Jingjing Zhan

Multifunctional Iron−Carbon Nanocomposites through an Aerosol-Based Process for the In Situ Remediation of Chlorinated Hydrocarbons

Spherical iron-carbon nanocomposites were developed through a facile aerosol-based process with sucrose and iron chloride as starting materials. These composites exhibit multiple functionalities relevant to the in situ remediation of chlorinated hydrocarbons such as trichloroethylene (TCE). The distribution and immobilization of iron nanoparticles on the surface of carbon spheres prevents zerovalent nanoiron aggregation with maintenance of reactivity. The aerosol-based carbon microspheres allow adsorption of TCE, thus removing dissolved TCE rapidly and facilitating reaction by increasing the local concentration of TCE in the vicinity of iron nanoparticles. The strongly adsorptive property of the composites may also prevent release of any toxic chlorinated intermediate products. The composite particles are in the optimal range for transport through groundwater saturated sediments. Furthermore, those iron-carbon composites can be designed at low cost, the process is amenable to scale-up for in situ application, and the materials are intrinsically benign to the environment.

Multifunctional Colloidal Particles for in Situ Remediation of Chlorinated Hydrocarbons

Effective in situ injection technology for the remediation of dense nonaqueous phase liquids (DNAPLs) such as trichloroethylene (TCE) requires the use of decontamination agents that effectively migrate through the soil media and react efficiently with dissolved TCE and bulk TCE. We describe the use of a novel decontamination system containing highly uniform carbon microspheres in the optimal size range for transport through the soil. The microspheres are enveloped in a polyelectrolyte (carboxymethyl cellulose, CMC) to which a bimetallic nanoparticle system of zero-valent iron and Pd is attached. The carbon serves as a strong adsorbent to TCE, while the bimetallic nanoparticle system provides the reactive component. The polyelectrolyte serves to stabilize the carbon microspheres in aqueous solution. The overall system resembles a colloidal micelle with a hydrophilic shell (polyelectrolyte coating) and hard hydrophobic core (carbon). In contact with bulk TCE, there is a sharp partitioning of the system to the TCE side of the interface due to the hydrophobicity of the core. These multifunctional systems appear to satisfy criteria related to remediation and are made with potentially environmentally benign materials.

The Synthesis of Mesoporous TiO2/SiO2/Fe2O3 Hybrid Particles Containing Micelle- Induced Macropores through an Aerosol Based Process

Mesoporous SiO(2)/TiO(2)/Fe(2)O(3) particles containing macropores of about 50 nm in diameter have been prepared by an aerosol process using cetyltrimethylammonium bromide (CTAB) as a templating agent. In contrast to the traditional templating effect of CTAB to form ordered mesoporous silicas, the morphology here is vastly different due to the presence of precursor iron salts. The particles have mesoporosity templated by CTAB but additionally have large voids leading to a combined macroporous and mesoporous structure. The morphology is explained through the formation of colloidal structures containing species such as CTA(+)X(-1)Fe(3+) colloids in the aerosol droplets, indicating of a salt bridging effect. This dual porosity has applied implications, as the macropores provide easy entry to the particle interior in potentially diffusion limited situations. Furthermore, the particles encapsulate Fe(2)O(3) and contain TiO(2) leading to the dual functional properties of magnetic response and photocatalytic activity.

Modifying metal nanoparticle placement on carbon supports using an aerosol-based process, with application to the environmental remediation of chlorinated hydrocarbons.

A facile aerosol-based process (ABP) is developed to vary the placement of iron nanoparticles on the external surface of carbon microspheres or within the interior. This is accomplished through the competitive mechanisms of sucrose carbonization and the precipitation of soluble iron salts, in an aerosol droplet passing through a high temperature heating zone. At lower aerosolization temperatures, carbonization occurs first leading to iron salt precipitation on the external surface, while at higher temperatures interior placement occurs through concurrent iron salt precipitation and sucrose carbonization. The resulting composites are highly conducive to the reductive dechlorination of compounds such as trichloroethylene (TCE) as the carbon support is a strong adsorbent, and zerovalent iron effectively reduces TCE to innocuous gases such as ethane. Since both iron and carbon are widely used catalysts and catalyst supports, the simple process of modifying iron placement has significant potential applications in heterogeneous catalysis.

Shear Induced Formation of Patterned Porous Titania with Applications to Photocatalysis

Patterned macroporous titania (TiO2) materials have been synthesized via a shear-aligned rigid crystalline surfactant mesophase. The macropores inherit the hexagonal geometry of the water channels of the template. Scanning electron microscopy (SEM) and cut-section transmission electron microscopy (TEM) images show that the macropores templated by the sheared mesophase attain considerably greater alignment than pores templated by the nonsheared mesophase. The mean pore diameter, the crystalline size of TiO2 particles, and the photoactivity of the materials increase with the increase of water content in the template. The sheared TiO2 samples exhibit higher photocatalytic activity for the degradation of Rhodamine B than the corresponding materials synthesized in the nonsheared template. The improvement in photocatalytic activity of the sheared TiO2 materials is attributed to its higher photoabsorption efficiency and the patterned channels which facilitate the diffusion and transport of reactant molecules within the frameworks. Such patterned porous materials may have promise as advanced catalytic supports and photocatalytic materials.

