Porous Nanosheets Research Articles

Stable Cu (I) single copper atoms supported on porous carbon nitride nanosheets for efficient photocatalytic degradation of antibiotics

Stable Cu (I) single copper atoms supported on porous carbon nitride nanosheets for efficient photocatalytic degradation of antibiotics

Hierarchical Nanowire Host Material for High‐Areal‐Capacity All‐Solid‐State S/SeS2 Batteries

AbstractAll‐solid‐state sulfur batteries (ASBs) suffer from electrical and ionic conduction problems due to the insulating sulfur. By comparing three host materials with different structural characteristics, herein, carbon nanotubes (CNTs) decorated with a conductive metal sulfide (CoMoS2@CNT) is demonstrated, designed to host sulfur and exchange both Li‐ions and electrons, effectively. In this hierarchical wire structure, porous CoMoS2 nanosheets form close interfaces with sulfur, and the CNT core directly transfers electrons to the sulfur‐impregnated CoMoS2. Simultaneously, the solid electrolyte positioned on the outer region of the nanowire material ensures facile Li‐ion conduction to the sulfur‐impregnated CoMoS2. An ASB featuring a CoMoS2@CNT host material with a sulfur loading of 3 mg cm−2 exhibits a high‐areal‐capacity of 4.5 mAh cm−2 at a current density of 2.5 mA cm−2, while retaining 79.4% of its initial capacity after 300 cycles. When sulfur is replaced with SeS2 to further reinforce the charge conduction properties, all‐solid‐state SeS2 batteries (ASeS2Bs) with an extremely high‐areal‐capacity of 16.3 mAh cm−2 retain 99.3% of their initial capacities after 60 cycles at 60 °C. This study provides guidelines for the design principles of cathode composites for the ASBs and ASeS2Bs through multiangle comparative analysis.

Performance study of bimetallic Mn-Zn porous flower-like nanosheets as supercapacitor positive electrode materials

As environmental and carbon emission issues become increasingly severe, electrochemical energy storage systems have gained attention. Compared to traditional supercapacitors, zinc-ion hybrid capacitors (ZIHCs) are not only environmentally friendly but also cost-effective. MnO2, with its low cost, eco-friendliness, high theoretical capacity, and stable crystal structure, is considered a promising positive electrode material. In this study, the morphology of MnO2 was optimized using electrodeposition. During cycling, zinc ions reversibly intercalate and extract from MnO2, forming a cactus-like nanoflower structure. This structure is loose and porous, providing ample reaction space for active materials. The assembled device exhibits excellent performance in both energy density (85.68 Wh kg−1) and stability (91.60 %).

Bimetal anchoring porous MXene nanosheets for driving tandem catalytic high‐efficiency electrochemical nitrate reduction

AbstractElectrochemical nitrate reduction reaction (NO3RR) is considered a promising strategy for ammonia synthesis and nitrate removal, in which catalyst development is crucial. Herein, a series of bimetal (Co and Cu) anchoring porous MXene nanosheets (CoxCuy@PM) catalysts were prepared by combining etching and reduction strategy. On the one hand, Cu and Co bimetals provided tandem catalytic active sites for NO3RR. On the other hand, the in‐plane PM exhibited good electrical conductivity and multiple transport pathways. Consequently, the optimized Co7Cu3@PM catalyst achieved a high ammonia yield of 7.43 mg h−1 mg cat.−1 and an excellent Faraday efficiency (FE) of 95.9%. The mechanism of NO3RR was investigated by analyzing electrolysis products and in situ Fourier transform infrared spectroscopy. Furthermore, the Co7Cu3@PM based ZnNO3− battery exhibited the superior power density of 5.59 mW cm−2 and an NH3 FE of 92.3%. This work presents an effective strategy to design MXene‐based high‐performance NO3RR electrocatalysts.

