Search Results (33)

The electrocatalytic CO₂ reduction reaction (CO₂RR) offers an energy-saving and environmentally friendly approach to producing hydrocarbon fuels. The use of a gas diffusion electrode (GDE) flow cell has generally improved the rate of CO₂RR, while the gas diffusion layer (GDL) remains a significant challenge. In this study, we successfully engineered a novel metal–organic framework (MOF) heterojunction through the controlled coating of zeolitic imidazolate framework (ZIF-L) on ultrathin nickel—metal–organic framework (Ni-MOF) nanosheets. This innovative architecture simultaneously integrates GDL functionality and exposes abundant solid–liquid–gas triple-phase boundaries. The resulting Ni-MOF@ZIF-L heterostructure demonstrates exceptional performance, achieving a formate Faradaic efficiency of 92.4% while suppressing the hydrogen evolution reaction (HER) to 6.7%. Through computational modeling of the optimized heterojunction configuration, we further elucidated its competitive adsorption behavior and electronic modulation effects. The experimental and theoretical results demonstrate an improvement in electrochemical CO₂ reduction activity with suppressed hydrogen evolution for the heterojunction because of its hydrophobic interface, good electron transfer capability, and high CO₂ adsorption at the catalyst interface. This work provides a new insight into the rational design of porous crystalline materials in electrocatalytic CO₂RR. Full article

A supercapacitor’s energy storage capability is greatly dependent on electrode materials. Layered double hydroxides (LDHs) were extensively studied as battery-type electrodes because of their 2D structure and quick intercalation/deintercalation of electrolyte ions. However, the energy storage capability for pristine LDHs is limited by their large aggregation tendency and poor electrical conductivity. Herein, a novel NiCoMn-LDH/SWCNTs (single-walled carbon nanotubes) composite electrode material, with ultrathin NiCoMn-LDH nanosheets dispersedly grown among the highly conductive networks of SWCNTs, was prepared via a facile zeolitic imidazolate framework-67 (ZIF-67)-derived in situ etching and deposition procedure. The NiCoMn-LDH/SWCNTs electrode demonstrates a specific capacitance as large as 1704.3 F g⁻¹ at 1 A g⁻¹, which is ascribed to its exposure of more active sites than NiCoMn-LDH. Moreover, the assembled NiCoMn-LDH/SWCNTs//BGA (boron-doped graphene aerogel) hybrid supercapacitor exhibits a superior capacitance of 167.9 F g⁻¹ at 1.0 A g⁻¹, an excellent energy density of 45.7 Wh kg⁻¹ with a power density of 700 W kg⁻¹, and an outstanding cyclic stability with 82.3% incipient capacitance maintained when subjected to 5000 charge and discharge cycles at the current density of 10 A g⁻¹, suggesting the significant potential of NiCoMn-LDH/SWCNTs as the electrode material applicable in supercapacitors. Full article

The development of functional materials and the use of nanotechnology are ongoing projects. These fields are closely linked, but there is a need to combine them more actively. Nanoarchitectonics, a concept that comes after nanotechnology, is ready to do this. Among the related research efforts, research into creating functional materials through the formation of thin layers on surfaces, molecular membranes, and multilayer structures of these materials have a lot of implications. Layered structures are especially important as a key part of nanoarchitectonics. The diversity of the components and materials used in layer-by-layer (LbL) assemblies is a notable feature. Examples of LbL assemblies introduced in this review article include quantum dots, nanoparticles, nanocrystals, nanowires, nanotubes, g-C₃N₄, graphene oxide, MXene, nanosheets, zeolites, nanoporous materials, sol–gel materials, layered double hydroxides, metal–organic frameworks, covalent organic frameworks, conducting polymers, dyes, DNAs, polysaccharides, nanocelluloses, peptides, proteins, lipid bilayers, photosystems, viruses, living cells, and tissues. These examples of LbL assembly show how useful and versatile it is. Finally, this review will consider future challenges in layer-by-layer nanoarchitectonics. Full article

Titanium silicon molecular zeolite (TS-1) plays an important role in catalytic reactions due to its unique nanostructure. The straight channel on TS-1 was parallel to the orientation of the short b-axis and directly exposed to the aperture of the 10-member ring with a diameter of 0.54 nm × 0.56 nm. This structure could effectively reduce the diffuse restriction of bulk organic compounds during the oxidative desulfurization process. As a kind of cationic polymer electrolyte, polydimethyldiallyl ammonium chloride (PDDA) contains continuous [C₈H₁₆N⁺Cl⁻] chain segments, in which the Cl⁻ could function as an effective structure-directing agent in the synthesis of nanomaterials. The chain of PDDA could adequately interact with the [0 1 0] plane in the preparation process of zeolite, and then the TS-1 nanosheet with short b-axis thickness (6 nm) could be obtained. The pore structure of the TS-1 nanosheet is controlled by regulating the content of PDDA. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), N₂ physical adsorption analysis, infrared absorption spectrum and ultraviolet–visible spectrum were used to determine the TS-1. The thinner nanosheets exhibit excellent catalytic performance in oxidative desulfurization of dibenzothiophene (DBT), in which the removal rate could remain at 100% after three recycles. Here, the TS-1 nanosheet with short b-axis thickness has a promising future in catalytic reactions. Full article

