Polyvinylidene fluoride) composite membrane for organo-selective pervaporation. MethodsWe effectively preserved conspicuous crystallinity and high porosity during a conversion from hydrophilic to hydrophobic MOF, as confirmed by XRD and BET studies. The successful incorporation of palmitoyl long alkyl chains into PC-UiO-66 was verified through FTIR, XPS, and EDS studies. PC-UiO-66 particles exhibited an excellent dispersion in PDMS matrix due to a strong interfacial polymer-MOF interaction observed in FESEM and AFM studies. An organophilic pervaporation separation performance of pristine PDMS, NH2-UiO-66/PDMS, and PC-UiO-66/PDMS membranes coated on PVDF support was evaluated for ethanol/water, IPA/water, and 1,5 PDO/IPA feed solution. Significant findingsThe results demonstrated that adding PC-UiO-66 particles significantly improved the separation performance of PC-UiO-66/PDMS membranes, achieving the highest selectivity compared to pristine PDMS and NH2-UiO-66/PDMS membranes.

2D MXene Ti3C2 Coupled with 1D Co3O4 Nanowires on Carbon Cloth for Efficient Chlorine Evolution Activity

AbstractChlorine evolution reaction (CER) is a key anode reaction in chlor‐alkali electrolysis. Although non‐precious metals have been widely used as CER catalysts, their low catalytic activity has been a major constraint on their development. Herein, 1D Co3O4 coupled with 2D Ti3C2 MXene on carbon cloth for highly efficient CER is reported by constructing two different heterojunctions (1D Co3O4 tip to 2D Ti3C2 face and 1D face to 2D face) through electronic coupling and strong interfacial interaction. The decreased electron density around O atoms in Co─O and Ti─O at two heterojunctions is more conducive to the adsorption of Cl−, thereby reducing the free energy of the reaction and jointly promoting CER. Consequently, the MXene@Co3O4/CC (carbon cloth) exhibits a low overpotential of 86 mV at 10 mA cm−1, low tafel slope of 47.9 mV dec−1, which is superior to commercial DSA and other non‐precious metal materials. This work provides new insights into the rational design of multiple heterojunctions, which leads to a new path for non‐precious metal catalysts in CER.

Enhanced photocatalytic removal of tetracycline and methyl orange using Ta3N5@ZnIn2S4 nanocomposites

The presence of toxic substances in wastewater poses a severe threat to human survival and development. In recent years, photocatalytic technology has emerged as a promising solution for the efficient removal of harmful pharmaceutical pollutants and organic dyes. This study focuses on the synthesis and characterization of a novel Ta3N5@ZnIn2S4 (TN@ZIS) nanocomposite, which exhibits remarkable photocatalytic performance in degrading tetracycline hydrochloride (TC) and methyl orange (MO) under LED irradiation. The TN@ZIS nanocomposite was synthesized using a simple route involving flux-assisted nitridation and in-situ hydrothermal treatment processes. The resulting structure consists of layered ZnIn2S4 nanosheets firmly anchored onto the surface of Ta3N5 nanorods, as confirmed by SEM and TEM analysis. XPS tests revealed a strong interfacial interaction within the nanocomposite, which is advantageous for the separation of photogenerated charge carriers. Notably, the TN@ZIS hybrids demonstrated a significant improvement in photocatalytic activity compared to bare Ta3N5 nanorods. During the entire photocatalytic degradation process (60 min and 100 min), TC and MO achieved degradation efficiencies of approximately 72.3 % and 81.2 %, respectively. These results highlight the competitive nature of TN@ZIS among Ta3N5-based materials. The enhanced photocatalytic performance can be primarily attributed to the synergistic effect of improved separation of photogenerated charge carriers and the increased active sites provided by the TN@ZIS nanocomposite. This study contributes to the development of efficient and stable photocatalysts for the removal of pharmaceutical pollutants and organic dyes from wastewater, thereby addressing the urgent need for effective water treatment technologies.

Hexavalent Chromium Reduction Mediated by Interfacial Electron Transfer over the Co@NC Nanosheet-Assembled Microflowers.

The reductive transformation of Cr(VI) into Cr(III) mediated by formic acid with efficient, stable, and cost-effective catalysts is a promising strategy for remediating Cr(VI) contamination. Herein, we report the facile construction of uniform Co@NC nanosheet-assembled microflowers for the reduction of Cr(VI). Both experimental results and density functional theory (DFT) calculations reveal the vital role of the intensive interfacial electronic interaction between Co nanoparticles and the N-doped carbon layer in facilitating the anchoring and dispersion of Co nanoparticles within the carbon framework. The interfacial electron transfer from Co to NC contributes to the interaction with Cr2O72- ions, promoting the subsequent H-transfer reaction. A Langmuir-Hinshelwood kinetic model has been established for the Cr(VI) reduction catalyzed by the CNCF2 (pyrolyzed at 700 °C), which shows a superior reaction performance. This study provides a facile strategy to delicately design well-assembled heterostructures with rich interfaces and strong interfacial interactions for a series of applications in environmental/thermal catalysis.

