Jingming Gong

Efficient Removal of Heavy Metal Ions from Aqueous Systems with the Assembly of Anisotropic Layered Double Hydroxide Nanocrystals@Carbon Nanosphere

We report on the efficient removal of heavy metal ions from simulated wastewater with a nanostructured assembly. The nanoassembly was obtained via direct assembling the performed anisotropic layered double hydroxide nanocrystals (LDH-NCs) onto the surface of carbon nanospheres (labeled as LDH-NCs@CNs). It was found that the maximum adsorption capacity of the nanoassembly toward Cu(2+) was ∼ 19.93 mg g(-1) when the initial Cu(2+) concentration was 10.0 mg L(-1), displaying a high efficiency for the removal of heavy metal ions. The Freundlich adsorption isotherm was applicable to describe the removal processes. Kinetics of the Cu(2+) removal was found to follow pseudo-second-order rate equation. Furthermore, the as-prepared building unit of the assembly, including LDH-NCs, CNs, and the assembly, as well as Cu(2+)-adsorbed assembly, were carefully examined by transmission electron microscopy (TEM), Fourier transform infrared spectroscopy (FT-IR), nitrogen sorption measurements, and X-ray photoelectron spectroscopy (XPS). Based on the characterization results, a possible mechanism of Cu(2+) removal with the assembly of LDH-NCs@CNs was proposed. Comparison experiments show that the adsorption capacity of the resulting LDH-NCs@CNs assembly was much higher than its any building unit alone (CNs or LDH-NCs), exhibiting the deliberation of the assembly on water decontamination. This work provides a very efficient, fast and convenient approach for exploring promising nanoassembly materials for water treatment.

Stripping voltammetric detection of mercury(II) based on a bimetallic Au-Pt inorganic-organic hybrid nanocomposite modified glassy carbon electrode.

A new, highly sensitive and selective sensor for the electrochemical assay of Hg(II) by anodic stripping voltammetry has been developed, whereby a glassy carbon electrode is modified with a novel inorganic-organic hybrid nanocomposite, namely, bimetallic Au-Pt nanoparticles/organic nanofibers (labeled as Au-PtNPs/NFs). The sensor possesses a three-dimensional (3D) porous network nanoarchitecture, in which the bimetallic Au-Pt NPs serving as metal NP-based microelectrode ensembles are homogenously distributed in the matrix of interlaced organic NFs. The surface structure and composition of the sensor were characterized by scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). Its electrochemical performance was systematically investigated. Our results show that such a newly designed, Au-PtNPs/NF nanohybrid modified electrode provides remarkably improved sensitivity and selectivity for the stripping assay of Hg(II). The detection limit is found to be as low as 0.008 ppb (S/N = 3) that is much below the guideline value from the World Health Organization (WHO). Interferences from other heavy metal ions such as Cu(II), Cr(III), Co(II), Fe(II), Zn(II), and Mn(II) ions associated with mercury analysis are effectively inhibited. Toward the goal for practical applications, the sensor was further evaluated by monitoring Hg(II) in tap and river water specimens.

Electrochemical biosensing of methyl parathion pesticide based on acetylcholinesterase immobilized onto Au-polypyrrole interlaced network-like nanocomposite.

We developed a simple strategy for designing a highly sensitive electrochemical biosensor for organophosphate pesticides (OPs) based on acetylcholinesterase (AChE) immobilized onto Au nanoparticles-polypyrrole nanowires composite film modifid glassy carbon electrode (labeled as AChE-Au-PPy/GCE). Where, the generated Au nanoparticles (AuNPs) were homogenously distributed onto the interlaced PPy nanowires (PPy NWs) matrix, constructing a three-dimensional porous network. This network-like nanocomposite not only provided a biocompatible microenvironment to keep the bioactivity of AChE, but also exhibited a strong synergetic effect on improving the sensing properties of OPs. The combination of AuNPs and PPyNWs greatly catalyzed the oxidation of the enzymatically generated thiocholine product, thus increasing the detection sensitivity. On the basis of the inhibition of OPs on the enzymatic activity of AChE, the conditions for OPs detection were optimized by using methyl parathion as a model OP compound. The inhibition of methyl parathion was proportional to its concentration ranging from 0.005 to 0.12 and 0.5 to 4.5 microgmL(-1). The detection limit was 2 ngmL(-1). The developed biosensor exhibited good reproducibility and acceptable stability. This study provides a new promise tool for analysis of organophosphate pesticides.