The design of earth-abundant and highly efficient bifunctional electrocatalysts for hydrogen evolution and oxygen evolution reactions (HER/OER) is crucial for hydrogen production through overall water splitting. Herein, we report a novel nanostructure consisting of vertically oriented CoP hierarchical nanosheet arrays with in situ-assembled carbon skeletons on a Ti foil electrode. The novel Zeolitic Imidazolate Framework-67 (ZIF-67) template-derived hierarchical nanosheet architecture effectively improved electrical conductivity, facilitated electrolyte transport, and increased the exposure of the active sites. The obtained bifunctional hybrid exhibited a low overpotential of 72 mV at 10 mA cm⁻² and a small Tafel slope of 65 mV dec⁻¹ for HER, and an improved overpotential of 329 mV and a Tafel slope of 107 mV dec⁻¹ for OER. Furthermore, the assembled C@CoP||C@CoP electrolyzer showed excellent overall water splitting performance (1.63 V) at a current density of 10 mA cm⁻² and superior durability. This work provides a structure engineering strategy for metal–organic framework (MOF) template-derived hybrids with outstanding electrocatalytic performance. Full article

Bio-oils derived from the pyrolysis of lignin-based biomass often contain a variety of oxygenated compounds, which can compromise their usefulness as a fuel. To improve the quality of bio-oil, catalytic hydrodeoxygenation (HDO) is a crucial step that removes oxygen from the oil in the form of water. In this study, we showed that MFI nanosheets are excellent supports for Ru-catalysts. We synthesized highly crystalline MFI nanosheets using a simple hydrothermal seeding procedure; the final material was obtained in 56 h of crystallization. We investigated the activity of Ru supported on different materials. Our findings indicated that Ru supported on hierarchical MFI demonstrated excellent activity in HDO of guaiacol. Our results demonstrated that Ru/ZNS-56 achieved nearly 100% selectivity towards cyclohexane under mild conditions (200 °C, 50 bar H₂, 1 h). Full article

This work first transformed hazardous aluminum waste into low-cost MgAl−layered double hydroxide@ANA zeolite (LDHs@ANA) composite for dye wastewater adsorption, which was meaningful for waste recovery and pollution control. Based on this strategy, the Al(OH)₃ extracted from secondary aluminum dross (a hazardous waste in the aluminum industry) was used as an aluminum source to synthesize LDHs@ANA composite, which had more excellent adsorption capacity to methylene blue than MgAl−LDHs and ANA alone. The composite consisted of spherical ANA particles uniformly covered with LDH nanosheets, which effectively avoided a large amount of aggregation between nanosheets and increased specific surface areas and pore volumes. The kinetic results indicated that the adsorption process conformed to the pseudo-second-order kinetic model, and the adsorption site was the main factor affecting the adsorption process. The equilibrium studies showed the adsorption process was exothermic, and the Langmuir model best fitted for the adsorption process, with a maximum adsorption capacity reaching 65.27 mg/g. Meanwhile, the effects of pH, adsorbent concentration, initial methylene blue concentration, and adsorption time on the LDHs@ANA were analyzed. Overall, this work provides a fresh concept for the preparation of low-cost adsorbents from aluminum waste. Full article

Single crystalline ZSM-5 ZNs with thicknesses around 6 nm were obtained by secondary growth of silicalite nanoparticles using diquaternary bis-1,5(tripropyl ammonium) pentamethylene diiodide (dC₅) as a structure-directing agent (SDA). The dC₅ could be effectively removed from the ZN pores by either high-temperature calcination or UV irradiation in air at room temperature but not by the piranha solution treatment. Ultrathin ZN-laminated membranes (ZNLMs) were fabricated by sandwiching a UV-activated multilayered ZN film between two recast Nafion^® layers (ZNLM-Nafion) and by filtration coating from a suspension of thermally activated ZNs on a nonionic porous PVDF (ZNLM-PVDF). The ZNLMs on both supports demonstrated the ability of highly proton-selective ion conduction with low resistances in aqueous electrolyte solutions. The ZNLM-PVDF with PVDF binder was structurally stable, and it achieved a comparably low ASR but much higher proton selectivity compared with a Nafion membrane of same overall thickness. However, detachment between the ZNLM and Nafion layers occurred when the ZNLM-Nafion operated in aqueous electrolyte solutions. Results of this study show the potential for developing ZNLMs as efficient proton-conducting membranes without using expensive ionic polymer matrices. However, the development of polymer-supported ZNLMs is hindered by the current inefficiency in preparing well-dispersed suspensions of open-pore ZNs. Future development of efficient methods for synthesizing open-pore ZNs in dispersed states is key to realizing high-performance ZNLMs on polymers. Full article