Ferroelectric Control of Band Alignments in In2Se3/h‐BN and CuInP2S6/h‐BN van der Waals Heterostructures

Recently, 2D ferroelectric (FE) heterostructures have become a subject of great interest due to their potential device applications and the underlying physics involved. In this study, the first‐principles calculations are employed to examine the FE control of electronic structures in 2D FE heterostructures, specifically In2Se3/h‐BN and CuInP2S6 (CIPS)/h‐BN. In these results, it is demonstrated that by reversing the polarization of the FE layers, the band alignment of the heterostructures can be interconverted between type II and type I. For In2Se3/h‐BN, the variation of out‐of‐plane polarization can be attributed to the hindrance and facilitation of charge transfer from h‐BN to In2Se3 by the intrinsic electric field of the In2Se3 monolayer. For CIPS/h‐BN heterostructures, the higher transferred charge in the Cdn configuration due to the presence of built‐in electric fields and the stronger interfacial interaction in the Cdn configuration result in a higher polarization value compared to the Cdn configuration. Moreover, the carrier mobility of the heterostructures can also be effectively modulated by the FE polarization. In these findings, the potential significance of FE heterostructures with tunable band alignment and bandgap is highlighted in the development of nanoscale optoelectronic devices.

Argon ion sputtering bridging plasma nitriding and GLC film deposition: Effects on the mechanical and tribological properties

A duplex coating consisting of a nitrided layer and a GLC (Graphite-like carbon) film was deposited on the surface of the M50NiL steel via a one-step process in a plasma nitriding system. The influence of argon ion sputtering, a critical process bridging plasma nitriding and GLC film deposition, was studied. Effects of argon ion sputtering on the growth of the GLC film were investigated by means of Raman spectroscopy, scanning electron microscopy and transmission electron microscopy. The mechanical and tribological properties of the duplex coating were evaluated by a Vickers hardness tester, a scratching tester and a rotating ball-on-disc tribometer. Results reveal that pre-treatment by ion sputtering improves the surface condition of the nitrided layers and increases its surface energy, thus facilitating nucleation growth and GLC film adhesion. The combined effect of better film-substrate adhesion, strong interfacial chemical interaction and the self-lubricating features of the GLC films are the main reasons for the excellent tribological properties of the coating. This study may provide a new idea for optimizing the duplex coating (nitrided layer + GLC film) with excellent tribological properties and high durability.

Facile formation of STO/gC3N4 hybrid composite to effectively degrade the dye and antibiotic under white light

Abstract A novel organic-inorganic photocatalyst like layer structured graphitic carbon nitride (g-C3N4 or CN) hybrid with strontium titanate (SrTiO3 or STO) was prepared by a precipitation-sonication technique for photocatalytic activity. The crystal phases, morphologies, elemental composition, optical properties, and porous structure of the prepared pristine and STO/CN hybrid composite were measured using various physicochemical characterizations. It is indicated that STO nanospheres were effectively loaded on the g-C3N4 nanosheets, resulting in the STO/CN hybrid composite, high surface area, enhanced visible-light absorption, enhancing photoinduced charge separation and suppressing the recombination rate. Furthermore, the 3 wt% of g-C3N4 composited STO (STO/CN-3) catalyst demonstrated higher photocatalytic activity than pristine STO in 100 min under white light irradiation, reaching the degradation efficiency of 92.66 % and 93.31 % toward methylene blue (MB) and tetracycline (TC), respectively. The improved photocatalytic activity of STO/gCN hybrid composite could be ascribed to the synergistic effect between STO and CN with strong interfacial interaction facilitating efficient charge separation and inhibiting the charge recombination of photogenerated electron-hole pairs. Moreover, a possible photocatalytic mechanism has been proposed for the degradation of MB and TC. Besides, the excellent photocatalytic performance, STO/CN-3 nanocomposite also exhibits outstanding photostability under the current factors, suggesting that they are suitable for practical applications.

Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting.

