Huile Jin

Graphene Quantum Dots Supported by Graphene Nanoribbons with Ultrahigh Electrocatalytic Performance for Oxygen Reduction

A new class of oxygen reduction reaction (ORR) catalysts based on graphene quantum dots (GQDs) supported by graphene nanoribbons (GNRs) has been developed through a one-step simultaneous reduction reaction, leading to ultrahigh performance for O reduction with an excellent electrocatalytic activity (higher limiting current density and lower overpotential than those of platinum) and high selectivity and stability in alkaline media comparable to the best C-based ORR catalysts reported so far. Electron microscopy revealed numerous surface/edge defects on the GQD/GNR surfaces and at their interface to act as the active sites. This, coupled with efficient charge transfer between the intimately contacted GQDs and GNRs, rationalized the observed ultrahigh electrocatalytic performance for the resultant GQD-GNR hybrids. Thus, this study opens a new direction for developing low-cost, highly efficient, C-based ORR electrocatalysts.

A Versatile Strategy for Shish-Kebab-like Multi-heterostructured Chalcogenides and Enhanced Photocatalytic Hydrogen Evolution.

A series of multi-heterostructured metal chalcogenides (CdS-Te, NiS/CdS-Te, and MoS2/CdS-Te) with a surprising shish-kebab-like structure have been synthesized via a one-step microwave-assisted pyrolysis of dithiocarbamate precursors in ethylene glycol. Subsequently, CdS-Te composites were exploited as a self-sacrificial template to craft various CdS-Te@(Pt, Pd) multi-heterostructures. Highly uniform dispersion and intimate interactions between CdS and multicomponent cocatalysts, together with improved separation of photogenerated carriers due to the presence of Te nanotubes (NTs) and trace CdTe, enable CdS-based heterostructured photocatalysts to exhibit greatly enhanced efficiency and stability in the photocatalytic production of H2. Thorough morphological characterizations revealed that the growth of metal sulfide/Te heterostructures originates from the growth of Te tubes, which is likely governed by diffusion-limited depletion of the Te precursor and the dissolution-crystallization process of Te seeds followed by the formation of metal sulfide kebabs.

Electrochemical detection of hepatitis B and papilloma virus DNAs using SWCNT array coated with gold nanoparticles

This study investigated electrochemical detection of human hepatitis B and papilloma viruses using electrochemical impedance spectroscopy technique. The sensor was fabricated by electrochemically depositing Au nanoparticles on the in situ prepared single walled carbon nanotube (SWCNTs) arrays, followed by the self-assembly of single-stranded probe DNA on the SWCNTs/Au platform. The as-prepared electrochemical sensor could detect lower than 1 attomole complimentary hepatitis B single-stranded DNA (ssDNA), which corresponds to having 600 ssDNA molecules in a 1.0 mL sample. For a 1-base mismatched hepatitis B ssDNA, the experimental detection limit is 0.1 pmol. When being applied to detect 24-base papilloma virus ssDNA, the experimentally determined low detection limit is 1 attomole. In addition to the low detection limit, the SWCNTs/Au/ssDNA sensor also showed great stability, where after being kept in a refrigerator for a month at a temperature 4-8 °C its charge transfer resistance decreased by less than 1%. The sensor could be conveniently regenerated via dehybridization in hot water. Both aligned and random SWCNTs arrays have been investigated in this study and there was nearly no difference in the low limit in the detection of hepatitis B and papilloma viruses. This study illustrates that combining Au nanoparticles with the in situ fabricated SWCNTs array is a promising platform for ultrasensitive biosensing.

Synthesis of Au-Decorated Tripod-Shaped Te Hybrids for Applications in the Ultrasensitive Detection of Arsenic

Novel Au-decorated Te hybrids with a tripod-shaped planar microstructure were prepared through a two-step hydrothermal process: the synthesis of Te single crystals and the subsequent self-sacrificial reaction of Te template with HAuCl4. Based on the influences of reaction temperature and solvent compositions on the as-obtained microstructures, a plausible mechanism was proposed to account for the formation of the tripod-shaped Te and Au/Te crystals. The as-prepared Au/Te hybrids have the sensitivity of 6.35 μA/ppb in the electrochemical detection of As(III), which represents the highest sensitivity reported in literature. The Au/Te sensor also has a low detection limit of 0.0026 ppb and could work in complex mixtures containing As(III), Cu(II) and other heavy metal ions, exhibiting excellent selectivity on As(III) and Cu(II) ions. The enhanced electrocatalytic property may be attributed to the synergetic interactions between the noble metal and semiconductor and the presence of a large number of active sites on the hybrids surface.

