Jiatao Zhang

Formation of crystalline carbon nitride powder by a mild solvothermal method

Crystalline carbon nitride powder has been successfully prepared via the liquid–solid reaction between anhydrous C3N3Cl3 and Li3N in benzene at 355 °C and 5–6 MPa for 12 h. X-Ray diffraction (XRD) indicated that the major part of our brown sample was composed mainly of α-C3N4 and β-C3N4 with lattice parameters of a = 6.49 A, c = 4.70 A for α-C3N4 and a = 6.43 A, c = 2.43 A for β-C3N4. X-Ray photoelectron spectra (XPS), Fourier transform infrared spectroscopy (FTIR), electron energy-loss spectroscopy (EELS) and energy loss near edge structure (ELNES) strongly supported the existence of C–N covalent bonds. The relative N/C ratio is about 0.66. The temperature had an effect on the crystallization of carbon nitride powder. We have shown that the solvothermal technique might hold some promise for synthesizing pure crystalline α-C3N4 and β-C3N4.

Structurally Well-Defined Au@Cu2−xS Core–Shell Nanocrystals for Improved Cancer Treatment Based on Enhanced Photothermal Efficiency

Au@Cu2- x S core-shell nanocrystals (NCs) have been synthesized under large lattice mismatch with high crystallinity, controllable shape, and nonstoichiometric composition. Both experimental observations and simulations are used to verify the flexible dual-mode plasmon coupling. The enhanced photothermal effect is harnessed for diverse HeLa cancer cell ablation applications in the NIR-I window (750-900 nm) and the NIR-II window (1000-1400 nm).

Rigid three-dimensional Ni3S4 nanosheet frames: controlled synthesis and their enhanced electrochemical performance

Rigid three-dimensional (3D) Ni3S4 nanosheet frames assembled from ultrathin nanosheets are synthesized via a facile solvothermal method. Compared to flat Ni3S4 sheets, 3D Ni3S4 nanosheet frames have both a high free volume and high compressive strength. They can deliver a very high specific capacitance of 1213 F g−1 with good rate performance. In addition, these 3D Ni3S4 nanosheet frames are stabilized by plastically deformed ridges. The stabilized nanosheet frames did not unfold or collapse during electrochemical tests, and thus showed enhanced cycling ability.

Bamboo‐Like Nitrogen‐Doped Carbon Nanotubes with Co Nanoparticles Encapsulated at the Tips: Uniform and Large‐Scale Synthesis and High‐Performance Electrocatalysts for Oxygen Reduction

In recent years, various non-precious metal electrocatalysts for the oxygen reduction reaction (ORR) have been extensively investigated. The development of an efficient and simple method to synthesize non-precious metal catalysts with ORR activity superior to that of Pt is extremely significant for large-scale applications of fuel cells. Here, we develop a facile, low-cost, and large-scale synthesis method for uniform nitrogen-doped (N-doped) bamboo-like CNTs (NBCNT) with Co nanoparticles encapsulated at the tips by annealing a mixture of cobalt acetate and melamine. The uniform NBCNT shows better ORR catalytic activity and higher stability in alkaline solutions as compared with commercial Pt/C and comparable catalytic activity to Pt/C in acidic media. NBCNTs exhibit outstanding ORR catalytic activity due to high defect density, uniform bamboo-like structure, and the synergistic effect between the Co nanoparticles and protective graphitic layers. This facile method to synthesize catalysts, which is amenable to the large-scale commercialization of fuel cells, will open a new avenue for the development of low-cost and high-performance ORR catalysts to replace Pt-based catalysts for applications in energy conversion.

Plasmon enhanced photoelectrochemical sensing of mercury (II) ions in human serum based on Au@Ag nanorods modified TiO₂ nanosheets film.

Taking advantages of the monodisperse TiO2 nanosheets (NSs) with high active crystal face exposure and the tunable localized surface plasmon resonance (LSPR) properties of Au@Ag nanorods (NRs), this study demonstrated that TiO2 NSs film with trace amount of Au@Ag NRs modification possess a strong enhancement of photocurrent response, which was remarkably inhibited with the addition of mercury (II) ions (Hg(2+)). Based on the selective decrease of photocurrent with the addition of Hg(2+), a simple photoelectrochemical (PEC) sensor has been assembled. The PEC sensor exhibits wide linear range (0.01-10nM), low detection limit (2.5 pM), satisfying selectivity, reproducibility and acceptable stability for Hg(2+) detection. The feasibility of this method for practical application in human serum has been evaluated and the result was satisfactory. This PEC sensing method would provide a potential application for Hg(2+) detection in clinical diagnosis.