The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential for sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni2P/MoS2-CoMo2S4@C heterometallic electrocatalysts based on the high-nuclearity cluster {Co24(TC4A)6(MoO4)8Cl6}, in which Ni2P nanoparticles were anchored to the surface of the MoS2-CoMo2S4@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that the introduction of Ni2P phases induces significant disturbances in the surface electronic configuration of Ni2P/MoS2-CoMo2S4@C, resulting in more relaxed d-d orbital electron transfers between the metal atoms. Moreover, continuous electron transport was established by the formation of multiple heterojunction interfaces. The optimized Ni2P/MoS2-CoMo2S4@C electrocatalyst exhibited ultralow overpotentials of 198 and 73 mV for oxygen and hydrogen evolution reactions, respectively, in alkaline media, at 10 mA cm-2. The alkali electrolyzer constructed using Ni2P/MoS2-CoMo2S4@C required a cell voltage of only 1.45 V (10 mA cm-2) to drive overall water splitting with excellent long-term stability.

Immobilizing ultrafine PtRu alloy nanoparticles onto 3D interconnected MXene-graphene frameworks for highly efficient methanol oxidation

Although direct methanol fuel cell (DMFC) is regarded as a promising power source to establish green energy conversion system, its overall performance is largely limited by the slow methanol oxidation kinetics of current anode catalysts. Herein, we demonstrate a robust and facile bottom-up strategy for the controllable construction of ultrafine PtRu alloy nanoparticles immobilized onto three-dimensional (3D) interconnected Ti3C2Tx MXene-graphene frameworks (PtRu/MXene-G) through a co-assembly process. Interestingly, the utilization of 3D porous MXene-G matrix provides strong interfacial interactions with alloy nanocrystals and promotes the transportation of both reactant and electron during the electrocatalytic process, while the introduction of Ru atoms ameliorates the Pt electronic structure and generates plentiful hydroxyl species for the oxidative removal of CO byproducts. Working together, the resulting PtRu/MXene-G nanoarchitecture with an appropriate Pt/Ru atomic ratio exhibits exceptional methanol oxidation properties in terms of a large electrochemically active surface area of 101.8 m2 g−1, a high mass (specific) activity of 1779.5 mA mg−1 (1.75 mA cm−2), and good long-term stability, all of which are significantly superior to those of conventional Pt/carbon black, Pt/G, Pt/MXene, and Pt/MXene-G catalysts with an identical Pt usage.

A dual cone actuator with high energy density and long fatigue life by developing a nano-silica reinforced dielectric elastomer composite

Dielectric elastomer actuator (DEA) is considered as one of the most promising soft actuators due to its light weight, good flexibility, high actuated strain and energy density. Herein, a novel DEA material is developed by introducing a kind of SiO2 nanoparticles with strong interfacial polarizability into polydimethyl(methylvinyl) siloxane (PMVS). The 7.5 SiO2/PMVS DEA exhibits a high actuated strain of 31.3 % and blocked stress of 68.4 kPa, 2.4 and 2.9 times of pure PMVS DEA. A dual cone DEA (DCDEA) device was self-designed by using 7.5 SiO2/PMVS films, which possesses a high actuated displacement of 1.3 mm, output force of 0.3 N and energy density of 4.7 J/kg. More importantly, because of the high elasticity and strong interfacial interaction, the 7.5 SiO2/PMVS DCDEA exhibits a long fatigue life of 500,000 times, resulting in a full-life energy density of 2.3 × 106 J/kg, 39 times higher than that of the VHB based DCDEA.

Synergistic enhancement of interfacial adhesion for CF/PEEK composites through carbene chemistry and water‐based self‐catalyzed cross‐linkable PENK‐NH2 sizing agent

AbstractTo address the issue of inadequate interfacial adhesion in carbon fiber/poly ether ether ketone (CF/PEEK) composites, an innovative approach that combines carbene chemistry and sizing treatment was meticulously designed to achieve remarkable synergistic enhancement. Specifically, cyano groups were chemical‐grafted on CF surface via carbene reaction. Meanwhile, a water‐based self‐catalyzed cross‐linkable PENK‐NH2 sizing agent with good storage stability was prepared. Noteworthy, the presence of amino groups as blocking agents of sizing agent significantly accelerated the rate of cyano‐crosslinking, thus effectively avoiding the adverse effects of excessively prolonged cross‐linking period during composites preparation. As a result, robust interaction between cyano‐modified CF and PEEK was established by cross‐linking reaction, along with chemical bonds generated between amino groups of sizing agent and ketone groups in PEEK. The maximum interlaminar shear strength (ILSS) of CF‐CN‐1.5/PEEK composites was 22.0% and 57.0% higher than CF‐1.5/PEEK and CF/PEEK composites. Furthermore, the presence of cyano‐cross‐linked structure endowed interphase with outstanding solvent‐resistance, the mechanical properties of CF composites after solvent treatment were well‐preserved. The strong synergistic interfacial interactions facilitated by chemical bonds in different components provide an effective and fascinating methodology for producing high‐performance CF/composites.Highlights Water‐based self‐catalyzed cross‐linkable PENK‐NH2 sizing agents for CF/PEEK were prepared. NH2 was introduced to avoid the adverse effects of prolonged cyano‐crosslinking. Designed carbenoid motif with cyano group was grafted on CF via carbene chemistry. The interaction between sizing agent and CF was boosted by the cyano‐crosslinking. Mechanical properties of sized composites corroded by solvent were well‐preserved.