An enzymeless organophosphate pesticide sensor using Au nanoparticle-decorated graphene hybrid nanosheet as solid-phase extraction

A sensitive enzymeless organophosphate pesticides (OPs) sensor is fabricated by using Au nanoparticles (AuNPs) decorated graphene nanosheets (GNs) modified glassy carbon electrode as solid phase extraction (SPE). Such a nanostructured composite film, combining the advantages of AuNPs with two dimensional GNs, dramatically facilitates the enrichment of nitroaromatic OPs onto the surface and realizes their stripping voltammetric detection of OPs by using methyl parathion (MP) as a model. The stripping voltammetric performances of captured MP were evaluated by cyclic voltammetric and square-wave voltammetric analysis. The combination of the nanoassembly of AuNPs-GNs, SPE, and stripping voltammetry provides a fast, simple, and sensitive electrochemical method for detecting nitroaromatic OPs. The stripping analysis is highly linear over the MP concentration ranges of 0.001-0.1 and 0.2-1.0 μg mL(-1) with a detection limit of 0.6 ng mL(-1). This designed enzymeless sensor exhibits good reproducibility and acceptable stability.

Highly sensitive visible light activated photoelectrochemical biosensing of organophosphate pesticide using biofunctional crossed bismuth oxyiodide flake arrays

A new, highly sensitive and selective biosensor for the photoelectrochemical (PEC) detection of organophosphate pesticides (OPs) has been developed, whereby newly synthesized crossed bismuth oxyiodide (BiOI) nanoflake arrays (BiOINFs) are fabricated as a photoactive electrode via a successive ionic layer adsorption and reaction (SILAR) approach. The smart integration of BiOINFs with biomolecules acetylcholinesterase (AChE) yields a novel AChE-BiOINFs hybrid, constructing a three-dimensional (3D) porous network biosensing platform. The composition and surface structure of the sensor were carefully characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), and various electrochemical techniques. Such interlaced network architectures, providing better mass transport and allowing more AChE loading per unit area, as well as the intrinsically strong visible light-harvesting effect from BiOI, greatly facilitate the PEC responses. On the basis of the effect of OPs on the photocurrent of AChE-BiOINFs/ITO, a highly sensitive visible light-activated photoelectrochemical biosensor was developed for biosensing OPs. The conditions for OPs detection were optimized by using methyl parathion (MP) as a model OP compound. Under the optimized experimental conditions, our results show that such a newly designed AChE-BiOINFs/ITO photoactive electrode provides remarkably improved sensitivity and selectivity for the biosensing of OPs. The detection limit was found to be as low as about 0.04 ng mL(-1) (S/N=3). Toward the goal for practical applications, the resulting sensor was further evaluated by monitoring MP in spiked vegetable samples, showing fine applicability for the detection of MP in real samples.

Signal-on electrochemiluminescence of biofunctional CdTe quantum dots for biosensing of organophosphate pesticides.

A new, highly sensitive and selective ECL assay biosensor based on target induced signal on has been developed for the detection of organophosphate pesticides (OPs), whereby the smart integration of graphene nanosheets (GNs), CdTe quantum dots (CdTe QDs), and acetylcholinesterase (AChE) enzymatic reaction yields a biofunctional AChE-GNs-QDs hybrid as cathodic ECL emitters for OPs sensing. The electrochemically synthesized GNs were selected as a supporting material to anchor CdTe QDs, exhibiting a significantly amplified ECL signal of QDs. On the basis of the effect of OPs on the ECL signal of AChE-QDs-GNs modified glassy carbon electrode (GCE), a highly sensitive GNs-anchored-QDs-based signal-on ECL biosensor was developed for sensing OPs, combined with the enzymatic reactions and the dissolved oxygen as coreactant. The conditions for OPs detection were optimized by using methyl parathion (MP) as a model OP compound. Under the optimized experimental conditions, such a newly designed system shows remarkably improved sensitivity and selectivity for the sensing of OPs. The detection limit was found to be as low as about 0.06 ng mL(-1) (S/N=3). Toward the goal for practical applications, the resulting sensor was further evaluated by monitoring MP in spiked vegetable samples, showing fine applicability for the detection of MP in real samples.

Biosensor based on acetylcholinesterase immobilized onto layered double hydroxides for flow injection/amperometric detection of organophosphate pesticides.

We developed a highly sensitive flow injection/amperometric biosensor for the detection of organophosphate pesticides (OPs) using layered double hydroxides (LDHs) as the immobilization matrix of acetylcholinesterase (AChE). LDHs provided a biocompatible microenvironment to keep the bioactivity of AChE, due to the intrinsic properties of LDHs (such as a regular structure, good mechanical, chemical and thermal stabilities, and swelling properties). By integrating the flow injection analysis (FIA) with amperometric detection, the resulting AChE-LDHs modified electrode greatly catalyzed the oxidation of the enzymatically generated thiocholine product, and facilitated the detection automation, thus increasing the detection sensitivity. The analytical conditions for the FIA/amperometric detection of OPs were optimized by using methyl parathion (MP) as a model. The inhibition of MP was proportional to its concentration ranging from 0.005 to 0.3μg mL(-1) and 0.3 to 4.0μg mL(-1) with a detection limit 0.6ng mL(-1) (S/N=3). The developed biosensor exhibited good reproducibility and acceptable stability.