A rapid green route for fabricating efficient SERS substrates

This study develops a simple, rapid electrochemical approach for preparing dendrite-shaped Ag nanomaterials, which are well known as effective SERS substrates. In addition to yielding silver that exhibits a strong enhancement in SERS measurements when tested with 2,2′-dithiodipyridine and ethylenethiourea, this new fabrication method does not require any template, surfactants or supporting electrolyte, making it environment friendly. Analysis illustrates that the as-prepared Ag products are essentially pure silver consisting of abundant {111}-oriented crystallites. These Ag dendrites formed on a commercially available tin-doped indium oxide electrode could also be easily transferred onto other desired surfaces, making their application in SERS measurements more versatile.

Thermal and FTIR spectral studies of N,N′-diphenylguanidine

Thermal decomposition of N,N′-diphenylguanidine (DPG) was investigated by simultaneous TG/DSC-FTIR techniques under nonisothermal conditions. Online FTIR measurements illustrate that aniline is a major product of DPG decomposition. The observation that the activation energy depends on the extent of conversion indicates that the DPG decomposition kinetics features multiple processes. The initial elimination of aniline from DPG involves two pathways because of the isomerization of DPG. Mass spectrometry and thin film chromatography suggest that there are two major intermediate products with the major one of C21N3H17. The most probable kinetic model deduced through multivariate nonlinear regression method agrees well with the experimental data with a correlation coefficient of 0.9998. The temperature-independent function of conversion f(α), activation energy E and the pre-exponential factor A of DPG decomposition was also established through model-fitting method in this research.

Strong Graphene 3D Assemblies with High Elastic Recovery and Hardness

The rational design and construction of 3D graphene assemblies is a crucial step to extend the graphene properties for practical applications. Here, a novel interfacially reactive self-assembling process is reported to prepare well-organized 3D honeycomb-like graphene assemblies with unique polygonal nanopores interconnected by silicon-oxygen chemical bonds. The newly developed silicate-bridged graphene assembly (SGA) exhibits an exceptionally high hardness of 13.09 GPa, outperforming all existing 3D graphene materials, while maintains high Youngs modulus (162.96 GPa), elastic recovery (75.27%), and superb thermal stability (600 °C in air). The observed unusual merits are resulted from unique pore structure combining the mechanical stability of the trihedral-nanopore structure and the deformability of the other polygonal nanopores. As a filling material, a merely 0.05% (w/w) addition of SGA could double the impact resistance of unsaturated resins (e.g., polyester). While SGA is attractive for various applications, including body armors, wearable electronics, space elevators, and multifunctional reinforcement fibers for automobiles, and aerospace vehicles, the novel liquid sodium-water interfacial reactive self-assembling developed in this study could open avenues for further development of various well-defined 3D assemblies from graphene and many other materials.

Fabrication of noble-metal catalysts with a desired surface wettability and their applications in deciphering multiphase reactions.

Noble-metal Pd and Pt catalysts with a wide range of surface wettability were fabricated through an electrochemical approach and were characterized with scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy, and atomic force microscopy. The importance of surface wettability of solid catalysts in multiphase reactions-especially their correlation to the nature of the studied chemical system-was investigated by reducing oxygen in an alkaline solution and oxidizing hydrogen peroxide and sodium formate in alkaline or buffered solutions at the as-prepared catalysts. These experiments illustrate that the nature of a multiphase reaction plays a critical role in determining the influence of surface wettability on the catalyst performance, providing a unique approach to decipher the reaction process. The investigation allows us to gain new insights into the electrochemical oxidation of sodium formate.