Jingping Hu

Shape‐Dependent Acidity and Photocatalytic Activity of Nb2O5 Nanocrystals with an Active TT (001) Surface

Nb(2)O(5) nanorods and nanospheres were synthesized, and their photocatalytic activity for methylene blue decomposition in water compared. Nb(2)O(5) nanorods clearly displayed higher activity, despite their comparable surface area. With a shape-dependent surface acidity, hydrothermal stability, and high photoactivity, these Nb(2)O(5) nanorods are a unique and exciting nanomaterial for non-classical photocatalytic mineralization of organic compounds in water.

Heterogeneous electron transfer kinetics at the ionic liquid/metal interface studied using cyclic voltammetry and scanning electrochemical microscopy.

The electrochemical behavior of a redox-active, ferrocene-modified ionic liquid (1-ferrocenylmethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide) in acetonitrile and in an ionic liquid electrolyte (1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide) is reported. Reversible electrochemical behavior was observed in each electrolyte with responses typical of those for unmodified ferrocene observed in each medium. In the ionic liquid electrolyte, the diffusion coefficient of the redox-active ionic liquid increased by a factor of 5 upon increasing the temperature from 27 to 90 degrees C. The kinetics of electron transfer across the ionic liquid/electrode interface were studied using cyclic voltammetry, and the standard heterogeneous electron transfer rate constant, k (0) was determined to be 4.25 x 10 (-3) cm s (-1). Scanning electrochemical microscopy was then also used to probe the heterogeneous kinetics at the interface between the ionic liquid and the solid electrode and conventional kinetic SECM theory was used to determine k (0). The k (0) value obtained using SECM was higher than that determined using cyclic voltammetry. These results indicate that SECM is a very useful technique for studying electron transfer dynamics in ionic liquids.

Radiotracer measurements as a sensitive tool for the detection of metal penetration in molecular-based organic electronics

The metallization of organic thin films is a crucial point in the development of molecular electronics. However, there is no method established yet to detect trace amounts of metal atoms in those thin films. Radiotracer measurements can quantify even very small amounts of material penetrating into the bulk, in our case less than 0.01% of a monolayer. Here, the application of this technique on two different well-characterized organic thin film systems (diindenoperylene and pentacene) is demonstrated. The results show that Ag is mainly adsorbed on the surface, but indicate that already at moderate deposition temperatures Ag can penetrate into the organic thin films and agglomerate at the film/substrate interface.

Focused Ion Beam Fabrication of Boron-Doped Diamond Ultramicroelectrodes

The fabrication of ultramicroelectrodes (UMEs) for analytical electrochemical applications has been explored, using boron-doped diamond as the active electrode material in an insulating coating formed by deposition of electrophoretic paint. Because of the rough nature of the diamond film, the property of such coatings that is normally exploited in the fabrication of UMEs, namely the tendency to retract automatically from sharp protrusions, cannot be used in the present instance. Instead focused ion beam (FIB) sputtering was employed to controllably produce UMEs with well-defined geometry, critical dimension of a few micrometers, and very thin insulating coatings. If the FIB machining is carried out at normal incidence to the diamond electrode surface, significant ion beam damage reduces the yield of successful electrodes. However, if a parallel machining geometry is employed, high yields of ultramicroelectrodes with a flat disk geometry can be obtained very reliably. The electrochemical properties of diamond UMEs are characterized. They show much lower background currents than the equivalent Pt or carbon fiber electrodes but more varied electrochemical response than macroscopic diamond electrodes.

A novel hollow sphere bismuth oxide doped mesoporous carbon nanocomposite material derived from sustainable biomass for picomolar electrochemical detection of lead and cadmium

A novel ultrasensitive, selective and low cost electrochemical sensor based on a hollow sphere bismuth oxide doped mesoporous carbon aerogel nanocomposite derived from a sustainable biomass material was successfully fabricated for simultaneous Pb2+ and Cd2+ detection at picomolar levels. In this nanocomposite material, we successfully brought together the advantages of an extraordinarily large surface area biomass derived carbon matrix with mesopores for analyte pre-enrichment and the excellent electroanalytical activity of the bismuth oxide hollow sphere structure for highly sensitive heavy metal sensing. Under optimized conditions, this electrode material exhibited a very low detection limit of 1.72 pM for Pb2+ and 1.58 pM for Cd2+ under ambient conditions, the lowest ever limit of detection recorded for the detection of both Pb2+ and Cd2+ using activated carbon. Furthermore, two wide linear ranges from 0.5 pM to 10 pM and from 10 pM to100 pM were observed due to the differences of adsorption dynamics at different metal ion concentration ranges. The nanocomposite sensor material demonstrated excellent reproducibility and great resistance to interference. Furthermore, the application for real water analysis was demonstrated and the result was highly consistent with the measurement from inductively coupled plasma optical emission spectroscopy (ICP-OES).

