Ultrathin TiS2@N,S-Doped Carbon Hybrid Nanosheets as Highly Efficient Photoresponsive Antibacterial Agents.

Nanobactericides are employed as a promising class of nanomaterials for eradicating microbial infections, considering the rapid resistance risks of conventional antibiotics. Herein, we present a pioneering approach, reporting the synthesis of two-dimensional titanium disulfide nanosheets coated by nitrogen/sulfur-codoped carbon nanosheets (2D-TiS2@NSCLAA hybrid NSs) using a rapid l-ascorbic acid-assisted sulfurization of Ti3C2Tx-MXene to achieve efficient alternative bactericides. The as-developed materials were systematically characterized using a suite of different spectroscopy and microscopy techniques, in which the X-ray diffraction/Raman spectroscopy/X-ray photoelectron spectroscopy data confirm the existence of TiS2 and C, while the morphological investigation reveals single- to few-layered TiS2 NSs confined by N,S-doped C, suggesting the successful synthesis of the ultrathin hybrid NSs. From in vitro evaluation, the resultant product demonstrates impressive bactericidal potential against both Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli bacteria, achieving a substantial decrease in the bacterial viability under a 1.2 J dose of visible-light irradiation at the lowest concentration of 5 µg·mL-1 compared to Ti3C2Tx (15 µg·mL-1), TiS2-C (10 µg·mL-1), and standard antibiotic ciprofloxacin (15 µg·mL-1), respectively. The enhanced degradation efficiency is attributed to the ultrathin TiS2 NSs encapsulated within heteroatom N,S-doped C, facilitating effective photogenerated charge-carrier separation that generates multiple reactive oxygen species (ROS) and induced physical stress as well as piercing action due to its ultrathin structure, resulting in multimechanistic cytotoxicity and damage to bacterial cells. Furthermore, the obtained results from molecular docking studies conducted via computational simulation (in silico) of the as-synthesized materials against selected proteins (ß-lactamasE. coli/DNA-GyrasE. coli) are well-consistent with the in vitro antibacterial results, providing strong and consistent validation. Thus, this sophisticated study presents a simple and effective synthesis technique for the structural engineering of metal sulfide-based hybrids as functionalized synthetic bactericides.

Biomineralization-Inspired Synthesis of Hybrid COF Nanosheets toward Efficient Desalination Membranes.

Synthesis of covalent organic framework nanosheets (CONs) with high aspect ratio is crucial to their assembly into advanced membranes. Nonetheless, the π-π stacking between covalent organic framework (COF) layers often leads to thick CONs. Herein, inspired by biomineralization process, a series of aspect ratio CONs >15 000 is synthesized by multifunctional polyelectrolytes which not only provide the nucleation sites for pre-assembly with COF monomer, but also suppress π-π interaction for anisotropic growth through protonation. The membrane assembled from CONs exhibited water permeance of 341 kg m-2 h-1 and salt rejection of 99.5% in desalination, outperforming ever-reported membranes. This method establishes a platform for the synthesis of crystalline nanosheets.

Molybdenum Disulfide/Nickel-Metal Organic Framework Hybrid Nanosheets Based Disposable Electrochemical Sensor for Determination of 4-Aminophenol in Presence of Acetaminophen.

The toxicity of commonly used drugs, such as acetaminophen (ACAP) and its degradation-derived metabolite of 4-aminophenol (4-AP), underscores the need to achieve an effective approach in their simultaneous electrochemical determination. Hence, the present study attempts to introduce an ultra-sensitive disposable electrochemical 4-AP and ACAP sensor based on surface modification of a screen-printed graphite electrode (SPGE) with a combination of MoS2 nanosheets and a nickel-based metal organic framework (MoS2/Ni-MOF/SPGE sensor). A simple hydrothermal protocol was implemented to fabricate MoS2/Ni-MOF hybrid nanosheets, which was subsequently tested for properties using valid techniques including X-ray diffraction (XRD), field emission-scanning electron microscopy (FE-SEM), energy dispersive X-ray spectroscopy (EDX), Fourier transformed infrared spectroscopy (FTIR), and N2 adsorption-desorption isotherm. The 4-AP detection behavior on MoS2/Ni-MOF/SPGE sensor was followed by cyclic voltammetry (CV), chronoamperometry and differential pulse voltammetry (DPV). Our experimental findings on the generated sensor confirmed a broad linear dynamic range (LDR) for 4-AP from 0.1 to 600 µM with a high sensitivity of 0.0666 µA/µM and a low limit of detection (LOD) of 0.04 µM. In addition, an analysis of real specimens such as tap water sample as well as a commercial sample (acetaminophen tablets) illuminated the successful applicability of as-developed sensor in determining ACAP and 4-AP, with an impressive recovery rate.