Hierarchically Structured CuNiP/CuOx‐VP Nanoarrays Construction by Heteroatom Doping Boosting Glycerol Valorization at Industrial‐Level Current Density

AbstractElectrocatalytic valorization of glycerol to formate is considered to be a promising sustainable approach; however, it holds great challenges to increase catalyst activity and deliver market‐demanded chemicals with high Faradaic efficiency (FE) and selectivity under industrial‐level current density. Herein, hierarchically structured phosphorus vacancy‐enriched nickel phosphide porous nanoarrays by copper doping, denoted as CuNiP/CuOx‐VP, are constructed via a facile glycol‐mediated solvothermal approach. The CuNiP/CuOx‐VP yields an industry‐level 1 A cm−2 at the ultralow potential of 1.75 V, while showing notable FE (96.94%) and selectivity (96.76%) to formate over a wide range of potentials. Impressively, a two‐electrode electrolyzer linked to H2 evolution possesses exceptional activity that merely requires a cell voltage of 1.45 V to deliver 40 mA cm−2, exhibiting a high FE (97.53%) for formate production and surpassing the vast majority of previously reported precious metal electrocatalysts. Microscopic and electrochemical characterizations manifest that the CuNiP/CuOx‐VP composed of porous NiP nanosheets attached to aggregated CuOx particles featuring superaerophobic‐hydrophilic morphology enables increased active sites, favorable electronic redistribution, and thus boosted electrocatalytic performance. This study demonstrates an effective nanoarrays electrode for catalyst discovery, going from facile catalyst synthesis to structure‐activity relationship and subsequently developing more highly active electrocatalysts for energy‐saving coproduction of valuable chemicals.

Molten Salt-Assisted Synthesis of Ferric Oxide/M-N-C Nanosheet Electrocatalysts for Efficient Oxygen Reduction Reaction.

Efficient, stable, and low-cost oxygen reduction catalysts are the key to the large-scale application of metal-air batteries. Herein, high-dispersive Fe2O3 nanoparticles (NPs) with abundant oxygen vacancies uniformly are anchored on lignin-derived metal-nitrogen-carbon (M-N-C) hierarchical porous nanosheets as efficient oxygen reduction reaction (ORR) catalysts (Fe2O3/M-N-C, M═Cu, Mn, W, Mo) based on a general and economical KCl molten salt-assisted method. The combination of Fe with the highly electronegative O induces charge redistribution through the Fe-O-M structure, thereby reducing the adsorption energy of oxygen-containing substances. The coupling effect of Fe2O3 NPs with M-N-C expedites the catalytic activity toward ORR by promoting proton generation on Fe2O3 and transfer to M-N-C. Experimental and theoretical calculation further revealed the remarkable electronic structure evolution of the metal site during the ORR process, where the emission density and local magnetic moment of the metal atoms change continuously throughout their reaction. The unique layered porous structure and highly active M-N4 sites resulted in the excellent ORR activity of Fe2O3/Cu-N-C with the onset potential of 0.977V, which is superior to Pt/C. This study offers a feasible strategy for the preparation of non-noble metal catalysts and provides a new comprehension of the catalytic mechanism of M-N-C catalysts.

Heterointerface engineering in mesoporous g-C3N4@MnFe2O4 photocatalysts for superior hydrogen (H2) evolution

Surfaces and interfaces play a pivotal role in heterostructures-based photocatalysts, which regulate the transfer, separation, and migration of photogenerated charge carriers. In this study, p-type MnFe2O4 nanoparticles (NPs) with complementary band structures were purposefully integrated with n-type porous g-C3N4 nanosheets (NSs) through precise interface engineering. The synergies in the g-C3N4@MnFe2O4 nanocomposites (NCs), leading to performance enhancement and functionalities, arise from their optimized mass fractions within the composite. The heterojunction interface formed in NCs possesses uniformly distributed mesopores (<4 nm), abundant active sites, and a high specific surface area (116 m2/g). Mesoporous heterojunctions improve photocatalytic activity by promoting the transfer of photogenerated electrons and holes to the photocatalyst surface. Notably, the optimized NCs, containing 20 wt% MnFe2O4, display the highest hydrogen evolution rate of 3.17 mmol g⁻¹ h⁻¹ (with methanol) and 5.77 mmol g⁻¹ h⁻¹ (with triethanolamine), which is many folds higher than bare MnFe2O4 and porous g-C3N4, using 1.0 wt.% of Pt as co-catalyst. The enhanced performance is corroborated by the efficient separation of photoinduced charge carriers, facilitated by an induced internal electric field arising from the Fermi level differences between the semiconductors. This study provides new insights into the advantages of designing and constructing mesoporous Z-scheme heterojunction photocatalysts for hydrogen evolution.