The excessively leached metal ions from traditional metallic antimicrobial nanoparticles are harmful to biological and human tissues. Metal-organic frameworks (MOFs) coordinating bioactive metal ions to organic bridging ligands can potentially address this issue, avoiding the excessive leaching of metal ions and simultaneously exhibiting high effective antibacterial activities. Here, we report the preparation of a 2-dimensional leaves-like zeolitic imidazolate framework (ZIF-L) for potential antibacterial and anti-algae applications. The ZIF-L nanosheet exhibits complete inactivation of Escherichia coli (phosphate buffer saline: 4 h) and Bacillus subtilis (seawater: 0.5 h). The ZIF-L/epoxy composite has excellent antibacterial effect, poisoning effect and anti-adhesion effect on a variety of marine algae. It is worth noting that the removal rate (Escherichia coli) for ZIF/epoxy composite can be reached to 90.20% by only adding ZIF-L (0.25 wt%). This work will inspire researchers to develop more metal-organic frameworks materials for applications in the antibacterial and anti-algae fields. Full article

Solar photocatalytic technology based on semiconducting materials has gained the attention of the scientific community to solve the energy crisis and environmental remediation. Zeolitic imidazolate frameworks (ZIFs) are a subfamily of metal–organic frameworks (MOFs) with the isomorphic topologies of zeolites and coordinative compositions of MOFs. Owing to high specific surface areas, tunable channels and high thermal stabilities, zeolitic imidazolate frameworks (ZIFs) have been used in catalytic applications. In this paper, ZIF-8 was used as a matrix to synthesize 0D/2D heterojunction photocatalysts, viz., ZnO/C₃N₄-x% (x = 2.5, 5 and 10), for the photocatalytic degradation study of rhodamine B (RhB). The synthesized composite materials were characterized using FTIR, PXRD, UVDRS, PL, TEM, and BET analyses. TEM images showed the nearby contacts between ZnO and C₃N₄ in the hybrid and the uniform distribution of ZnO on the surface of the C₃N₄ nanosheet, thus increasing the development of 0D/2D heterojunction. The hybrid system ZnO/C₃N₄-5% (ZCN-5) showed good photocatalytic activity for the degradation of RhB under sunlight. A possible mechanism for the improved photocatalytic activity of the ZnO/C₃N₄ composite is also suggested. This exploratory study demonstrates the effective separation and migration of photo-induced electron–hole pairs between the 2D C₃N₄ sheet and 0D ZnO for the improved performance of heterojunction photocatalysts. Full article

Copper oxide nanosheet-loaded zeolite 10X nanocomposites (CuO-zeolite NCs) were successfully prepared by modifying zeolite 10X with CuSO₄ aqueous solution. The formation of copper oxide nanosheets on the surface of zeolite 10X was observed by SEM. The thickness of CuO nanosheets was about 30–40 nm, and the width ranged from 200 nm to 300 nm. The XRD patterns showed that the new diffraction peaks of copper oxide appeared at 35.6° and 38.8°. According to the XPS results, the Cu 2p_3/2 and Cu 2p_1/2 peaks in CuO-zeolite NC were centered at 934.1 eV and 953.8 eV, which could be attributed to Cu(II). The EDS analysis revealed that the energy spectra of calcium gradually decreased as the copper ion concentration increased during the preparation of CuO-zeolite NCs. Meanwhile, the energy spectra of copper increased gradually, and the highest content of copper in CuO-zeolite NCs reached 22.35 wt.%. The BET surface areas of zeolite 10X and CuO-zeolite NCs were 587 and 363 m²/g, respectively, based on the N₂ adsorption–desorption experiment. The antibacterial activities of CuO-zeolite NC were evaluated using Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus). The antibacterial activities were related to both copper ion content in CuO-zeolite NCs and the particle size of copper oxide. The results showed that nano CuO-loaded zeolite 10X inhibited the activity of E. coli and S. aureus. CuO-zeolite NCs are expected to be further used in antifouling coating. Full article