Co-disposal of MSWI fly ash and Bayer red mud using an one-part geopolymeric system

In this research, Bayer red mud (RM) was pretreated through alkali-thermal activation process, and prepared as an one-part geopolymer precursor, which could be used as geopolymeric solidification/stabilization (S/S) reagent for municipal solid waste incineration fly ash (MSWI FA). Compressive strength test, modified TCLP leaching test and sequential extraction test were conducted to evaluate the effectiveness of the RM-based geopolymeric S/S reagent. The results show that the S/S effects for heavy metals of RM-based geopolymer exhibit the following order: Pb>Cu>Zn>Cr. Most of the Zn, Pb and Cu in the MSWI FA transform from the leachable fractions into the inactive fractions difficult or unavailable to leach out. In the geopolymeric S/S solid, the active aluminosilicates in MSWI FA are dissolved in the alkaline environment formed by pretreated RM and then participate in the geopolymerization, which increases the SiO2/Al2O3 ratio and enhances the structural stability of geopolymeric S/S solid. MSWI FA offsets the strength deterioration of RM based one-part geopolymer and improves the immobilization efficiency for heavy metals in the geopolymer structure.

Pretreatment of eucalyptus with recycled ionic liquids for low-cost biorefinery

It is urgent to develop recycled ionic liquids (ILs) as green solvents for sustainable biomass pretreatment. The goal of this study is to explore the availability and performance of reusing 1-allyl-3-methylimidazolium chloride ([amim]Cl) and 1-butyl-3-methylimidazolium acetate ([bmim]OAc) for pretreatment, structural evolution, and enzymatic hydrolysis of eucalyptus. Cellulose enzymatic digestibility slightly decreased with the increased number of pretreatment recycles. The hydrolysis efficiencies of eucalyptus pretreated via 4th recycled ILs were 54.3% for [amim]Cl and 72.8% for [bmim]OAc, which were 5.0 and 6.7-folds higher than that of untreated eucalyptus. Deteriorations of ILs were observed by the relatively lower sugar conversion and lignin removal from eucalyptus after 4th reuse. No appreciable changes in fundamental framework and thermal stability of [amim]Cl were observed even after successive pretreatments, whereas the anionic structure of [bmim]OAc was destroyed or replaced. This study suggested that the biomass pretreatment with recycled ILs was a potential alternative for low-cost biorefinery.

Plasma Electrochemistry: Development of a Reference Electrode Material for High Temperature Plasma

This report describes the development of a high temperature reference electrode material for gas phase electrochemistry investigations. The electrode is constructed by careful assessment of different metal/metal oxide materials and operational stability in flame electrolyte medium. This will enable reliable dynamic electrochemistry investigations into redox reactions at the solid/gas interface, free of any solvent defined potential window restrictions.

Cross-linked chitosan/β-cyclodextrin composite for selective removal of methyl orange: Adsorption performance and mechanism

A complex chitosan/β-cyclodextrin polymer was synthesized by bridging with maleoyl chains followed by cross-linking with glutaraldehyde. The adsorption performance of the synthetic polymer was investigated for selective removal of methyl orange (MO) from aqueous solution. The kinetic behavior was well fitted by the pseudo-second order model, while the adsorption process at equilibrium followed the Langmuir isotherm model. The thermodynamic parameters suggested that the adsorption was exothermic and spontaneous. Under optimal adsorption conditions, the capacity for MO reached 392mg/g with the dosage of 10mg/50mL. Based on the analysis from FTIR, 1H NMR, TGA and zeta potential, the adsorption mechanism could be explained by the synergistic effect of electrostatic attraction of amino groups from chitosan and host-guest interaction from β-cyclodextrin. This adsorbent also demonstrated high selectivity towards MO due to the unique structure of cross-linked chitosan/β-cyclodextrin polymer that are complementary to that of MO molecule.

Enhanced Cr(VI) removal from acidic solutions using biochar modified by Fe 3 O 4 @SiO 2 -NH 2 particles

Fe3O4@SiO2-NH2 magnetic particles with core-shell structure were attached on carboxylated biochar derived from phoenix tree leaves to synthesize a novel magnetic biochar for removing Cr(VI) ions from acidic solutions. FSEM, FTEM, XRD characterizations of the synthesized magnetic biochar revealed that the Fe3O4@SiO2-NH2 magnetic particles distributed uniformly on the surface or macrospores of carboxylated biochar by strong chemical bonding. The Cr(VI) ions adsorption capacity of magnetic biochar was 27.2mg·g-1, surpassing original carboxylated biochar (18.2mg·g-1). VSM and XPS characterizations demonstrated that the attached Fe3O4@SiO2-NH2 magnetic particles not only endowed biochar with perfect magnetic property (23emu·g-1) but also provided complexing sites for binding Cr(III) cations reduced from Cr(VI) anions. The Cr(VI) ions removal by magnetic biochar contained three steps: (1) adsorption of Cr(VI) anions by protonated functional groups; (2) reduction of Cr(VI) anions to Cr(III) cations by electron-donor groups; and (3) chelation of Cr(III) cations by amine groups. The adsorption recycling test showed that magnetic biochar kept 85% of its initial Cr(VI) adsorption capacity at the sixth cycle, and the Fe leakage under pH1.0 was smaller than 0.25mg·L-1. The results indicated that this novel magnetic biochar was applicable for the practical treatment of Cr(VI)-containing wastewater.