Stimulus-Responsive Ultrathin Films for Bioapplications: A Concise Review.

The term "nanosheets" has been coined recently to describe supported and free-standing "ultrathin film" materials, with thicknesses ranging from a single atomic layer to a few tens of nanometers. Owing to their physicochemical properties and their large surface area with abundant accessible active sites, nanosheets (NSHs) of inorganic materials such as Au, amorphous carbon, graphene, and boron nitride (BN) are considered ideal building blocks or scaffolds for a wide range of applications encompassing electronic and optical devices, membranes, drug delivery systems, and multimodal contrast agents, among others. A wide variety of synthetic methods are employed for the manufacturing of these NSHs, and they can be categorized into (1) top-down approaches involving exfoliation of layered materials, or (2) bottom-up approaches where crystal growth of nanocomposites takes place in a liquid or gas phase. Of note, polymer template liquid exfoliation (PTLE) methods are the most suitable as they lead to the fabrication of high-performance and stable hybrid NSHs and NSH composites with the appropriate quality, solubility, and properties. Moreover, PTLE methods allow for the production of stimulus-responsive NSHs, whose response is commonly driven by a favorable growth in the appropriate polymer chains onto one side of the NSHs, resulting in the ability of the NSHs to roll up to form nanoscrolls (NSCs), i.e., open tubular structures with tunable interlayer gaps between their walls. On the other hand, this review gives insight into the potential of the stimulus-responsive nanostructures for biosensing and controlled drug release systems, illustrating the last advances in the PTLE methods of synthesis of these nanostructures and their applications.

Supramolecular Precursor Strategy to Construct g-C3N4/Silica Hybrid Nanosheets for Photocatalytic Degradation of Dye and Antibiotic Pollutants.

To construct a highly active g-C3N4 (CN)/silica hybrid nanosystem, the supramolecular precursor strategy of introducing melamine-cyanuric acid (MCA) by synergistically using micromolecular melamine (m) and urea (u) for CN nanostructure construction on the silica nanosheets (SiNSs) surface was researched. The results showed that the introduction of MCA supramolecular aggregates promoted the generation of ordered CN nanostructures attached to SiNSs, and the morphology of the CN nanostructure could be regulated through the m/u mass ratio. When the ratio is equal to 1/30, a typical g-C3N4/silica hybrid nanosheet (mu-CN/SiNSs-3) was successfully prepared, which showed the ultra-high photocatalytic activity for Rhodamine B dye degradation within 25 min with an apparent rate constant of 0.186 min-1, owing to the large surface area of highly dispersed and ordered CN nanosheets, a strong interaction between CN and SiNSs, high photogenerated carriers separation efficiency, and the more negative conduction band potential offering more active species of 1O2 and •O2-. Unexpectedly, the mu-CN/SiNSs-2 composite (m/u = 1/10) exhibited the highest activity for tetracycline antibiotic degradation, mainly due to the morphological advantage of a certain number of nanotubes generated on the CN/SiNSs hybrid nanosheets. It indicates that the supramolecular precursor strategy by synergistically using melamine and urea is highly efficient for the nanostructure construction of the CN/SiNSs hybrid system, enabling an appropriate nanostructure for the photodegradation of various pollutants.

Biomimetic synthesis of protein-DNA-CaHPO4 hybrid nanosheets for biosensing: Detection of thrombin as an example.

Traditional strategies for coupling of proteins with DNA involve the additional modifications on protein or DNA to construct protein-DNA conjugates, resulting in complex or time-consuming coupling process. This study presented a biomimetic synthesis strategy to elaborately synthesize a new type of biomolecule-inorganic hybrid nanosheets. Horseradish peroxidase (HRP) and DNA aptamer can be easily combined with CaHPO4 via coprecipitation simultaneously to form all-inclusive HRP-aptamer-CaHPO4 hybrid (HAC) nanosheets integrating bifunction of biorecognition and signal amplification, which was proceeded in the green environment at room temperature and required no additional modifications on CaHPO4, protein and DNA. Therefore, it avoided tedious linking and purification procedures. The HAC nanosheets were then employed as the signal labels and showed excellent performance for detecting thrombin. This bioinspired approach provides great possibilities to facile and efficient immobilization of protein, DNA or even other types of biomolecules (e.g., RNA and peptide) on inorganic nanomaterials and endows great potential in the preparation of a variety of multifunctional biomolecule-CaHPO4 two-dimensional (2D) nanobiohybrids for various applications extending from biosensing to energy, biomedicine, environmental science and catalysis.