A Sandwich Structure Ag/MgFe2O4-Deposited Surface Carbonized Wood for Integrated Solar Steam Generation and Photoreduction of Cr(VI).

The severe deterioration of the marine ecosystem significantly negatively impacts the performance of solar-driven steam generation (SSG) and the quality of the obtained freshwater. Herein, a bifunctional Ag/MgFe2O4@SCW reactor with a sandwich structure is designed for efficient SSG and Cr(VI) reduction, which is constructed via in situ deposit Ag nanoparticles (NPs) and MgFe2O4 onto surface carbonized wood (SCW). Owing to the advanced sandwich structure and strong interfacial interactions between each component, an ultra-high evaporation rate of 1.55kg m-2 h-1 and the efficiency of 88.6% are achieved using Ag/MgFe2O4@SCW under 1 sun. The system exhibits the long-term evaporation performance in the simulated sewage and strong acid/base solutions along with water-harvesting capacity in outdoor solar desalination. The quality of distilled water after desalination of actual seawater and NaCl solutions with different concentrations meets the WHO-recommended drinkable water standards. Furthermore, Ag/MgFe2O4@SCW shows outstanding antibacterial property, self-desalting capacity, as well as reusability and structure stability. Most importantly, the fast carrier separation endows Ag/MgFe2O4@SCW with superior photocatalytic activity and Cr(VI) photoreduction of up to 96.1% after 180min of illumination. The bifunctional Ag/MgFe2O4@SCW reactor provides an advanced synergistic mechanism for improving SSG and photocatalytic performance, while being promising for solar-powered production of clean water.

Milled graphitic nanoparticle toughened epoxy composites via increased resistance to in-plane crack propagation

Fascinating features of 2D-based carbon materials like graphene have drawn increasing attention to fulfill the desire to enhance the fracture toughness of epoxy composites. However, challenges remain to improve their dispersibility in polymers and increase interaction ability. Thus, work is needed to synthesize alternative cost-effective 2D carbon nanofillers capable of delivering consistent performance as a reinforcer to monitor the fracture toughness of the epoxy composites. The present study demonstrates transforming graphite to ball-milled graphite (BMG) via an effective high-energy wet ball milling process. Herein a noteworthy size reduction is achieved for the BMG ranging from ∼217 to 227 nm. Microscopic investigation spotted an exfoliated 3D networked graphite nanosheet with nanopores. These BMGs were functionalized to attach amine-based silane moieties and were incorporated into the epoxy network. Consequently, even at higher loading levels, they showed their astonishing capability to enhance the crack far field resistance of nanocomposite resulting in significantly improved fracture toughness and energy to ∼2.31 MPa m1/2 and ∼11.30 kJ/m2, respectively. Improvement is ascribed to the better dispersing ability of BMG, which provides a consistent strong interfacial interaction with the epoxy network to modulate material resistance to fracture. Such environmentally friendly nanofillers must be industrially acceptable for synthesizing durable epoxy nanocomposite systems and can be utilized to prepare structural composites.

Ultrafine Ru nanoparticles stabilized by V8C7/C for enhanced hydrogen evolution reaction at all pH

The development of cost-effective electrocatalysts with high efficiency and long durability for hydrogen evolution reaction (HER) remains a great challenge in the field of water splitting. Herein, we design an ultrafine and highly dispersed Ru nanoparticles stabilized on porous V8C7/C matrix via pyrolysis of the metal–organic frameworks V-BDC (BDC: 1,4-benzenedicarboxylate). The obtained Ru-V8C7/C composite exhibits excellent HER performance in all pH ranges. At the overpotential of 40 mV, its mass activity is about 1.9, 4.1 and 9.4 times higher than that of commercial Pt/C in acidic, neutral and alkaline media, respectively. Meanwhile, Ru-V8C7/C shows the remarkably high stability in all pH ranges which, in particular, can maintain the current density of 10 mA cm−2 for over 150 h in 1.0 mol L−1 phosphate buffer saline (PBS). This outstanding HER performance can be attributed to the high intrinsic activity of Ru species and their strong interface interactions to the V8C7/C substrate. The synergistic effect of abundant active sites on the surface and the formed Ru–C–V units at the interface promotes the adsorption of reaction intermediates and the release of active sites, contributing the fast HER kinetics. This work provides a reference for developing versatile and robust HER catalysts by surface and interface regulation for pH tolerance.