Oxygen-doped Porous Ultrathin Graphitic Carbon Nitride Nanosheets for Photocatalytic Hydrogen Evolution and Rhodamine B Degradation.

Graphite phase carbon nitride (g-C3N4) is a highly promising metal-free photocatalyst. However, its applicability is restricted by low activity, due to weak quantum efficiency and small specific surface area. Exfoliating bulk crystals into porous thin-layer nanosheets and introducing element doping have been shown to improve photocatalytic efficiency, but these methods are often complex, time-consuming, and costly processes. In this study, we successfully synthesized porous oxygen-doped g-C3N4 (OCN) nanosheets utilizing a straightforward method. Our findings show that OCN have much higher light absorption and visible-light photocatalytic activity than bulk g-C3N4 (BCN) and nonporous g-C3N4 (CN). The OCN photocatalyst has a remarkable hydrogen evolution reaction (HER) rate of 8.02 mmol·g-1 h-1, which is 8 times greater than BCN. Additionally, the OCN shows a high degradation rate of 97.3% for Rhodamine B (RhB). This enhanced photocatalytic activity is ascribed to the narrow band gap and superior electron transfer capacity. Our findings suggest a potential technique for generating efficient g-C3N4 photocatalysts.

π-Conjugated Porous Polymer Nanosheets for Explosive Sensing: Investigation on the Role of H-Bonding.

Nitroaromatic explosive sensing plays a critical role in ensuring public security and environmental protection. Herein, we report 2-pyridyl-thiazolothiazole (pyTTz) integrated blue-fluorescent π-conjugated porous polymer nanosheets, NTzCMP and TzCMP for selective sensing of picric acid (PA) among nitrophenol explosives. Acid-base interactions between PA and pyTTz of CMP lead to H-bonding interactions, where the hydroxy group of PA engaged in weak H-bonding interactions with pyridine and TTz of pyTTz moiety. This led to a strong fluorescence quenching of CMPs-such formation of ground state complex was supported by linear Stern-Volmer quenching plots, unaltered excited state lifetimes, and detailed FTIR analysis of PA exposed CMPs. Interestingly, both CMPs exhibited an excellent response to smaller analytes such as o-nitrotoluene compared to electron-deficient 2,4-dinitrotoluene. Both NTzCMP and TzCMP CMPs exhibited high KSV values of 9×103 and 2.1×103 M-1 for PA and the corresponding limit of detection values were found to be 0.46 and 1.6 ppm, respectively.

Microwave-assisted CuO-modified porous ZnO nanosheet for photocatalytic degradation of organic pollutants and antibacterial inactivation

The present study investigated the development of a porous ZnO/CuO photocatalyst for photocatalytic dye degradation and antibacterial inactivation of bacteria. Porous ZnO nanosheets are prepared by calcinating inorganic-organic ZnS(en)0.5. Further, CuO was integrated on a porous ZnO nanosheet using the microwave (MW)-assisted synthesis technique. Additionally, the effect of CuO at different concentrations on the photocatalytic activity of CuO/ZnO was investigated. Under 1.5G light illumination, an optimized ZnO/CuO-5 photocatalyst exhibited higher degradation efficiencies of 99.3%, 98%, and 99% for orange II dye, methylene blue (MB), and Eosin-Y respectively. The optimized photocatalyst exhibited inactivation efficiencies of 98% and 90% towards Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) bacteria, after 3h. The enhanced photocatalytic activity was attributable to a porous structure, extended visible light responsiveness, and delayed electron-hole recombination in nanostructured CuO/ZnO photocatalysts. Moreover, radical scavenger tests confirmed that superoxide radicals (•O2−) accompanied most degradation, followed by holes (h+) as minor factors. Our work suggests a simple photocatalytic interfacial engineering technique based on porous ZnO/CuO nanostructures to decompose organic chemicals and inactivate microorganisms in wastewater sources.