Aerosol-Assisted Self-Assembly of Reticulated N-Doped Carbonaceous Submicron Spheres for Effective Removal of Hexavalent Chromium.

This Research Article described a facile one-step method to prepare reticulated N-doped carbonaceous submicron spheres. Through a simple aerosol-assisted technology, glucosamine sulfate used as a carbon source was aerosolized and carbonized to functionalized carbonaceous submicron spheres. The electrostatic attraction between protonated amino groups and sulfate in the aerosol droplets induced a self-assembly and led to the formation of reticular structure, avoiding the use of templates. Compared to bare carbonaceous materials produced from glucose, reticulated N-doped carbonaceous spheres exhibit higher efficiency in the removal of Cr(VI), where the doping of element nitrogen led to electrostatic attraction between protonated nitrogen and chromium ions, and reticulated structure created relatively higher surface area and pore volume, facilitating materials to contact with Cr(VI) ions. XPS characterization proved these novel N-doped carbonaceous materials could effectively transform Cr(VI) to less toxic Cr(III) because of the surface reducing groups. For the practical application, several factors including the initial pH, materials dosage and recycle numbers on the removal performance were studied.

Synthesis of Submicrometer Hollow Particles with a Nanoscale Double-Layer Shell Structure

The morphology of hollow, double-shelled submicrometer particles is generated through a rapid aerosol-based process. The inner shell is an essentially hydrophobic carbon layer of nanoscale dimension (20 nm), and the outer shell is a hydrophilic silica layer of approximately 40 nm, with the shell thickness being a function of the particle size. The particles are synthesized by exploiting concepts of salt bridging to lock in a surfactant (CTAB) and carbon precursors together with iron species in the interior of a droplet. This deliberate negation of surfactant templating allows a silica shell to form extremely rapidly, sealing in the organic species in the particle interior. Subsequent pyrolysis results in a buildup of internal pressure, forcing carbonaceous species against the silica wall to form an inner shell of carbon. The incorporation of magnetic iron oxide into the shells opens up applications in external stimuli-responsive nanomaterials.

Water Decontamination Using Iron and Iron Oxide Nanoparticles

Publisher Summary The enhancement of environmental quality and sustainability through pollution prevention, treatment, and remediation can be provided by the usage of nanoscale materials. These benefits are derived from the enhanced reactivity, surface area, and subsurface transport characteristics of nanomaterials. Among this material family, nanoparticles have great promise for uses in many areas including catalyst, optical, biological, microelectronic, and environmental applications. Nanoparticles can be designed and synthesized to act as separation and reaction media for pollutants, proving revolutionary opportunities to develop more efficient and cost-effective water purification processes and systems relative to current conventional approaches. Water pollutants, such as waterborne bacteria, toxic metals, and chlorinated hydrocarbons, are introduced into the environment from natural sources and are produced from municipal, industrial, and agricultural processes.

Iron-carbon composite microspheres prepared through a facile aerosol-based process for the simultaneous adsorption and reduction of chlorinated hydrocarbons

Iron-carbon (Fe-C) composite microspheres prepared through a facile aerosol-based process are effective remediation agents for the simultaneous adsorption and reduction of chlorinated hydrocarbons. Complete dechlorination was achieved for the class of chlorinated ethenes that include tetrachloroethylene (PCE), trichloroethylene (TCE), cis- and trans-1,2-dicloroethylene (c-DCE, t-DCE), 1,1-dichloroethylene (1,1-DCE) and, vinyl chloride (VC). The Fe-C particles potentially provides multi-functionality with requisite characteristics of adsorption, reaction, and transport for the effective in situ remediation of chlorinated hydrocarbons. The carbon support immobilizes the ferromagnetic iron nanoparticles onto its surface, thereby inhibiting aggregation. The adsorptive nature of the carbon support prevents the release of toxic intermediates such as the dichloroethylenes and vinyl chloride. The adsorption of chlorinated ethenes on the Fe-C composites is higher (>80%) than that of humic acid (<35%) and comparable to adsorption on commercial activated carbons (>90%). The aerosol-based process is an efficient method to prepare adsorptivereactive composite particles in the optimal size range for transport through the porous media and as effective targeted delivery agents for the in situ remediation of soil and groundwater contaminants.

Aerosol-assisted in situ synthesis of iron–carbon composites for the synergistic adsorption and reduction of Cr(VI)

In this work, we adopted newly developed spherical iron–carbon composites to remove hexavalent chromium (Cr(VI)) from contaminated water. These composites were prepared in situ through a facile aerosol-assisted process followed by an economic carbothermal reduction using only common sugar and ferrous sulfate as starting materials, and then characterized by SEM, TEM, XRD and BET. Because of the diverse functions of carbon and nanoscale zero-valent iron, aerosol-assisted iron–carbon composites show synergistic adsorption and reaction towards a more efficient removal of Cr(VI). Under identical experimental conditions, such composites exhibit the highest removal efficiency compared to other materials including nanoscale zero-valent iron particles, aerosol-assisted carbon and their physical mixture. Meanwhile, X-ray photoelectron spectroscopy analysis proved as-prepared iron–carbon composites could effectively transform Cr(VI) to much less toxic trivalent chromium (Cr(III)). These iron–carbon composites produced at low cost show significant potential for the remediation of groundwater and sediment contaminated with heavy metals such as Cr(VI).