Hybrid MXene-Graphene/Hexagonal Boron Nitride Structures: Electronic and Molecular Adsorption Properties.

Recent advances in experimental techniques allow for the fabrication of hybrid structures. Here, we study the electronic and molecular adsorption properties of the graphene (G)/hexagonal boron nitride (h-BN)-MXenes (Mo2C) hybrid nanosheets. We use first-principles calculations to explore the structure and electronic properties of the hybrid structures of G-2H-Mo2C and h-BN-2H-Mo2C with two different oxygen terminations of the Mo2C surface. The embedding of G or h-BN patches creates structural defects at the patch-Mo2C border and adds new states in the vicinity of the Fermi energy. Since this can be utilized for molecular adsorption and/or sensing, we investigate the ability of the G-M-O1 and BN-M-O1 hybrid structures to adsorb twelve molecules. Generally, the adsorption on the hybrid systems is significantly higher than on the pristine systems, except for N2 and H2, which are weakly adsorbed on all systems. We find that OH, NO, NO2, and SO2 are chemisorbed on the hybrid systems. COOH may be chemisorbed, or it may dissociate depending on its location at the edge between the G/h-BN and the MXene. NH3 is chemisorbed/physisorbed on the BN/G-M-O1 systems. CO, H2S, CO2, and CH4 are physisorbed on the hybrid systems. Our results indicate that the studied hybrid systems can be used for molecular filtration/sensing and catalysis.

Thermal treatment for promoting interfacial interaction in Co-BDC/Ti3C2Tx hybrid nanosheets for hybrid supercapacitors.

The design and synthesis of high-performance metal-organic frameworks (MOFs)-based electrodes are important for hybrid supercapacitors (HSC). Herein, enhanced interfacial interaction in Co-BDC/Ti3C2Tx (denoted as CoTC) hybrid nanosheets is achieved through thermal treatment, giving remarkably improved capacity performance compared with CoTC. The low temperature annealing treatment enables modulation of the bridging bonds content of CoTC and thus regulates the interfacial coupling effect between Co-BDC and Ti3C2Tx. Moreover, both the detailed XPS and XANES analysis reveal that the strong interfacial interactions between the two components promote a partial electron transfer from Ti3C2Tx to Co-BDC through the Ti-O-Co interfacial bonds. Consequently, it endows the Co-BDC with enhanced conductivity as well as the higher valence of Ti species in Ti3C2Tx, hence contributes a remarkable enhanced specific capacity. This work will provide a pathway to design advanced MOF/MXene materials for HSC.

Hierarchical Octahedra Constructed by Cu2 S/MoS2 ⊂Carbon Framework with Enhanced Sodium Storage.

Metal sulfides have aroused considerable attention for efficient sodium storage because of their high capacity and decent redox reversibility. However, the poor rate capability and fast capacity decay greatly hinder their practical application in sodium-ion batteries. Herein, a self-template-based strategy is designed to controllably synthesize hierarchical microoctahedra assembled with Cu2 S/MoS2 heterojunction nanosheets in the porous carbon framework (Cu2 S/MoS2 ⊂PCF) via a facile coprecipitation method coupled with vulcanization treatment. The Cu2 S/MoS2 ⊂PCF microoctahedra with 2D hybrid nanosubunits reasonably integrate several merits including facilitating the diffusion of electrons and Na+ ions, enhancing the electric conductivity, accelerating the ion and charge transfer, and buffering the volume variation. Therefore, the Cu2 S/MoS2 ⊂PCF composite manifests efficient sodium storage performance with high capacity, long cycling life, and excellent rate capability.

Polyethyleneimine-Mediated Fabrication of Two-Dimensional Cobalt Sulfide/Graphene Hybrid Nanosheets for High-Performance Supercapacitors.