Stripping voltammetric analysis of organophosphate pesticides using Ni/Al layered double hydroxides as solid-phase extraction

A sensitive electrochemical stripping voltammetric biosensor is designed for organophosphate pesticides (OPs) based on solid-phase extraction (SPE) using Ni/Al layered double hydroxides (LDHs) modified glassy carbon electrode (labeled as Ni/Al-LDHs/GCE). The Ni/Al-LDHs as the host are highly efficient to capture OPs, which dramatically facilitates the enrichment of nitroaromatic OPs onto their surface and realizes the stripping voltammetric detection of OPs. The stripping voltammetric performances of methyl parathion (MP) intercalated into LDHs were evaluated by cyclic voltammetric and square-wave voltammetric (SWV) analysis. The combination of the host-guest supramolecular structure, SPE, and stripping voltammetry provides a fast, simple, and sensitive electrochemical method for detecting nitroaromatic OPs by using MP as a model. The stripping analysis is linear over the MP concentration ranges of 0.001-0.1 and 0.2-1.0 microg mL(-1) with a detection limit of 0.6 ng mL(-1) (S/N=3). The developed biosensor exhibits good reproducibility and acceptable stability. This study offers a new promising protocol for OPs analysis.

Adsorption of heavy metal ions by hierarchically structured magnetite-carbonaceous spheres.

Magnetically driven separation technology has received considerable attention in recent decade for its great potential application. In this work, hierarchically structured magnetite-carbonaceous microspheres (Fe(3)O(4)-C MSs) have been synthesized for the adsorption of heavy metal ions from aqueous solution. Each sphere contains numerous unique rattle-type structured magnetic particles, realizing the integration of rattle-type building unit into microspheres. The as-prepared composites with high BET surface area, hierarchical as well as mesoporous structures, exhibit an excellent adsorption capacity for heavy metal ions and a convenient separation procedure with the help of an external magnet. It was found that the maximum adsorption capacity of the composite toward Pb(2+) was ∼126mgg(-1), displaying a high efficiency for the removal of heavy metal ions. The Freundlich adsorption isotherm was applicable to describe the removal processes. Kinetics of the Pb(2+) removal was found to follow pseudo-second-order rate equation. The as-prepared composite of Fe(3)O(4)-C MSs as well as Pb(2+)-adsorbed composite were carefully examined by scanning electron microscopy (SEM), Zeta potential measurements, Fourier transform infrared spectroscopy (FT-IR), nitrogen sorption measurements, and X-ray photoelectron spectroscopy (XPS). Based on the characterization results, a possible mechanism of Pb(2+) removal with the composite of Fe(3)O(4)-C MSs was proposed.

Bifunctional sensor of pentachlorophenol and copper ions based on nanostructured hybrid films of humic acid and exfoliated layered double hydroxide via a facile layer-by-layer assembly

A new, highly sensitive bifunctional electrochemical sensor for the simultaneous determination of pentachlorophenol (PCP) and copper ions (Cu(2+)) has been developed, where organic-inorganic hybrid ultrathin films were fabricated by alternate assembly of humic acid (HA) and exfoliated Mg-Al-layered double hydroxide (LDH) nanosheets onto ITO substrates via a layer-by-layer (LBL) approach. The multilayer films were then characterized by means of UV-vis spectrometry, scanning electron microscopy (SEM), and atomic force microscope (AFM). These films were found to have a relatively smooth surface with almost equal amounts of HA incorporated in each cycle. Its electrochemical performance was systematically investigated. Our results demonstrate that such a newly designed (LDH/HA)n multilayer films, combining the individual properties of HA (dual recognition ability for organic herbicides and metal ions) together with LDH nanosheets (a rigid inorganic matrix), can be applied to the simultaneous analysis of PCP and Cu(II) without interference from each other. The LBL assembled nanoarchitectures were further investigated by X-ray photoelectron spectroscopy (XPS) and infrared spectroscopy (IR), which provides insight for bifunctional sensing behavior. Under the optimized conditions, the detection limit was found to be as low as 0.4 nM PCP, well below the guideline value of PCP in drinking water (3.7 nM) set by the United States Environmental Protection Agency (U.S. EPA), and 2.0 nM Cu(2+), much below the guideline value (2.0 mg L(-1), ~31.2 nM) from the World Health Organization (WHO), respectively. Toward the goal for practical applications, this simple and cost-effective probe was further evaluated by monitoring PCP and Cu(II) in water samples.