Construction of 2D/2D heterostructure with porous few layer g-C3N4 and NiCo2O4 nanosheets towards electromagnetic wave absorption

Developing high-performance materials with ultra-high reflection loss (RL ≤ -65 dB) for electromagnetic wave (EMW) absorption is pivotal to address electromagnetic pollution, but it is still challenging. Herein, a two-dimensional (2D)/2D PFL g-C3N4/NiCo2O4 heterostructure with porous few-layer g-C3N4 (PFL g-C3N4) and ultrathin NiCo2O4 nanosheets has been prepared by self-assembly, hydrothermal reaction, and calcination strategies. The 2D/2D heterostructure exhibits extraordinary EMW absorption property, achieving a reflection loss (RL) value of -68.59 dB and an effective absorption bandwidth (EAB) of 1.92 GHz at a matching thickness of 2.5 mm. As expected, the porous few layer g-C3N4 nanosheets provide rich interface which increases multiple reflection paths and enhances the conduction loss. The cooperative effects of magnetic loss, dielectric loss, and impedance matching contribute to the exceptional EMW absorption property of PFL g-C3N4/NiCo2O4 (2D/2D) heterostructure. The potential of PFL g-C3N4/NiCo2O4 in actual radar stealth is verified through radar scattering cross-section (RCS) simulation. This work paves the way for utilizing 2D/2D heterostructure as an ultra-efficient EMW absorbers.

Porous fluorine-cerium nanosheets anchored with FeOOH quantum dots for synergistic enhanced visible-light-driven photo-Fenton degradation of phenol

The utilization of two-dimensional (2D) materials to construct heterogeneous catalysts provides opportunities for environmental remediation, while the incorporation of porous structures can further enhance catalytic performance. In this work, a porous 2D FeOOH/fluorine-cerium (F-Ce) nanosheet composite was designed and synthesized by a simple impregnation-precipitation method. The unique 2D porous structure of F-Ce promoted the high dispersion of FeOOH quantum dots (QDs) (∼1.4 nm) and their tight integration to form S-scheme heterojunctions. This structure offered a greater number of active sites, and significantly improved the capacity of light absorption and the separation and migration efficiency of photogenerated carriers, thus improving catalytic activity. This catalyst achieved a phenol removal rate of 98.1 % within 20 min during the photo-Fenton reaction, which significantly surpasses pure FeOOH (32.9 %) and F-Ce (21.7 %) alone. In particular, the optimized 14FeOOH/F-Ce catalyst achieved more than 95.0 % degradation efficiency within a remarkably short period of 5 min. Mott Schottky and in situ irradiated X-ray photoelectron spectroscopy (ISI-XPS) studies demonstrated that the S-scheme charge transfer mechanism of this heterojunction synergistically enhanced the catalytic activity of the Fenton-like reaction. This study provides valuable insights for designing efficient 2D porous heterojunction catalysts for visible-light-driven Fenton applications.

Pd nanocubes supported on the porous V2CTx nanosheets with enhanced nanozyme activity and photothermal property for antibacterial application

Rational design and controllable construction of supported nanostructures with excellent antibacterial property remain a great challenge. Recently, transition metal carbides/nitrides/carbonitrides (MXenes) have attracted much interest in many fields due to their large specific surface areas and good photothermal property. Herein, a simple yet effective surface engineering strategy based on the tuning of MXene surface chemistry is presented, which allows in-situ controlled growth of the Pd nanocubes on the V2CTx nanosheets. Briefly, the exfoliated V2CTx nanosheets by HF are annealed, which changes the composition of surface terminations while creating the mesoporous structures. The annealing largely affects the exposure and oxidation states of the adjacent V atoms and allows the controllable growth of Pd nanocubes. Interestingly, the obtained Pd@V2CTx nanocomposites show enhanced peroxidase-/oxidase-like activities and intrinsic photothermal effect in the near infra-red (NIR) region due to the strong metal-support interaction. Furthermore, the combined nanocatalytic-photothermal treatment by their versatilities remarkably improves the antibacterial efficacy, giving a high killing rate (above 98 % for both Escherichia coli and Staphylococcus aureus). This work provides a new avenue to develop the supported metal nanostructures based on MXenes for antibacterial application.