In this work, a novel three-dimensional (3D) hollow nickel-cobalt layered double hydroxide (NiCo-LDH) was synthesized using zeolitic imidazole framework-67 (ZIF-67) as a template, and then utilized to functionalize molybdenum disulfide (NiCo-LDH/MoS₂) via electrostatic force. Flame retardant thermoplastic polyurethane (TPU) composites were prepared by the melt blending method. Compared to pure TPU, NiCo-LDH/MoS₂ filled TPU composite was endowed with a decrease of 30.9% and 55.7% of the peak heat release rate (PHRR) and the peak smoke production rate (PSPR), respectively. Furthermore, the addition of NiCo-LDH/MoS₂ can significantly improve the thermal stability and char yield of the TPU composite. The catalytic carbonization effect and dilution effect of NiCo-LDH, and the barrier effect of MoS₂ nanosheets enable TPU composites with excellent flame retardancy and toxic gas suppression ability. Full article

The Co₃O₄ electrode is a very promising material owing to its ultrahigh capacitance. Nevertheless, the electrochemical performance of Co₃O₄-based supercapacitors is practically confined by the limited active sites and poor conductivity of Co₃O₄. Herein, we provide a facile synthetic strategy of tightly anchoring Co₃O₄ nanosheets to a carbon fiber conductive cloth (Co₃O₄@C) using the zeolitic imidazolate framework-67 (ZIF-67) sacrificial template via in situ impregnation and the pyrolysis method. Benefiting from the enhancement of conductivity and the increase in active sites, the binder-free porous Co₃O₄@C supercapacitor electrodes possess typical pseudocapacitance characteristics, with an acceptable specific capacitance of ~251 F/g at 1 A/g and long-term cycling stability (90% after cycling 5000 times at 3 A/g). Moreover, the asymmetric and flexible supercapacitor composed of Co₃O₄@C and activated carbon is further assembled, and it can drive the red LED for 6 min. Full article

The development of an effective strategy for synthesizing two-dimensional MFI zeolites has attracted more and more attention. Herein, nanosheet-stacked hierarchical ZSM-5 zeolite was obtained by a seed-assisted hydrothermal synthesis route using a small amount of [C₁₈H₃₇-N⁺(CH₃)₂-C₆H₁₂-N⁺(CH₃)₂-C₆H₁₂]Br₂ (C_18-6-6Br₂) as a zeolite structure-directing agent and triethylamine (TEA) as a zeolite growth modifier. By varying the molar ratio of C_18-6-6Br₂/TEA from 2.5/0 to 2.5/40, the morphologies and textural properties of the resultant HZ5-2.5/x catalysts were finely modulated. By increasing x from 5 to 40, the morphology of the HZ5-2.5/x changed from unilamellar assembly with narrow a–c plane to intertwined nanosheets with wide a–c plane and multilamellar nanosheets with house-of-cards morphology. The thickness of these nanosheets was almost 8–10 nm. In addition, selectivity to light olefins reached 70.7% for the HZ5-2.5/10 catalyst, which was 6.6% higher than that for CZSM-5 (64.1%). Furthermore, the MFI zeolite nanosheets exhibited better anticoking stability within the 60 h reaction time compared to conventional ZSM-5 zeolite, which could be attributed to the short diffusion path and hierarchical porosity. This work will provide valuable insights into the rational design of novel zeolite catalysts for the efficient cracking of hydrocarbons. Full article

Proper control of a 3d transition metal-based catalyst with advanced structures toward oxygen evolution reaction (OER) with a more feasible synthesis strategy is of great significance for sustainable energy-related devices. Herein, carbon nanotube interconnected NiCo layered double hydroxide rhombic dodecahedral nanocages (NiCo-LDH RDC@CNTs) were developed here with the assistance of a feasible zeolitic imidazolate framework (ZIF) self-sacrificing template strategy as a highly efficient OER electrocatalyst. Profited by the well-fined rhombic dodecahedral nanocage architecture, CNTs’ interconnected characteristic and structural feature of the vertically aligned nanosheets, the as-synthesized NiCo-LDH RDC@CNTs integrated large exposed active surface areas, enhanced electron transfer capacity and multidimensional mass diffusion channels, and thereby collaboratively afforded the remarkable electrocatalytic performance of the OER. Specifically, the designed NiCo-LDH RDC@CNTs exhibited a distinguished OER activity, which only required a low overpotential of 255 mV to reach a current density of 10 mA cm⁻² for the OER. For the stability, no obvious current attenuation was detected, even after continuous operation for more than 27 h. We certainly believe that the current extraordinary OER activity combined with the robust stability of NiCo-LDH RDC@CNTs enables it to be a great candidate electrocatalyst for economical and sustainable energy-related devices. Full article