Construction of fully coated polypyrrole oxygen-barrier film based on MXene nanosheets for high reliability capacitive deionization

MXene has emerged as a promising capacitive deionization (CDI) faradic material for the advantages of excellent hydrophilicity, outstanding specific capacitance, and highly reversible ions intercalation/de-intercalation. However, its practical applications are severely restricted by the bottleneck problems of severe self-stacking and susceptibility to be oxidized by dissolved oxygen in aqueous solution. Herein, polypyrrole (PPy) oxygen-barrier film was fabricated and fully coated on the surface of MXene by the in-situ polymerization method to construct the composite electrode of PPy@MXene. In this unique architecture, the PPy oxygen-barrier film both enhances the antioxidant properties of MXene and weakens the strong interfacial interactions between MXene nanosheets to reduce the self-aggregation. Meanwhile, by doping different ions (Cl– and dodecyl benzene sulfonate, DBS–), PPy films were provided with excellent conductivity, abundant hole sites, and good ion exchange properties, which significantly promoted the charge priority adsorption capability of PPy-Cl@MXene and PPy-DBS@MXene electrodes. Consequently, compared with MXene//MXene cell, the PPy-Cl@MXene//PPy-DBS@MXene CDI cell presents dominant deionization capacity (55 mg g−1) and outstanding cycling stability (3 % degradation after 40 cycles). Most importantly, the morphology, structure and surface charge characteristics of the electrodes after long-term desalination confirmed that the MXene with fully coated PPy film was not destroyed by dissolved oxygen and maintained good structural integrity, which is conducive to improving the reliability of the MXene-based electrodes in CDI. Additionally, ion doped PPy@MXene electrodes highlight preferential adsorption to divalent cations. The work proposes a new strategy to advance the practical application of MXene by simultaneously solving its self-stacking and oxidative degradation issues.

High fractal-dimensional carbon conductive agent for improving the Li storage performance of Si-based electrode

Constructing stable Si electrodes with high areal capacity is crucial for improving the total energy density of lithium ion batteries (LIBs). However, it remains challenging because the poor intrinsic conductivity and serious pulverization of Si usually lead to the active material falling-off from the conductive network. Herein, we demonstrate novel spatially extended graphene ribbons with a high fractal-dimension structure (HFGR-400), which can construct highly conductive and mechanically reinforced networks when used as the conductive agent for Si electrodes. The HFGR-400 added electrode shows 1.5–3.2 times higher conductivity and 1.4–2.3 times larger peeling strength than those of the commonly used carbon conductive agent added electrodes. Moreover, the flexible HFGR-400 ribbons with appropriate amount of functional groups ensure large contact area and strong interfacial interaction with Si particles, but without blocking the ion transport channels. Therefore, the HFGR-400 added Si electrode exhibits good cycle stability (2051.8 mAh/g after 200 cycles) and high rate performance. Moreover, the high Si mass loading HFGR-400 electrode shows a competitive areal capacity of 3.5 mAh cm−2 after 200 cycles, superior to most of the reported Si-based electrodes. Our work highlights the importance of conductive agents with high fractal-dimension structure for practical Si-based electrodes.

Chemically bonded interface construction of the covalent organic framework/CsPbBr3 heterojunction for efficient photocatalytic CO2 reduction driven by visible light

The Pb–N coordination in the TpBpy/CsPbBr3 NCs heterojunction with strong interfacial interactions, acts as a delivery channel that facilitates the migration of photogenerated carriers, improving the efficiency and stability of photocatalytic CO2RR.

Boosting charge transport in the BiVO4 photoanode interface modified with an aluminum hydroxide layer for solar water oxidation

Modifying BiVO4 with Al(OH)3 layers improved its PEC properties due to an increase of surface wettability. The strong interfacial interaction with H2O played a vital role in efficient charge carrier transportation on the BiVO4 interface.

Ultrasmall RuO2/CoFe2O4 nanoparticles with robust interfacial interactions for the enhanced acidic oxygen evolution reaction

Ultrasmall RuO2/CoFe2O4 nanoparticles with strong interfacial interactions exhibit enhanced oxygen evolution reaction (OER) performance, driven by efficient charge transfer between RuO2 and CoFe2O4.