Journal of Colloid and Interface Science最新文献

The limited transport of oxygen at the solid-liquid interface and the poor charge separation efficiency of single catalyst significantly impedes the generation of reactive oxygen species (ROS), thereby weakening the application potential of photocatalytic technology in water pollution control. Herein, a hollow porous photocatalytic aerogel sphere (calcium alginate/cellulose nanofibers (CA/CNF)) loaded BiOBr/Ti₃C₂, combining a favourable mass transfer structure with effective catalytic centers was firstly presented. The floatability and hollow pore structure facilitated rapid O₂ transfer via a triphase interface, thereby promoting the generation of ROS. The oxygen diffusion flux of aerogel spheres' upper surface in triphase system exhibited a 0.151 μmol·(m²·S)^-1 increase compared to that of the diphase one based on Finite element simulation (FEM). Furthermore, owing to the regulation of charge spatial distribution by Schottky junction of BiOBr/Ti₃C₂, internal electric field (IEF) of CA/CNF@BiOBr/Ti₃C₂ achieved 1.8-fold improvement compared with CA/CNF@BiOBr, thus enhancing the separation of photogenerated charges. Accordingly, the degradation efficiency and catalytic rate constant of moxifloxacin (MOX) by CA/CNF@BiOBr/Ti₃C₂ in triphase system have improved by 20.1% and 1.5 times compared to those of diphase system, respectively. Moreover, the potential to mineralize multiple quinolone antibiotics (FQs), high resistance to complex water disturbances and excellent stability were revealed in CA/CNF@BiOBr/Ti₃C₂. Besides, the triphase system based on CA/CNF@BiOBr/Ti₃C₂ confirmed the potential for large-scale water treatment application in 500 mL MOX circular flow, reaching 90% MOX removal within 120 min. This research clarifies the oxygen mass transfer mechanism and pathways to the enhanced ROS production in a triphase system, and provides new insights into designing efficient floatable photocatalyst and adaptive reaction devices for new pollutants remediation.

As a novel carbon-based material with two-dimensional (2D) characteristics, graphdiyne (GDY) shows great potential in constructing active catalytic sites due to its distinctive atomic configuration and sp/sp² conjugated hybrid two-dimensional networks. In this study, the layered GDY was synthesized using the ball milling method, and Zn_0.5Cd_0.5S/Graphdiyne/NiO (ZnCdS/GDY/NiO) composite was synthesized by in-situ composite and physical mixing method. The prepared ZnCdS/GDY/NiO has good photostability outstanding performance in photocatalytic hydrogen production. When exposed to 5 W of white light, the ZnCdS/GDY/NiO photocatalyst demonstrates a hydrogen production rate of 24.44 mmol·g^-1·h^-1, which was 8.4 times greater than that of pure Zn_0.5Cd_0.5S under the same conditions. Various characterization tests and theoretical calculations show that the improved photocatalytic efficiency resulted from the formation of a dual S-scheme heterostructure in the ZnCdS/GDY/NiO composite catalyst, which promoted the recombination of relatively useless photogenerated electron holes. Furthermore, strong photogenerated holes and electrons in the more positive valence band (VB) and the more negative conduction band (CB) were retained, which significantly improved the photogenerated carrier separation ability of the composite catalyst, and thus enhances the hydrogen evolution activity.

Aqueous Zn-ion batteries (AZIBs) have attracted widespread attention owing to the feature of low cost, inherent safety and eco-friendliness. However, the poor reversibility of Zn anode severely hinders the practical applicability of AZIBs. Separator modification is an effective way to functionalize the electrode/electrolyte interface and improve the cycling performance. Here, we propose a modified glass fiber separator with Au coating (Au@GF), which could realize uniform Zn²⁺ distribution at the electrode/electrolyte interface and regulate the plating/stripping behaviors, achieving a dense and homogenous deposition. Zn||Zn symmetric cells assembled with Au@GF separator demonstrate evidently prolonged cycle life over 1600 h at the current density of 5 mA cm^-2 and the capacity of 1 mAh cm^-2, while symmetric cells with GF fail in less than 40 h. Even at the condition of 15 mA cm^-2/3 mAh cm^-2, lifespan of Zn||Zn cells with Au@GF is extended to 750 h, which is more than 3 times compared with that of GF. The modified separator with highly conductive coating is capable of a longtime stable Zn plating/stripping. Moreover, an enhanced cycling performance is also detected in a series of full cells with different cathode materials. This work provides an easy and efficient approach to homogenize Zn²⁺ deposition.