An explore method for quick screening biomarkers based on effective enrichment capacity and data mining

Protein glycosylation acts as a crucial role in regulating protein function and maintaining cellular homeostasis. Efficient peptide enrichment can be utilized to effectively solve the inherent challenges of protein glycosylation analysis to search unknown cancer biomarkers. In this research, a low dimensional porous hydrophilic nanosheets with a multi-level porous structure (Co-MOF-SiO2@HA) was synthetized via an easy one-pot method for the efficient enrichment of the N-glycopeptides in the digests of complex biosamples. The synthetized nanosheets Co-MOF-SiO2@HA demonstrated excellent enriching performances including a high enrichment capacity (300 mg g-1 calculated), a spectacular selectivity (IgG digests and BSA digests at the molar ratio of 1/1200), and an excellent spatial confinement ability (IgG digests, IgG and BSA at the molar ratio of 1/1000/1000). As an explore result, after the enrichment of human colorectal cancer tissue and human healthy tissue by the nanosheets, several proteins related to cancers and one protein directly related to well-known human colorectal cancer were identified by detecting the corresponding glycopeptides. It presented the potential value of the feasibility of this analysis mode by nanosheets Co-MOF-SiO2@HA in proteomic analysis.

Construction of g-C3N4-based donor-acceptor conjugated copolymer for photocatalytic selective oxidation of biomass-derived 5-hydroxymethylfurfural under visible light

Donor-acceptor structure porous nanosheets CNSA-x (x denotes the amount of salicylic acid) were prepared by co-thermal condensation polymerization of aromatic compound salicylic acid (SA) and prepolymer melamine. A variety of characterization methods have been used to thoroughly analyze the morphology, structure, optical and electrical features of the synthesized catalysts. It turned out that the introduction of SA promotes the formation of pore structure and an enhanced specific surface area, which resulted in more reactive sites. Moreover, the introduction of SA improves light absorption capacity and effectively adjusts the valence band position. Meanwhile, it also extends the delocalization system, thereby promoting the migration and separation of photogenerated electron-hole pairs. The catalyst exhibited high performance and stability in the photocatalytic oxidation of 5-hydroxymethylfurfural (HMF) under the synergies of these advantages. Additionally, the elucidation of active reaction species and proposed reaction mechanism enriched the understanding of the catalytic process.

Modulation of metal centers of MOF in-situ grown on lignin-derived carbon to enhance adsorption capacity and electrochemical sensing performance for bisphenol A

Metal-organic framework materials have unique advantages in providing active sites and shortening electron/proton transfer distances. Here, an efficient electrochemical sensing material LPC-700@NiCo-MOF has been obtained by in-situ growth of bimetallic NiCo-MOF on lignin-derived porous quasi-carbon nanosheets (LPC-700). Due to the electronic synergistic effect of bimetallic centers of NiCo-MOF, it has better electrochemical sensing performance for bisphenol A (BPA) than the monometallic MOF. The density of states and adsorption energies of monometallic and bimetallic MOF on BPA have been investigated by DFT theory, which further demonstrated that the bimetallic NiCo-MOF has better electrochemical performance and adsorption effect on BPA. The high-performance portable sensor based on LPC-700@NiCo-MOF has been able to quickly, sensitively and accurately detect BPA in water samples and food packaging. This strategy of metal-modulated MOF grown in-situ on conducting carbon-based materials to enhance electrochemical activity provides a method for application in electrochemical fields.

Unlocking Efficient Alkaline Hydrogen Evolution Through Ru-Sn Dual Metal Sites and a Novel Hydroxyl Spillover Effect.