Nature-Inspired Na2Ti3O7 Nanosheets-Formed Three-Dimensional Microflowers Architecture as a High-Performance Anode Material for Rechargeable Sodium-Ion Batteries

Low cycling stability and poor rate performance are two of the distinctive drawbacks of most electrode materials for sodium-ion batteries (SIBs). Here, inspired by natural flower structures, we take advantage of the three-dimensional (3D) hierarchical flower-like stable microstructures formed by two-dimensional (2D) nanosheets to solve these problems. By precise control of the hydrothermal synthesis conditions, a novel three-dimensional (3D) flower-like architecture consisting of 2D Na2Ti3O7 nanosheets (Na-TNSs) has been successfully synthesized. The arbitrarily arranged but closely interlinked thin nanosheets in carnation-shaped 3D Na2Ti3O7 microflowers (Na-TMFs) originate a good network of electrically conductive paths in an electrode. Thus, Na-TMFs can get electrons from all directions and be fully utilized for sodium-ion insertion and extraction reactions, which can improve sodium storage properties with enhanced rate capability and super cycling performance. Furthermore, the large specific surface area provides a high capacity, which can be ascribed to the pseudo-capacitance effect. The wettability of the electrolyte was also improved by the porous and crumpled structure. The remarkably improved cycling performance and rate capability of Na-TMFs make a captivating case for its development as an advanced anode material for SIBs.

Noble metal nanoclusters and their in situ calcination to nanocrystals: Precise control of their size and interface with TiO2 nanosheets and their versatile catalysis applications

In this work, we present a new versatile strategy to prepare noble metal (Au, Ag and Cu) nanoclusters on TiO2 nanosheets in large scales with exposed (001) facets with controlled size, crystalline interface, and loading amount. By precise in situ calcination, the metal (M = Au, Ag, and Cu) nanocrystals with controllable size and better crystalline interface with the TiO2 support have been prepared. The potential application of the as-prepared Au, Ag, and Cu nanoclusters on TiO2 nanosheets as potential heterogeneous catalysts for organic synthesis, such as catalytic reduction of 4-nitrophenol to 4-aminophenol, has been demonstrated. After calcination, Au, Ag, and Cu nanocrystals were found to be proficient cocatalysts for photocatalytic H2 evolution, particularly the Au cocatalyst. Based on precise high-resolution transmission electron microscopy (HRTEM) and inductively coupled plasma optical emission spectrometry (ICP-OES) analyses, the flexible control of their size and loading amount as well as their intimate contact with the TiO2 nanosheet enhanced the photocatalytic H2 evolution activity and the sensitivity of the photocurrent response of the film. Furthermore, this aqueous-directed synthesis of metal nanoclusters on a support will generate further interest in the field of nanocatalysis.

Phosphine-Initiated Cation Exchange for Precisely Tailoring Composition and Properties of Semiconductor Nanostructures: Old Concept, New Applications†

Phosphine-initiated cation exchange is a well-known inorganic chemistry reaction. In this work, different phosphines have been used to modulate the thermodynamic and kinetic parameters of the cation exchange reaction to synthesize complex semiconductor nanostructures. Besides preserving the original shape and size, phosphine-initiated cation exchange reactions show potential to precisely tune the crystallinity and composition of metal/semiconductor core-shell and doped nanocrystals. Furthermore, systematic studies on different phosphines and on the elementary reaction mechanisms have been performed.

Core@shell sub-ten-nanometer noble metal nanoparticles with a controllable thin Pt shell and their catalytic activity towards oxygen reduction

AbstractReducing Pt loading, while improving electrocatalytic activity and the stability of Pt-based nanostructured materials, is currently a key challenge in green energy technology. Herein, we report the controllable synthesis of tri-metallic (Au@Ag@Pt) and bimetallic (Ag@Pt) particles consisting of a controllable thin Pt shell, via interface-mediated galvanic displacement. Through oil-ethanol-H2O interface mediation, the controllable “out to in” displacement of Ag atoms to Pt enables the formation of a thin Pt shell on monodisperse sub-ten-nanometer Au@Ag and Ag nanocrystals. The synthesized nanoparticles with a thin Pt shell exhibited potential catalytic activity towards the oxygen reduction reaction (ORR) due to the high exposure of Pt atoms.

Bimetallic ruthenium-copper nanoparticles embedded in mesoporous carbon as an effective hydrogenation catalyst.

Bimetallic ruthenium-copper nanoparticles embedded in the pore walls of mesoporous carbon were prepared via a template route and evaluated in terms of catalytic properties in D-glucose hydrogenation. The existence of bimetallic entities was supported by Ru L3-edge and Cu K-edge X-ray absorption results. The hydrogen spillover effect of the bimetallic catalyst on the hydrogenation reaction was evidenced by the results of both hydrogen and carbon monoxide chemisorptions. The bimetallic catalyst displayed a higher catalytic activity than the single-metal catalysts prepared using the same approach, namely ruthenium or copper nanoparticles embedded in the pore walls of mesoporous carbon. This improvement was due to the changes in the geometric and electronic structures of the bimetallic catalyst because of the presence of the second metal.