The demand for lightweight heat dissipation design in highly miniaturized and portable electronic devices with high thermal density is becoming increasingly urgent. Herein, highly thermal conductive carbon nanotubes (CNTs) reinforced aluminum foam composites were prepared by catalyst chemical bath and subsequent in-situ growth approach. The dense CNTs show the intertwined structure features and construct high-speed channels near the surface of the skeletons for efficient thermal conduction, promoting the transport efficiency of heat flow. The regulation of the process leads to a proportion increase in the (1 1 0) crystal plane of the aluminum substrate. The calculation results of non-equilibrium molecular dynamics (NEMD) demonstrate that (1 1 0) crystal plane is conducive to enhancing thermal boundary conductance thus the desirable equivalent thermal conductivity is obtained in the model system. Moreover, the phonon behaviors at the heterointerface observed in phonon density of states spectrums (PDOS) show that the interface system with (1 1 0) crystal plane possesses the superior coupling effect suggesting the brilliant transmission capacity. The theoretical results of NEMD and PDOS provide a microscopic explanation for the high thermal conductivity observed in the prepared composites with a high content of Al (1 1 0) crystal plane. The composites exhibit a thermal conductivity of 30.63 W·m^-1·K^-1, improved by ∼300 % as compared to unmodified aluminum foam. The cooling efficiency of 28.63 % obtained in the composites indicates outstanding heat dissipative performance among other similar works. The composites prepared in the work could hold bright prospects for the thermal management field.

Interfacial hydrogen bonds are pivotal in enhancing proton activity and accelerating the kinetics of proton-coupled electron transfer during electrocatalytic oxygen reduction reaction (ORR). Here we propose a novel FeCr bimetallic atomic sites catalyst supported on a honeycomb-like porous carbon layer, designed to optimize the microenvironment for efficient electrocatalytic ORR through the induction of interfacial hydrogen bonds. Characterizations, including X-ray absorption spectroscopy and in situ infrared spectroscopy, disclose the rearrangement of delocalized electrons due to the formation of FeCr sites, which facilitates the dissociation of interfacial water molecules and the subsequent formation of hydrogen bonds. This process significantly accelerates the proton-coupled electron transfer process and enhances the ORR reaction kinetics. As a result, the catalyst FeCrNC achieves a remarkable half-wave potential of 0.92 V and exhibits superior four-electron selectivity in 0.1 M KOH solution. Moreover, the zinc-air battery assembled by FeCrNC demonstrates a high power density of 207 mW cm^-2 and negligible degradation over 240 h at a current density of 10 mA cm^-2.

Hydrogen is increasingly acknowledged as a viable alternative to traditional fossil fuels. However, the photothermal properties of CoFe₂S₄, a photocatalyst displaying metal-like behavior, have not been adequately explored in the context of photocatalytic H₂ generation. To improve photocatalytic hydrogen evolution, it is crucial to understand how to expedite the transfer of photogenerated electrons and the dissociation of H-OH bonds for enhanced hydrogen ion release. Herein, a type-II heterostructure was constructed between CoFe₂S₄ nanosheets and ZnIn₂S₄ nanoparticles, a non-precious metal photocatalyst, which effectively separates photogenerated carriers and holes. More importantly, the photothermal effect and localized surface plasmon resonance (LSPR) effects induced by CoFe₂S₄ improved the sluggish kinetics of water dissociation. The CoFe₂S₄/ZnIn₂S₄-5 photocatalyst achieved H₂ evolution rate of 6.84 mmol·g^-1·h^-1, and an apparent quantum efficiency of 15.6 % at 400 nm, significantly enhancing the efficiency of photocatalytic splitting for hydrogen production. This work advances the application of metal CoFe₂S₄ in solar-to-fuel conversion and offers valuable insights for designing semiconductor-based photothermally assisted photocatalytic systems.