Alkaline hydrogen evolution reaction (HER) has great potential in practical hydrogen production but is still limited by the lack of active and stable electrocatalysts. Herein, the efficient water dissociation process, fast transfer of adsorbed hydroxyl and optimized hydrogen adsorption are first achieved on a cooperative electrocatalyst, named as Ru-Sn/SnO2 NS, in which the Ru-Sn dual metal sites and SnO2 heterojunction are constructed based on porous Ru nanosheet. The density functional theory (DFT) calculations and in situ infrared spectra suggest that Ru-Sn dual sites can optimize the water dissociation process and hydrogen adsorption, while the existence of SnO2 can induce the unique hydroxyl spillover effect, accelerating the hydroxyl transfer process and avoiding the poison of active sites. As results, Ru-Sn/SnO2 NS display remarkable alkaline HER performance with an extremely low overpotential (12mV at 10mA cm-2) and robust stability (650h), much superior to those of Ru NS (27mV at 10mA cm-2 with 90h stability) and Ru-Sn NS (16mV at 10mA cm-2 with 120h stability). The work sheds new light on designing of efficient alkaline HER electrocatalyst.

Enhanced photocatalytic degradation of Cr (VI) and organic pollutants using novel 3D/2D MoS2/SnS2 heterostructures for water remediation

In this study, 3D flower-like MoS2 nanostructures were synthesized using a hydrothermal technique to form heterostructures with 2D porous SnS2 nanosheets. The resulting 3D/2D MoS2/SnS2 heterostructures were evaluated for their photocatalytic abilities in removing Cr (VI), tetracycline (TC), and methylene blue (MB) under simulated solar irradiation. The results demonstrate that the MoS2/SnS2 heterostructures significantly outperformed pristine MoS2 and SnS2 in photocatalytic efficiency. Specifically, the MoS2/SnS2 photocatalysts achieved 99.9% degradation of Cr (VI) within 50 min, 96% degradation of TC in the same timeframe, and 99.9% elimination of MB in just 10 min. The reduction rate constant for Cr (VI) reduction by MoS2/SnS2 photocatalysts was 0.117 min−1, surpassing that of pure SnS2 (0.007 min−1) and MoS2 (0.0034 min−1) by 16 and 30 times, respectively. This outstanding performance is attributed to the heterojunction formation between SnS2 and MoS2, which suppresses the recombination of photogenerated charge carriers and provides abundant reactive sites due to their large specific surface area. The proposed photodegradation mechanism illustrates the facilitated migration of photogenerated charge carriers under light irradiation, enabled by the energy band alignment at the MoS2/SnS2 interface. These findings represent a significant advancement in the development of photocatalysts based on 3D flower-like MoS2 and porous SnS2 nanostructures, offering promise for applications in wastewater treatment and environmental remediation.

Self‐assembly synthesis of oxygen and sulfur co‐doped porous graphitic carbon nitride nanosheets for boosting CO2 photoreduction

Graphitic carbon nitride (CN) has garnered considerable attention in the field of visible‐light CO2 photoreduction, but its efficiency remains limited by the intrinsic π‐conjugated skeleton. Here, O and S were co‐doped CN (O, S/CN) by a facile “hydrolysis + calcination” approach to modulate the physicochemical and electronic structure. Distinctive from S doped CN (SCN), O, S/CN owned porous layer structure with several nanosheets and less SO42‐ groups on the surface. The amount of heteroatom‐doping was achieved by changing the hydrothermal temperature. The optimum O, S/CN‐80 achieved moderate CO production rate of 1.29 μmol g‐1h‐1, which was 3.79 times as much as SCN (0.34 μmol g‐1h‐1). The O and most S atoms were substitutionally doped and the effect of S doped state on the improved efficiency of CO generation in O, S/CN was also explored based on the theoretical calculations. This work provides an inspiration to develop efficient dual‐doped CN photocatalysts for photocatalytic CO2 reduction.

Enhanced Phosphate Adsorption by Cerium-Doped Porous Boron Nitride Nanosheets

Enhanced Phosphate Adsorption by Cerium-Doped Porous Boron Nitride Nanosheets