Two-dimensional (2D) hybrid nanosheets made of electrochemically active materials and graphene, featuring fast reaction kinetics and excellent structural stability, are appealing as electrodes for supercapacitors. Herein, we report a general polyethyleneimine (PEI)-mediated fabrication of the 2D cobalt sulfide/graphene hybrid nanosheets via a facile hydrothermal strategy. Detailed analysis reveals that the uniform cobalt sulfide (CoS) nanoparticles are well-anchored on the 2D graphene surface. Thereinto, the nitrogen species originating from the PEI molecules as bridging sites are helpful in enhancing the coupling effect between the graphene and CoS species, which endows the hybrid nanosheets with high electroactivity and excellent structural stability. The as-obtained hybrid nanosheets with typical pseudocapacitive features demonstrate a high specific capacitance (320 F g-1@1 A g-1) and a superior electrochemical stability with the initial capacitance of 86.5% after 20 000 cycles as electrodes for supercapacitors. The assembled asymmetric supercapacitors by combining activated carbon electrodes further show a high charge storage of 28.8 Wh kg-1 with an output power of 130 W kg-1. More importantly, the similar strategy can be easily extended to fabricate other 2D hybrid nanosheets with extraordinary electrochemical performance with the maximum charge storage of 815 F g-1 and energy density of 44. 6 Wh kg-1. The present work, which achieves the general fabrication of 2D hybrid nanosheets with tuned compositions, may provide a new opportunity for the development of supercapacitors.

Vertically Aligned N-Doped Diamond/Graphite Hybrid Nanosheets Epitaxially Grown on B-Doped Diamond Films as Electrocatalysts for Oxygen Reduction Reaction in an Alkaline Medium.

Diamond/graphite hybrid nanosheets (DGNSs) have been epitaxially grown on boron-doped diamond (BDD) films from CH4/H2 mixture gas by microwave plasma chemical vapor deposition. The DGNSs are vertically aligned on the crystal facets of the BDD films uniformly, densely, and orderly. The DGNSs are composed of the core diamond sheets and the surface graphitic overlayers, which possess an open edge structure. By posttreatment in NH3 atmosphere in a microwave plasma or a tube furnace, the N-doped DGNSs (NDGNSs) were obtained. The electrocatalytic performance toward oxygen reduction reaction (ORR) for the DGNSs was greatly enhanced after doping with N, and the doped pyridinic N contributes more to the ORR. The electrocatalytic activity for ORR of the NDGNSs doped at 650 °C in NH3 in a tube furnace is the highest in all of the samples, which is comparable to the commercial Pt/C. The present work provides a novel electrocatalyst for the ORR with high performance.

Nanocavity-in-Multiple Nanogap Plasmonic Coupling Effects from Vertical Sandwich-Like Au@Al2O3@Au Arrays for Surface-Enhanced Raman Scattering.

The development of ideal three-dimensional (3D) tailorable surface-enhanced Raman scattering (SERS) substrates with the properties of timesaving, large area, high throughput, single or few molecules detection, reproducibility, reusable ability, and high density of "hot spots" has been the mainstream challenge and the robust task. Here, we construct perpendicular sandwich-like Au@Al2O3@Au hybrid nanosheets (PSHNs) on the Al foil as a 3D flexible substrate for SERS. The design of 3D PSHNs incorporates several advantageous aspects for SERS to enhance the performance of plasmonic diamers via bifunctions of vertical Al2O3 nanosheets (NSs) including the nanoscaffold and nanobaffle plate effects. As a nanoscaffold, it increases the space utilization of Au-Au diamers, whereas as a nanobaffle, it forms densely homogeneous Au@Al2O3@Au nanojunctions by sub-4 nm thickness of Al2O3 NSs as the dielectric isolated layer for the double-sided exposure of slitlike surface plasmon resonance. The optimized PSHN substrate exhibits a fascinating SERS sensitivity with an experimental enhancement factor of 1012 and is able to detect rhodamine B at an extremely low concentration up to the limit of single or few molecules (10-18 M), as well as can be recycled without the loss of SERS enhancement via the simple impregnation process. These advantages will greatly facilitate the wider use of SERS in many fields.

General One-Pot Synthesis of Transition-Metal Phosphide/Nitrogen-Doped Carbon Hybrid Nanosheets as Ultrastable Anodes for Sodium-Ion Batteries.