Despite the ultrahigh theoretical energy density and cost-effectiveness, aprotic lithium-oxygen (Li-O₂) batteries suffer from slow oxygen redox kinetics at cathodes and large voltage hysteresis. Here, we well-design ultrafine Co nanoparticles supported by N-doped mesoporous hollow carbon nanospindles (Co@HCNs) to serve as efficient electrocatalysts for Li-O₂ battery. Benefiting from strong metal-support interactions, the obtained Co@HCNs manifest high affinity for the LiO₂ intermediate, promoting formation of ultrathin nanosheet-like Li₂O₂ with low-impedance contact interface on the Co@HCNs cathode surface, which facilitates the reversible decomposition upon charging. The mesoporous hollow nanospindles can provide abundant electron/ions transport channels to synergistically accelerate the formation and decomposition of discharge products. The Li-O₂ battery based on Co@HCNs displays remarkably reduced discharge/charge polarization of 0.92 V, impressive rate performance, and stable operation for 250 cycles. This work will provide a new avenue to design advanced oxygen electrocatalysts for high-performance Li-O₂ battery.

We report here a Bi₂WO₆/Ti₃C₂T_x@Ag (BT@Ag) photothermal photocatalyst for efficient CO₂ reduction with tunable CH₄ selectivity. Incorporation of Ti₃C₂T_x MXene creates well-defined heterointerfaces between Bi₂WO₆ and Ti₃C₂T_x and converts thermal energy upon light illumination via photothermal effect, which contributes to a mitigation of the recombination of photo-induced charge carries for a high electron mobility. Density functional theory calculations substantiate that Ti₃C₂T_x functions as the adsorption site and active center where the transferred electrons are effectively involved in CO₂ reduction for enhanced CH₄ selectivity. Moreover, the in situ deposited Ag nanoparticles demonstrate an exceptional surface plasmon resonance effect, giving rise to additional hot electrons that further benefits the CH₄ generation.

Employing metallic nanoclusters as cocatalysts for semiconductor-based photocatalysts and understanding their roles in enhancing photocatalytic performance is crucial. Herein, a nickel thiolate with cyclohexanethiol as the ligands (i.e. Ni₄(S-cy)₈, cy = cyclohexyl) was synthesized and developed as the cocatalyst for CdS to promote its photocatalytic activity for hydrogen evolution. With a 5 wt% cluster loading, the obtained samples achieve a hydrogen evolution efficiency of approximately 106 mmol g_cat^-1 h^-1 under visible light irradiation, which is five times higher than that of pure CdS. The enhanced catalytic activity is attributed to the removal of ligands from the nickel clusters during photocatalysis, which allows the nickel clusters to embed themselves onto the CdS surface through Ni-S bond interactions. This process generates nickel species on the CdS surface, facilitating the generation and separation of photoinduced electron-hole pairs and thereby enhancing photocatalytic performance. This work highlights the importance of the dynamic evolution of nanoclusters during catalysis and demonstrates the potential of leveraging catalytically inert species to form highly efficient component for photocatalysis.

Transition metal oxides (TMOs) can accelerate the sluggish kinetics of vanadium redox reaction, but face challenges like limited active sites and difficulties in nanometerization, highlighting the urgent need for new TMO electrocatalysts for vanadium redox flow battery (VRFB). CoMoO₄ features high electrochemical activity, numerous redox sites, flexible control, and short electron pathways. Herein, a high catalytic and super stable graphite felt electrode modified in situ with network cross-linking CoMoO₄ nanosheets (CoMoO₄@GF) was prepared via hydrothermal and heat treatment method to enhance VRFB performance. CoMoO₄@GF have large specific surface area, super hydrophilicity, and abundant reaction places, possessing well mass transfer, low charge transfer resistance, and sufficient catalytic sites. Therefore, the composite electrodes exhibit great electrocatalytic activity towards VO²⁺/VO₂⁺ and V³⁺/V²⁺ redox reactions and excellent stability for VRFB. At 200 mA cm^-2, the energy efficiency (EE) of the CoMoO₄@GF modified VRFB improved by 19.14 % over the blank VRFB with pristine graphite felt, and remained cycle stable after 350 cycles at 150 mA cm^-2. This work not only enriches the types of TMOs catalysts in VRFB, but also opens up a new direction for the research of bimetallic TMOs.