Sodium-ion batteries (SIBs) have been considered as promising energy storage devices in grid-level applications, owing to their largely reduced cost compared with that of lithium-ion batteries. However, the practical application of SIBs has been seriously hindered because of the lack of appropriate anode materials, limited by the thermodynamics perspective, which is one of the central task at current stage. Herein, we have developed a general one-pot strategy for the synthesis of transition-metal phosphide (TMP) based hybrid nanosheets composed of carbon-coated TMP nanoparticles anchored to the surface of nitrogen-doped carbon nanosheets. This facile and cost-effective method is quite universal and holds potential to be further extended to other metal phosphide materials. Significantly, the hybrid nanosheet electrode possesses excellent sodium storage properties as anodes for SIBs, including high specific capacity, an ultra-long cycle life and a remarkable rate performance. This work makes a significant contribution to not only the synthetic methodology of TMP-carbon two-dimensional hybrid nanostructures, but also the application of TMP-based anodes for high-energy SIBs.

Atomically Thin Mesoporous Co3 O4 Layers Strongly Coupled with N-rGO Nanosheets as High-Performance Bifunctional Catalysts for 1D Knittable Zinc-Air Batteries.

Under development for next-generation wearable electronics are flexible, knittable, and wearable energy-storage devices with high energy density that can be integrated into textiles. Herein, knittable fiber-shaped zinc-air batteries with high volumetric energy density (36.1 mWh cm-3 ) are fabricated via a facile and continuous method with low-cost materials. Furthermore, a high-yield method is developed to prepare the key component of the fiber-shaped zinc-air battery, i.e., a bifunctional catalyst composed of atomically thin layer-by-layer mesoporous Co3 O4 /nitrogen-doped reduced graphene oxide (N-rGO) nanosheets. Benefiting from the high surface area, mesoporous structure, and strong synergetic effect between the Co3 O4 and N-rGO nanosheets, the bifunctional catalyst exhibits high activity and superior durability for oxygen reduction and evolution reactions. Compared to a fiber-shaped zinc-air battery using state-of-the-art Pt/C + RuO2 catalysts, the battery based on these Co3 O4 /N-rGO nanosheets demonstrates enhanced and stable electrochemical performance, even under severe deformation. Such batteries, for the first time, can be successfully knitted into clothes without short circuits under external forces and can power various electronic devices and even charge a cellphone.

Sensitive Chronocoulometric Detection of miRNA at Screen-Printed Electrodes Modified by Gold-Decorated MoS2 Nanosheets.

Developing novel simple and ultrasensitive strategies for detecting microRNAs (miRNAs) is highly desirable because of their association with early cancer diagnostic and prognostic processes. Here a new chronocoulometric sensor, based on semiconducting 2H MoS2 nanosheets (MoS2 NSs) decorated with a controlled density of monodispersed small gold nanoparticles (AuNPs@MoS2), was fabricated via electrodeposition, for the highly sensitive detection of miRNA-21. The size and interparticle spacing of AuNPs were optimized by controlling nucleation and growth rates through the tuning of deposition potential and Au precursor concentration and by getting simultaneous feedback from morphological and electrochemical activity studies. The sensing strategy, involved the selective immobilization of the thiolated capture probe DNA (CP) at AuNPs and hybridization of CP to a part of the miRNA target, whereas the remaining part of the target was complementary to a signaling nonlabeled DNA sequence that served to amplify the target upon hybridization. Chronocoulometry provided precise quantification of nucleic acids at each step of the sensor assay by interrogating [Ru(NH3)6]3+ electrostatically bound to phosphate backbones of oligonucleotides. A detailed and systematic optimization study demonstrated that the thinnest and smallest MoS2 NSs improved the sensitivity of the AuNP@MoS2 sensor, achieving an impressive detection limit of ≈100 aM, which is 2 orders of magnitude lower than that of a bare Au electrode and also enhanced the DNA-miRNA hybridization efficiency by 25%. Such an improved performance can be attributed to the controlled packing density of CPs achieved by their self-assembly on AuNPs, large interparticle density, small size, and intimate coupling between AuNPs and MoS2. Alongside the outstanding sensitivity, the sensor exhibited an excellent selectivity down to femtomolar concentrations, for discriminating a complementary miRNA-21 target in a complex system composed of different foreign targets including mismatched and noncomplementary miRNA-155. These advantages make our sensor a promising contender in the point of care miRNA sensor family for medical diagnostics.

Growth of Au Nanoparticles on 2D Metalloporphyrinic Metal-Organic Framework Nanosheets Used as Biomimetic Catalysts for Cascade Reactions.

Inspired by the multiple functions of natural multienzyme systems, a new kind of hybrid nanosheet is designed and synthesized, i.e., ultrasmall Au nanoparticles (NPs) grown on 2D metalloporphyrinic metal-organic framework (MOF) nanosheets. Since 2D metalloporphyrinic MOF nanosheets can act as the peroxidase mimics and Au NPs can serve as artificial glucose oxidase, the hybrid nanosheets are used to mimic the natural enzymes and catalyze the cascade reactions. Furthermore, the synthesized hybrid nanosheets are used to detect biomolecules, such as glucose. This study paves a new avenue to design nanomaterial-based biomimetic catalysts with multiple complex functions.

Preparation of Ultrathin Two-Dimensional Tix Ta1-x Sy Oz Nanosheets as Highly Efficient Photothermal Agents.

Although two-dimensional (2D) metal oxide/sulfide hybrid nanostructures have been synthesized, the facile preparation of ultrathin 2D nanosheets in high yield still remains a challenge. Herein, we report the first high-yield preparation of solution-processed ultrathin 2D metal oxide/sulfide hybrid nanosheets, that is, Tix Ta1-x Sy Oz (x=0.71, 0.49, and 0.30), from Tix Ta1-x S2 precursors. The nanosheet exhibits strong absorbance in the near-infrared region, giving a large extinction coefficient of 54.1 L g-1 cm-1 at 808 nm, and a high photothermal conversion efficiency of 39.2 %. After modification with lipoic acid-conjugated polyethylene glycol, the nanosheet is a suitable photothermal agent for treatment of cancer cells under 808 nm laser irradiation. This work provides a facile and general method for the preparation of 2D metal oxide/sulfide hybrid nanosheets.

A novel bismuth oxychloride-graphene hybrid nanosheets based non-enzymatic photoelectrochemical glucose sensing platform for high performances.

A novel non-enzymatic photoelectrochemical (PEC) glucose sensor was first constructed based on the unique two-dimensional (2D) bismuth oxychloride-graphene nanohybrid sheets (BiOCl-G NHS). We have utilized a facile hydrothermal approach for the preparation of BiOCl-G NHS. Results from cyclic voltammetric and differential pulse voltammetric measurements revealed that the BiOCl-G NHS electrode is capable of generating photocurrent for glucose when its surface is irradiated with a light source (wavelength=365nm). The photocurrents produced for the presence of glucose at the bias potential of +0.50V showed a linear dependence on glucose concentration in the range between 0.5 and 10mM and had a detection limit of 0.22mM. The PEC detection of glucose at BiOCl-G NHS was not influenced by the presence of other common interfering species. The glucose levels, as determined by the BiOCl-G NHS sensor, agreed well with those obtained by the commercial glucometers. This novel non-enzymatic PEC glucose sensor exhibited good performances, such as a wider concentration range (500µM-10mM), high sensitivity (1.878µMmM-1cm-2 (500µM-2mM) and 127.2µMmM-1cm-2 (2mM-10mM)), good selectivity, reproducibility (RSD=2.4%) and applicability to real sample (human serum).

Strongly Coupled Ternary Hybrid Aerogels of N-deficient Porous Graphitic-C3N4 Nanosheets/N-Doped Graphene/NiFe-Layered Double Hydroxide for Solar-Driven Photoelectrochemical Water Oxidation.

Developing photoanodes with efficient sunlight harvesting, excellent charge separation and transfer, and fast surface reaction kinetics remains a key challenge in photoelectrochemical water splitting devices. Here we report a new strongly coupled ternary hybrid aerogel that is designed and constructed by in situ assembly of N-deficient porous carbon nitride nanosheets and NiFe-layered double hydroxide into a 3D N-doped graphene framework architecture using a facile hydrothermal method. Such a 3D hierarchical structure combines several advantageous features, including effective light-trapping, multidimensional electron transport pathways, short charge transport time and distance, strong coupling effect, and improved surface reaction kinetics. Benefiting from the desirable nanostructure, the ternary hybrid aerogels exhibited remarkable photoelectrochemical performance for water oxidation. Results included a record-high photocurrent density that reached 162.3 µA cm(-2) at 1.4 V versus the reversible hydrogen electrode with a maximum incident photon-to-current efficiency of 2.5% at 350 nm under AM 1.5G irradiation, and remarkable photostability. The work represents a significant step toward the development of novel 3D aerogel-based photoanodes for solar water splitting.